Michalina Oplatowska (2017)

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Critical Reviews in Food Science and Nutrition

ISSN: 1040-8398 (Print) 1549-7852 (Online) Journal homepage: http://www.tandfonline.com/loi/bfsn20

Food colors: Existing and emerging food safety


concerns

Michalina Oplatowska-Stachowiak & Christopher T. Elliott

To cite this article: Michalina Oplatowska-Stachowiak & Christopher T. Elliott (2017) Food colors:
Existing and emerging food safety concerns, Critical Reviews in Food Science and Nutrition, 57:3,
524-548, DOI: 10.1080/10408398.2014.889652

To link to this article: http://dx.doi.org/10.1080/10408398.2014.889652

Accepted author version posted online: 07


Apr 2015.
Published online: 07 Apr 2015.

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CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION
2017, VOL. 57, NO. 3, 524–548
http://dx.doi.org/10.1080/10408398.2014.889652

Food colors: Existing and emerging food safety concerns


Michalina Oplatowska-Stachowiak and Christopher T. Elliott
Institute for Global Food Security, School of Biological Sciences, Queen’s University Belfast, Belfast, United Kingdom

ABSTRACT KEYWORDS
Food colors are added to different types of commodities to increase their visual attractiveness or to Food dyes; synthetic colors;
compensate for natural color variations. The use of these additives is strictly regulated in the European legal and illegal food colors;
Union, the United States, and many other countries worldwide. There is a growing concern about the detection methods
safety of some commonly used legal food colorants and there is a trend to replace the synthetic forms
with natural products. Additionally, a number of dyes with known or suspected genotoxic or carcinogenic
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properties have been shown to be added illegally to foods. Robust monitoring programs based on reliable
detection methods are required to assure the food is free from harmful colors. The aim of this review is to
present an up to date status of the various concerns arising from use of color additives in food. The most
important food safety concerns in the field of food colors are lack of uniform regulation concerning legal
food colors worldwide, possible link of artificial colors to hyperactive behavior, replacement of synthetic
colors with natural ones, and the presence of harmful illegal dyes—both known but also new, emerging
ones in food. The legal status of food color additives in the EU, United States, and worldwide is
summarized. The reported negative health effects of both legal and illegal colors are presented. The
European Rapid Alert System for Food and Feed notifications and US import alerts concerning food colors
are analyzed and trends in fraudulent use of color additives identified. The detection methods for
synthetic colors are also reviewed.

1. Introduction
additives in the Developed World is strictly controlled by legis-
Colors are added to many foods to make them more attractive lation, since many of the synthetic compounds were shown to
to the eye of the consumer and to compensate for natural color be toxic and harmful to humans. However, the legislation varies
variations that exist in many foods. Color influences the per- in different countries. Therefore, the first important issue in the
ception of food quality and stimulates the appetite, since it is area of food colors is the lack of uniform regulations world-
perceived to relate to flavor (Downham and Collins, 2000). The wide. It causes problems to food importers and exporters as the
use of color additives dates back to the Ancient Egyptian period same food color can be legal in one country but illegal in
(1500 BC) when colorants were added to wine and confection- another.
aries (Downham and Collins, 2000; Watson, 2001). Since then The second current issue concerns the legally used synthetic
numerous naturally derived colors (such as indigo, alkanet colors and their link to hyperactive behavior in children (Bate-
(borage root), turmeric, safflower, parsley, spinach, fruits, man et al., 2004; McCann et al., 2007). Synthetic food colors do
flower petal extracts, annatto, paprika, brazilwood, and cochi- not provide any nutritional value and there is a growing con-
neal) have been used to improve the appearance of foods. The cern about their adverse health effects. Due to consumer
use of mineral and metal-based compounds for this purpose demands, there is an industry trend to remove synthetic colors
was also reported following the industrial revolution. However, from food and replace them with natural products. So far in
the ingestion of such toxic coloring chemicals as red lead the EU there has not been a ban placed on synthetic dyes; how-
(Pb3O4), vermillon (HgS), and copper arsenate in food could ever in the UK voluntary action of the industry has already
cause illness and death (Downham and Collins, 2000). In 1856, resulted in a marked change to the use of natural colors by
the British chemist Sir William Henry Perkin created the first major food manufacturers. The recent re-evaluations of all the
synthetic dye “mauveine” by oxidizing aniline (Watson, 2001). synthetic food colors performed by European Food Safety
As a result of the “color revolution” thousands of new coloring Authority (EFSA) did not raise substantial safety issues when
compounds were synthesized for industrial applications. The these compounds are used according to regulations (EFSA,
artificial colors were widely available and used also as food 2009a–2009f). However, there is a legal requirement in the EU
additives, due to a range of advantages over the natural coun- for foods containing six dyes (tatrazine, quinoline yellow, sun-
terparts such as ease of production, low cost, high stability, and set yellow, ponceau 4R, allura red, and carmoisine) that have
better coloring properties (Downham and Collins, 2000; Oreo- been linked to hyperactivity to be labeled with a warning that
poulou et al., 2009). Nowadays, the use of colors as food they might have an adverse effect on the attention in children

CONTACT Michalina Oplatowska-Stachowiak [email protected] Institute for Global Food Security, School of Biological Sciences, Queen’s University
Belfast, David Keir Building 18-30 Malone Road, BT95BN Belfast, United Kingdom.
© 2017 Taylor & Francis Group, LLC
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 525

(Regulation (EC) No 1333/2008). In the USA Food and Drug consumed as foods as such and not normally used as characteris-
Administration Food Advisory Committee did not find casual tic ingredients of food. Preparations obtained from foods and
evidence to support the link between food colors and hyperac- other edible natural source materials obtained by physical and/
tivity (F&DA, 2011a, 2011b). or chemical extraction resulting in a selective extraction of the
The third issue is the replacement of synthetic colors with natu- pigments relative to the nutritive or aromatic constituents are
ral ones, which is not that straightforward as it might appear and colors within the meaning of this Regulation.” Only additives
not all the natural colors are completely safe. The current trend of included in the Annex II to this Regulation can be used in food.
using “coloring foodstuffs” (food ingredients such as fruits of vege- There are currently 25 colors of natural (or nature identical)
tables that secondary effect is coloring) instead of color additives origin and 15 synthetic on the list (Fig. 1). The natural color
can lead to more regulatory problems as these substances in the EU canthaxanthin (E161g) cannot be added to any type of food,
are not covered by the Regulation on food additives. however it is included in the list as it is used in medicinal prod-
The fourth problem covers the illegal addition of known and ucts. Canthaxanthin can be also used in animal feed (Commis-
emerging industrial dyes to food. There are many coloring sion Regulation (EC) No 775/2008). The safety of this
compounds (such as sudan dyes, rhodamine B, methyl yellow, compound has been recently evaluated by EFSA (EFSA, 2010)
or malachite green) widely used in industry for coloring fabrics, and it was noted that the main adverse effect of this additive is
plastics, or inks that are known or are suspected to have nega- the deposition of canthaxanthin crystals in the retina. It was
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tive health effect and should not be consumed by humans. In concluded that the exposure to canthaxanthin arising from the
some countries, particularly in the Developing World, harmful consumption of edible products from animals that have been
dyes that are not intended for human consumption can be fed with feedstuff containing this color is unlikely to exceed the
added to foodstuffs due to a lack of legal restrictions on their Acceptable Daily Intake (ADI).
use or very limited ability to monitor and control. Their pres- The legislation on food additives does not cover foods that may
ence in food entering the EU, for example, has been reported be used for technological function such as saffron for coloring pur-
over a number of years on the Rapid Alert System for Food and poses. The regulation specifies preparations obtained from foods
Feed (RASFF). Such illegal practice results in economic incen- and natural sources by selective extraction that are used as coloring
tives as the quality of some types of foods such as spices are agents, but does not consider foodstuffs with coloring properties
assessed on the basis of color intensity (Perva-Uzunalic et al., (even concentrated forms or extracted in a non-selective way that
2004). Globalization has resulted in the importation of food retains most of the food characteristics like color, flavor, and taste)
from around the world to the Developed World. The lengthen- as food additives. Fruits and vegetables extracts do not fall under
ing and increasing complexities of the food supply chain and the regulation but chlorophylls or carotenoids selectively extracted
substandard control over the food production in exporters’ from them do and as such they must undergo safety assessment
countries can lead to the exposure of humans to the hazardous before they can be approved. This distinction can be unclear and
chemicals in imported foods (Lineback et al., 2009). There are there is an ongoing debate about differentiating between coloring
number of compounds such as sudan dyes for which there are foodstuffs and food additives (FSA, 2011).
monitoring programs in Europe or the United States. Due to a Interesting examples of color substances that can have two
large number of synthetic colors available for industrial appli- functions in food are beta-carotene (E160a) and riboflavin
cations, the well-known illegal food dyes can be replaced by (E101). Beta-carotene is vitamin A precursor and riboflavin is
other similar compounds that are not monitored for. Such vitamin B2. These two colors provide additional nutritious
unacceptable practices can be reduced in number and severity value to the products they are added to. Apart from being
by improving legislation, developing stricter, more comprehen- included in the regulation on food colors they are also covered
sive monitoring programmes, and by employing rapid, cost- by Regulation (EC) No 1925/2006 of the European Parliament
effective testing methods capable of detecting multiple hazards. and of the Council of 20 December 2006 on the addition of
vitamins and minerals and of certain other substances to foods.
The regulation on food colors specifies the approved color
2. Regulation on the food color additives in the
additives, foods in which food color presence is not permitted,
European Union
and the conditions of use of each additive in different foods.
Food color additives can be synthetic, natural (derived from Each additive is associated with a corresponding E number.
plant, animal, or mineral sources), and also so-called “nature The color number or name must be declared in the ingredients
identical” that are identical to those found in nature but are list of the product. Additionally, Annex V introduced the label-
synthesized by human, for example, synthetic carotenoids. The ing requirement for food containing six artificial colors (E102,
first regulation within the European Economic Community E104, E110, E122, E124, E129) stating that they “may have an
countries concerning coloring matters was introduced in 1962 adverse effect on activity and attention in children.”
(Council Directive 62/2645/EEC). This was replaced by Euro- A summary of the history of the legal status of each of the
pean Parliament and Council Directive 94/36/EC on colors for color additives in the EU is presented in Fig. 2. Within the first
use in foodstuffs. Most recently Regulation (EC) No 1333/2008 set of European regulations (Council Directive 62/2645/EEC), a
of the European Parliament and of the Council of 16 December number of synthetic dyes such as E103, E105, E111, E121,
2008 harmonizing the use of all food additives was introduced E125, E126 were allowed but they were later removed by an
within the EU. This regulation defines color as “substances amendment as questions about their safety emerged (Council
which add or restore color in a food, and include natural constit- Directive 76/399/EEC). The next piece of legislation, Council
uents of foods and natural sources which are normally not Directive 94/36/EC, approved 17 synthetic dyes and 26 natural
526 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT
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Figure 1. Food color additives currently permitted in the EU.

or nature identical. The use of E128 was suspended in 2007 as colors permitted for use in Council Directive 94/36/EC to the
there was sufficient evidence relating to its carcinogenicity Regulation 1333/2008 reveals that colors E154 and E160f were
(Commission Regulation (EC) No 884/2007). Current legisla- removed from the list of approved colors, the former due to the
tion (Regulation (EC) No 1333/2008) specifies the colors per- fact it was no longer used and there was not sufficient data on
mitted in food and is based on the state of knowledge, the its safety, the latter because it was no longer offered by the
technological need, and their practical use. A comparison of manufacturer (Commission Regulation (EU) No 1129/2011).
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 527
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Figure 2. The history of the legal status of color additives in the EU. The graph illustrates changes to the status of each color additive after the introduction of the new
regulation or amendment. For example, E100 has always been legal, while E103 had been allowed by Council Directive 62/2645/EEC, then it was removed from the list
by the amendments and it has been illegal since then.
528 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Both dyes had been previously permitted for special use only susceptible individuals (EFSA, 2009e) and six of them (tatrazine,
(E154 for kippers and E160f for Saucisses de Strasbourg). quinoline yellow, sunset yellow, ponceau 4R, allura red, and car-
moisine) have been linked to increase in the hyperactive behav-
ior in children (Bateman et al., 2004; McCann et al., 2007).
3. Regulation on food colors in the United States, However, natural colors have only been tested to a limited extent
India, Japan, and China and their evaluations are based on a number of assumptions.
The legislation concerning food colors varies widely across dif- With increasing use of natural colors in food, exposure to them
ferent countries. In the United States, the use of colors in food might not be in the “natural” or “normal” ranges any longer
is regulated by U.S. Food & Drug Administration (F&DA). The (Watson, 2001; Nordic Council of Ministers, 2002). In the EU,
regulations concerning food additives are contained in the Title the natural food colors are regulated by the same legislation as
21 of the Code of Federal Regulations (e-CFR, 2009). There are synthetic substances and there are restrictions on their use.
only nine synthetic food colors allowed (that are subject to cer- EFSA has recently decided to re-evaluate all food colors includ-
tification) of which seven are for general use. Thirty-five ing natural products (Commission Regulation (EU) No 257/
derived from vegetable, animal, mineral sources, or synthetic 2010 setting up a programme for re-evaluation of approved food
duplicates of naturally occurring coloring compounds are additives). This process should be completed in 2015 for all color
exempt from certification and eight of them are for use in ani- additives. The issues and concerns with replacing synthetic food
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mal feed only. The colors subject to certification must have colors with natural alternatives have been discussed elsewhere
their identity and purity checked by F&DA. Three synthetic (Scotter, 2011a). The important issues pertaining to a number of
colorants approved for consumption in the United States are natural colors are presented below.
not permitted in the European Union, while nine food syn-
thetic colors (out of 15) that are legal in Europe are not autho-
4.1. Cochineal
rized in the United States (Table 1.). The regulation in India
permits eight synthetic colors (one of which is not legal in the Cochineal is a natural red color obtained from crushed insects
EU) and 11 natural or nature identical additives, no inorganic (Dactylopius coccus). A substantial amount of attention recently
dyes are permitted (The Prevention of Food Adulteration has been directed to the use of cochineal in drinks as it makes
Rules, 1955). Japanese legislation allows use of 12 synthetic col- the product to which it is added non-vegan (CBSNews, 2012).
ors in food (four of them cannot be used in the EU) (JETO, However, cochineal is used widely as an alternative to artificial
2006). Chinese legislation permits 11 synthetic colors in food, colors. It is used in many types of foodstuff that the consumer
of which one (new red) is illegal in the EU, United States, Japan, is unlikely to be aware of. The extract from Dactylopius coccus
or India (Ministry of Health, People’s Republic of China, 2011). contains carminic acid that is responsible for dying properties
and also proteins that can cause allergic reactions and asthma
(Baldwin et al., 1997; Lizaso et al., 2000).
4. Natural vs. synthetic colors
The common belief is that natural colors are better from a health
4.2. Caramel
perspective and consumers demand their use instead of synthetic
substances (Downham and Collins, 1991). Some synthetic food Caramel is produced from sugar heated at high temperature.
dyes such as tartrazine can cause an intolerance reaction in Some concerns have been raised recently about formation of

Table 1. Comparison of the synthetic dyes authorized for use in food in different global regions.
EU US Japan India China

E102 tartrazine FD&C yellow No. 5. Food yellow No. 4 Tartrazine Tartrazine
E104 quinoline yellow Quinoline yellow
E110 sunset yellow FCF FD&C yellow No. 6. Food yellow No. 5 Sunset yellow FCF Sunset yellow
E122 azorubine Carmoisine Carmoisine
E123 amaranth Food red No. 2 Amaranth
E124 ponceau 4R Food red No. 102 Ponceau 4R Ponceau 4R
E127 erythrosine FD&C red No. 3. Food red No. 3 Erythrosine Erythrosine
E129 allura red AC FD&C red No. 40. Food red No. 40 Allura red
E131 patent blue V
E132 indigotine FD&C blue No. 2. Food blue No. 2 Indigo carmine Indigotine
E133 brilliant blue FCF FD&C blue No. 1. Food blue No. 1 Brilliant blue FCF Brilliant blue
E142 green S
E151 brilliant black BN
E155 brown HT
E180 litholrubine BK
FD&C green No. 3 Food green No. 3 Fast green FCF
orange B
citrus red No. 2.
Food red No.104 (phloxine B)
Food red No.105 (rose bengal)
Food red No.106 (acid red 52)
New red
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 529

the genotoxic or carcinogenic agents: 2- and 4-methylimida- 5. Assessment of the safety of food colors
zoles, furan and 5-hydroxymethyl-2-furfural (5-HMF), and
In the European Union, an additive can be used in food when
immunotoxin 2-acetyl-4-tetrahydroxy-butylimidazole during
the criteria laid down in Regulation (EC) No 1333/2008 are
caramel manufacturing process (EFSA, 2011; Jacobson, 2012).
met: there is a technological need for its use, it does not present
5-HMF is formed during caramelization and in Maillard
any hazard to health based on the scientific data available and
reaction when carbohydrates react with proteins at high tem-
it does not mislead the consumer. Additionally, it must provide
perature. It can be found not only in caramel but also in heat-
some advantages to the consumer. The specific conditions for
treated food such as dried fruit, coffee, honey, milk, and other
colors state that it should also serve one of the following func-
products (Abraham et al., 2011, EFSA, 2011). When carameli-
tions: restore the original appearance of the food, make food
zation is performed in the presence ammonium compounds
more appealing, and add color to colorless foods. The additive
then 2- and 4-methylimidazoles and 2-acetyl-4-tetrahydroxy-
must be subject to toxicological testing, evaluation, and re-eval-
butylimidazole can be formed in the reaction of ammonia with
uation in the light of new scientific data. The Regulation speci-
carbohydrates. Due to the safety question, EFSA recommended
fies the foodstuffs to which the additive can be added and the
to reduce the level of these compounds, update the purity speci-
level of addition, taking into accounts the Acceptable Daily
fication for caramel colors, and undertake further research into
Intakes (ADIs). ADI is “an estimate of an amount of a sub-
the nature of the formation of these constituents during the
stance in food or drinking water that can be ingested daily over
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production process of caramel (EFSA, 2011).


the lifetime without appreciable risk, expressed in mg per kg of
body weight” (JECFA, 2009).
4.3. Color additive vs. coloring foodstuffs The approval of a color for human consumption in the EU
can only be carried after a safety assessment is prepared by the
In the EU there is a distinction between color additives (that are
European Food Safety Authority (EFSA), specifically by The
covered by Regulations on food additives) and what is referred
Panel on Food Additives and Nutrient Sources Added to Food
to as “coloring foodstuffs” that are food ingredients with color-
(ANS). This panel is responsible for safety evaluations of new
ing properties. These are foods that are used during
food additives (excluding flavorings and enzymes) and re-eval-
manufacturing of the product and their secondary effect is col-
uation of all authorized food additives. The safety evaluation of
oring. “Foods, whether dried or in concentrated form, including
food additives for human consumption requires a review of
flavorings incorporated during the manufacture of compound
published scientific studies on the toxicity of the additive such
foods, because of their aromatic, sapid, or nutritive properties
as animal studies using large doses of additives for long periods
together with a secondary coloring effect” are not considered to
to show that the substance will not cause harmful effects at the
be color additives by Regulation (EC) No 1333/2008. Examples
expected levels of human consumption. The additive is permit-
of foodstuffs with coloring properties are fruits and vegetable
ted if according to the current state of knowledge, there is a rea-
concentrates prepared from safflower, radish, black carrot,
sonable certainty of no harm to the consumer from ingestion of
lemon, hibiscus, red cabbage, and spinach, for example. When
this additive under its proposed conditions of use. The assess-
spinach is processed by a non-selective extraction procedure to
ments of safety of food additives are based on available scien-
produce paste or concentrate and then added to the product, it
tific data on the toxicity of the chemicals that are collected and
is not considered as being a food additive but a food ingredient.
evaluated by International Agency for Research on Cancer
When spinach is selectively extracted to produce chlorophyll
(IARC), National Toxicology Program of the US Department
(E140), then this chlorophyll is classified as a food additive and
of Health and Human Services (NTP), or Joint Food and Agri-
is covered by the regulation on food additives. Thus, the differ-
culture Organization of the United Nation/World Health Orga-
ence lies in how the extract of the natural product is prepared
nization Expert Committee on Food Additives (JECFA).
and if this is treated as an intrinsic part of the product or as a
In 1994, when the European Parliament and Council Direc-
color additive. This division is rather unclear and there is an
tive 94/36/EC on colors for use in foodstuffs was published, the
ongoing debate on the distinction between color additives and
assessment of the safety of color additives was dated back over
coloring foodstuffs (FSA, 2011), as shown by the example of
a number of years. Therefore, when the new legislation was
spirulina. In 2005 Nestle decided to remove all synthetic colors
introduced (Regulation (EC) 1333/2008), the European Com-
from their products due to the concerns about their adverse
mission decided to re-evaluate all of the permitted food colors
health effects. As a result blue dyed variants of some popular
and other additives. All food additives approved before 20 Jan-
sweets were removed as there was no replacement for a blue
uary 2009 must be subjected to new risk assessments. Most of
synthetic color brilliant blue E133. Blue sweets were reintro-
the food colors have been already evaluated. The assessment of
duced in 2008 colored with a naturally occurring blue-green
the last group of colors should be completed by 31st of Decem-
dye obtained from spirulina (algae) extract, a permitted health
ber 2015 (Commission Regulation (EU) No 257/2010).
ingredient (Scotter, 2011a). Spirulina is currently considered as
The effect of the re-assessment can result in the change of
a coloring foodstuff but if the European Commission decides to
the legal status of the food additive. An example of such a re-
change its status, it will require the same approval process as
assessment can be demonstrated by the case of red 2G. Follow-
the other food additives do (Food Navigator, 2010, 2011). In
ing the EFSA re-evaluation of the dye red 2G in 2007 (EFSA,
the United States, spirulina derived from the dried biomass of
2007), Commission Regulation 884/2007 suspended its use.
the cyanobacteria Arthrospira platensis has been recently added
This dye was permitted previously for coloring breakfast sau-
to a list of approved color additives exempt from certification
sages; however there was sufficient evidence that it is
in response to Mars Inc. petition (F&DA, 2013a).
530 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

metabolized into the carcinogenic aniline to suspend its use. (c) Due to limited data, sudan III, sudan IV, and para red
Another dye brown FK (previously permitted in kippers only) are all considered to be potentially genotoxic and possi-
has been recently removed from the list of approved colors bly carcinogenic as they are structurally related to sudan
included in the Regulation (EC) 1333/2008 due to the fact it I (IARC, 1975; EFSA, 2005).
was no longer used and there was no sufficient data on its safety (d) In vitro mammalian cells study and in vivo tests showed
available. a potential genotoxic effect of orange II, while data on
carcinogenicity are limited (EFSA, 2005).
(e) Methyl yellow was shown to be carcinogenic in rats and
6. Illegal dyes for coloring and associated health risks
it is classified as group 2B carcinogen—possibly carcino-
Dyes used for industrial applications, under some circumstan- genic to humans (IARC, 1975).
ces, can be fraudulently added to a range of foods to increase Another dye rhodamine B is considered to be potentially
their value, i.e., when the color of a product is one of the indica- both genotoxic and carcinogenic (EFSA, 2005). It was demon-
tors of its quality or to mask low quality of a product. These strated to be carcinogenic in rats after subcutaneous injection
dyes are cheap to produce and readily available (Tripathi et al., (IARC, 1978). Triphenylmethane dyes such as malachite green
2007). A number of illegal dyes have been found or have been and its metabolite leucomalachite green are considered to be
suspected of being present in foods consumed in the EU genotoxic and/or carcinogenic (EFSA, 2005).
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(RASFF online database), United States (F&DA, 2013b), India


(Tripathi et al., 2007), or Japan (Ministry of Health Labour and
7. Illegal use of dyes as veterinary drugs and the
Welfare, Japan) with some examples (illegal in the EU) pre-
associated health risks from contaminated foods
sented in Fig. 3. Most of these dyes are considered to be geno-
toxic and/or carcinogenic or there is limited data available to Triphenylmethane dyes (such as malachite green and crystal
conclude if they are safe or not. The two main groups of dyes: violet) are a group of synthetic dyes that not only can be ille-
azo-dyes and triphenylmethanes have been identified as those gally added to food for coloring purposes but can also be pres-
most likely to be illegally added to food (EFSA, 2005). Azo dyes ent in fish tissues as residues due to the illegal usage as
are a group of organic compounds widely used in industry. The veterinary drugs. These dyes are applied in industry for color-
toxic activity of these dyes is a result of their metabolism (Golka ing leather, wool, cotton, paper, and fibers and in staining of
et al., 2004). The azoreduction (breakage of azo bond) is tissues and bacteria (Arnold et al., 2009). They have also been
enzyme-mediated and results in formation of active aromatic used in aquaculture as veterinary drugs for the treatment of
amines that can form DNA adducts. The azoreductive enzymes bacterial, protozoan, and fungal infections in fish, as they are
present in liver, skin, and gastrointestinal microflora appear to very cheap and easy to apply (Culp et al., 1999). European, US,
play the main role in the in vivo reduction (Xu et al., 2007). and Japanese surveillance systems (RASFF online database;
The metabolism of the azo-dyes is reduced by substitutions in F&DA, 2013c, Import Alert 16–124; Ministry of Health Labour
the aromatic ring—sulphonation or carboxylation and substitu- and Welfare, Japan, Imported Food Inspection Services) have
tion of the hydrogen of an amino group. Substitutions can reported the presence of malachite green and crystal violet in
reduce genotoxicity by decreasing lipid solubility of the dye fish imported from such countries as Vietnam, China, Thai-
and as a result its absorption (EFSA, 2005). Therefore, sudan I land, Taiwan, and Indonesia. Triphenylmethanes have never
is assumed to be carcinogenic while sunset yellow FCF is a legal been authorized for the use in fish for human consumption in
food additive. The only difference between these two chemicals the United States or the EU due to the concerns regarding their
is the presence of two sulpho groups in the sunset yellow FCF genotoxic/carcinogenic properties. Both short-term and long-
structure what causes a decrease in lipid solubility. term feeding studies in animals (Culp et al., 1999, 2002, 2006)
The potential of a chemical to be metabolized into a lipid showed some toxic properties of both malachite green and its
soluble aromatic amine has been considered to be an indication metabolite leucomalachite green. Gentian violet (comprised of
of genotoxic and/or carcinogenic action. Thus, several dyes pre- 96% crystal violet and 4% methyl violet) was demonstrated to
sented in Fig. 3 have been identified to be potentially harmful be carcinogenic in mice and rats in a long-term exposure study
(EFSA, 2005). According to the available toxicity data some of (Littlefield et al., 1985).
the illegal azo dyes that have been detected recently in foods in
the EU are possible genotoxic and/or carcinogenic agents. A
8. The effect of permitted food additives on the
number of examples are presented below:
behavior of children
(a) Sudan I is considered to be genotoxic both in vitro and
in vivo. The subcutaneous administration of this dye in In the 1970s, it was suggested that some food additives can
mice resulted in liver tumors. It was also shown to be cause behavioral disorders such as hyperactivity and learning
carcinogenic in rats after oral administration (IARC, disabilities in children (Feingold, 1975). Since that time a num-
1975; NTP, 1982; EFSA, 2005). ber of research studies have focused on this topic, some con-
(b) Sudan II was shown to be genotoxic in vitro; however firming while others rejecting this hypothesis (Arnold et al.,
no in vivo data are currently available. It is considered 2012). In 2004, a group of researchers (Bateman et al., 2004)
to be potentially genotoxic and also a possible carcino- reported the adverse effect of the artificial food colorings (sun-
gen as the increase in the incidence of bladder cancer set yellow, tartrazine, carmoisine, ponceau 4R) and sodium
was reported in mice following implantation of sudan benzoate on the behavior of three-year old children. In Septem-
II pellets (IARC, 1975; EFSA, 2005). ber 2007, the same group published further results of the
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 531
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Figure 3. Dyes not permitted for use in foods in the EU but possibly used/abused in the EU and other countries (EFSA, 2005; RASFF online database; Tripathi et al., 2007).

studies on three and eight/nine-year old children (McCann sodium benzoate. The authors concluded that there was a sig-
et al., 2007). The researchers used two mixtures of food addi- nificant reduction in hyperactive behavior during the with-
tives: one containing sunset yellow, carmoisine, tartrazine, pon- drawal phase and an increase in hyperactivity during the
ceau 4R, and sodium benzoate; the second was composed of exposure to artificial food additives. The findings of these stud-
sunset yellow, carmoisine, quinoline yellow, allura red AC, and ies were widely discussed and debated among the scientific
532 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

community. According to the Committee on Toxicity (COT) of between food colors and hyperactivity and did not recommend
Chemicals in Food, Consumer Products and the Environment additional labeling requirements (F&DA, 2011a, 2011b). Nev-
(a scientific committee that provides an advice to the Food ertheless, it was advised to conduct the exposure assessment of
Standards Agency, the Department of Health and other Gov- seven US certified synthetic colors in children. The quantitative
ernment Departments and Agencies on matters concerning the HPLC-DAD method applicable for different food matrices has
toxicity of chemicals in the UK), the study provided evidence been developed and validated for this purpose (Harp et al.,
that some mixtures of food additives could be linked to the 2013). The recent meta-analysis covering multiple studies in
increase in hyperactive behaviors in children. Additionally, it the area prepared by a group of US researchers found a statisti-
was noted that the effects were small and not clearly evident; cally significant effect of the reduction of the ADHD symptoms
therefore it was not possible to extrapolate the obtained results when synthetic food color additives free diet is applied (Nigg
to the whole population. However, the results were consistent et al., 2012). Another group of US researchers have recently
with previous reports concerning the hyperactivity after con- found a link between consumption of soft drinks and behav-
suming certain foods (COT, 2007). The European Food Safety ioral problems in five-year old children and suggested that one
Authority (EFSA, 2008) concluded that there was limited evi- of the possible explanations might be the presence of artificial
dence of the influence of the additives used in the research con- food colors in these products (Suglia et al., 2013).
ducted on the behavior of children. According to EFSA, the The exact biological mechanisms of the suspected influence
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effect was not statistically significant for both mixtures and age of artificial food additives on hyperactive behavior are
groups. It was not possible to determine the effect of individual unknown. The hyperactivity witnessed post exposure to some
colors since the mixtures were used in the study. According to food additives may be caused by an altered central nervous sys-
the UK Food Standards Agency (FSA, 2008a), the Southamp- tem dopamine function that can have a genetic basis. It was
ton study left uncertainty regarding the safety of the food addi- demonstrated that the artificial colors can also induce IgE-inde-
tives tested in this research. It was also noted that part of the pendent histamine release (Bateman et al., 2004). The South-
food industry was already withdrawing the artificial colors due ampton study provided some evidence that the hyperactive
to consumer demand. The Food Standard Agency Board agreed behavior can be associated with some genetic polymorphisms
at its 2008 April meeting to advice UK Ministers concerning thought to impair histamine clearance. In addition, it was
the withdrawal of these additives (FSA, 2008b). It was recom- shown (Lau et al., 2006) that combinations of various food
mended to phase out these colors by the voluntary action of the additives show synergistic effect to inhibit neuronal cell differ-
food industry by the end of 2009 and to undertake more action entiation in vitro, the mechanism of this effect and its influence
to remove them from food in the whole EU. Parents of children on the development of disorders is unknown. A study con-
showing hyperactive behavior were advised to decrease the con- ducted by Ceyhan et al., 2013 found that artificial food colors
sumption of the six artificial colors. and additives administered to female rats before and during
While EFSA does not consider the evidence for dyes and gestation can cause an alteration in the expression of N-
hyperactivity link to be convincing enough, the legislation in methyl-D-aspartate receptors (NMDARs) and nicotinic acetyl-
the EU requires all food containing artificial colors used in choline receptors (nACHRs) (that are linked to the learning
Bateman et al. and McCann et al. studies to be labeled with and memory-generating processes) in their offspring.
warning: “may have an adverse effect on the activity and atten-
tion in children”(Regulation (EC) No 1333/2008). EFSA initi-
9. The EU Rapid Alert System for Food and Feed, the
ated the re-assessment all of the permitted food colors and
United States import alerts and monitoring
completed the evaluation of six artificial colors on 23rd of Sep-
of food colors
tember 2009 (EFSA, 2009a–2009f). The Panel reduced the
ADIs for quinoline yellow, sunset yellow FCF, and ponceau 4R. The Rapid Alert System for Food and Feed (RASFF) is a Euro-
The Panel did not change the existing ADIs for the three other pean network developed for the exchange of the information
colors assessed, tartrazine, carmoisine, and allura red AC. They about the risks detected in relation to food and feed. It involves
stated that according to the evidence available quinoline yellow, the Member States, the European Commission as the manager
sunset yellow FCF, ponceau 4R, carmoisine, and allura red AC of the system, and the European Food Safety Authority. When-
can be linked to some sensitivity reactions. Tartrazine may ever a member of the network has any information relating to
bring about intolerance reactions in a small part of the popula- the risk to human health deriving from food or feed, the infor-
tion. For all six colors, the Panel concluded that the evidence mation is immediately notified under the RASFF. Food Inspec-
currently available did not substantiate a causal link between tions Authorities, Food Safety Authorities, Food Ministry, and
the individual colors and possible behavioral effects. There is other related organizations in every European Union country
still no conclusive answer to whether certain additives or their are directly responsible for such exchange of information.
combination can have an adverse effect on the behavior of chil- RASFF notifications are triggered by official controls on the
dren. Recently, due to new scientific data on genotoxicity of internal market and controls at the border posts of the outer
allura red, EFSA have recommended to perform more tests on European Economic Area borders. Other cases can involve
all sulphonated mono azo dyes currently approved to be used consumer complaints, companies notifying the outcome of an
in food (amaranth, ponceau 4R, sunset yellow, tartrazine, azor- internal check or food poisoning outbreak (Kleter et al., 2009).
ubine, and allura red) (EFSA, 2013). The notifications include details of the notifying country, the
The US Food and Drug Administration Food Advisory risk and the origin of food, the source of notification, and the
Committee did not find the causal evidence to support the link action that has been taken. The notifications concern all risks
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 533

connected to food such as bacterial contaminations, chemical Illegal and/or Undeclared Colors” Import Alert 45–02 (F&DA,
contaminations, drug residues, illegal food additives, excessive 2013b) lists the products in which illegal or undeclared colors
content of food additives, foreign bodies, insects, risk of migra- were found and as a result they can be detained without physi-
tion of package component, altered organoleptic characteristics cal examination upon entry to the United States. The product
(appearance, color, and taste), and risks of suffocation. is removed from the list when the importer provides the evi-
The notifications concerning food dyes are generally of fol- dence of compliance with the law or provides a number of
lowing types (Table 2): “clean shipments.” The list presents the current state of the
1) unauthorized color—illegal color fraudulent use of colors and is updated frequently (Table 3.).
2) unauthorized use of color—color is permitted in some Colors subject to certification (all synthetic colors) must come
foods only from F&DA certified lots, even if they are used in imported
3) too high content of authorized color foods. As a result a high number of products containing dyes
4) undeclared color legal in the United States imported from EEC or other foreign
Numerous notifications for the presence of sudan dyes countries for which producers cannot present the required cer-
(mainly sudan I and IV) in food are recorded every year tificate are detained on entry to the United States. A number of
(Table 2.). The highest number was observed between 2003 dyes illegal in the United States and legal in the EU such as
and 2005 when a large quantity of chilli and chilli products amaranth, brilliant black BN, brown HT, carmoisine, green S,
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imported to the EU was contaminated with these dyes. The patent blue V, ponceau 4R, quinoline yellow and illegal in both
contamination of fish with malachite green and crystal violet United States and Europe such as rhodamine B or orange II
has been observed over the years with the highest number of have been also reported.
cases recorded in 2005. Para red, orange II, methyl yellow, and
rhodamine B are also consistently detected in foods. The high
number of notifications concerning too high use or unautho-
10. Analytical methods developed for the detection
rized use of legal colors, mainly in imported foods, shows the
of synthetic food colors
problems faced by food importers to attempt to adhere to the
EU regulations. Lack of uniform regulation worldwide results Multiple chromatographic methods with different detection
in the withdrawal from the EU market or border rejection of systems, spectrophotometric, voltammetric, and capillary elec-
the products containing dyes legal in Japan (rose bengal, acid trophoresis techniques have been developed for the analysis of
red 52—JETO, 2006) or the United States (fast green FCF— synthetic color compounds in foodstuffs; some examples are
eCFR, 2009). presented in Table 4. Reviews on the detection of natural colors
Legal synthetic colors such as tartrazine, sunset yellow, azor- (Scotter, 2011b) and sudan I-IV specifically (Rebane et al.,
ubin, amaranth, ponceau 4R, erythrosine, and allura red appear 2010) have been presented elsewhere.
on RASFF when they are used in food to which they should not The multianalyte HPLC-DAD method developed by Yosh-
be added, when there is too high content of them or food con- ioka and Ichihashi (2008) can be used for the analysis of 40
taining the colors is not properly labeled. Natural colors such synthetic legal and illegal colors in drinks and confectionary.
as curcumin or cochineal have been also reported to be used in Other HPLC-DAD methods were developed to monitor the
an illegal way (Table 2). Annatto/bixin/norbixin (E160b) is a presence of 17 legal and illegal (Bonan et al., 2013), 14 legal
natural color (extracts from seeds of annatto tree) that appears (Kirschbaum et al., 2003), 13 legal (Minioti et al., 2007), or 7
in RASFF most frequently. It is detected in spices, fish and fish legal (Harp et al., 2013) synthetic food colors. Tandem mass
products, and non-alcoholic beverages, but is not authorized to spectrometry based detection has also been applied in the dye
be used in any of these types of food. analysis field, mainly to determine the presence of illegal and
RASFF has also recently reported new type of the notifica- potentially harmful dyes. The HPLC-MS/MS method devel-
tions concerning the lack of proper labeling of the presence of oped by Feng et al. (2011) can be used for the detection of 40
synthetic colors that have been linked to hyperactivity: “08//12/ synthetic dyes in soft drinks and Zhao et al., (2012) for the
2011 undeclared color (undeclared “Southampton” colors with monitoring of the presence of 23 illegal dyes; Sun et al. (2007)
absence of required health warning) in fruit flavored sweets of 10; Botek et al. (2007) of 8; and Fang et al. (2013b) of 7.
from Hong Kong” or “22/12/2011 insufficient labeling (absence HPLC-MS/MS was also developed for 13 triarylmethane and
of required health warning for “Southampton” colors) of green phenothiazine dyes (Tarbin et al., 2008). Recently, Liu et al.
masala paste from the United Kingdom (RASFF online data- (2011) used UPLC-MS/MS for the determination of 15 illegal
base). According to Regulation (EC) No 1333/2008 food con- dyes.
taining colours E102, E104, E110, E122, E124, E129 should be A number of antibody-based screening methods, i.e.,
additionally labeled with a warning stating that they “may have enzyme-linked immunosorbent assays (ELISA) were developed
an adverse effect on activity and attention in children.” This for the analysis of limited number of illegal synthetic colors:
labeling requirement is not strictly complied and, for example, sudan dyes, para red, orange II, triphenylmethanes (malachite
in the UK it is possible to find products placed on the market green, crystal violet, brilliant green), rhodamine B, methyl yel-
with “Southampton” colors present and without the required low, and chrysoidine. ELISA tests were also established for the
warning information based on the observation of this report’s detection of legal synthetic dyes—sunset yellow and tartrazine.
authors. A number of commercial companies in Europe provide ana-
The US Food and Drug Administration “Detention Without lytical services for sudan and related dyes. Eurofins can screen
Physical Examination and Guidance of Foods Containing for 28 (Eurofins, 2013), Premier Analytical Services for 21
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534

Table 2. Number of notifications concerning coloring compounds in food recorded by RASFF (RASFF online database).

Number of notifications recorder by RASFF

Dye 2003 2004 2005 2006 2007 2008 2009 2010 2011 2012 Type of notification Product category2 Conc. [mg/kg –ppm]

Acid red 52 (sulforhodamine B) 3 Unauthorized color I, J


Basic red 46 1 Unauthorized color J 500–1500
Crystal violet and 2 5 2 2 Unauthorized substance G 0.0009–0.654
leucocrystal violet
Fast garnet 1 1 Unauthorized color J 0.77–1.3
Fast green FCF 2 3 2 1 Unauthorized color A, C, M
Gardenia yellow 5 1 1 Unauthorized color A, C, K, S
Malachite green and 11 18 50 17 9 2 5 4 7 2 Unauthorized substance D, G 0.0003–4.875
leucomalachite green
Methyl yellow (butter yellow) 2 1 3 1 Unauthorized color J 0.24–44
Oil orange ss 1 Unauthorized color J 0.15
Orange II 1 2 2 1 3 2 Unauthorized color H, J, N, S 0.56–12,000
Orange RN 1 Unauthorized color J
Para red 42 12 1 1 Unauthorized color I, J, S 0.02–416
Red 2G 2 1 Unauthorized color L 1.4–6.3
M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Rhodamine B 5 3 5 2 1 3 5 3 Unauthorized color A, C, H, I, J, N, S, U 0.01–89.2


Rose bengal 1 3 Unauthorized color C, I
Sudan I 118 190 135 40 22 17 17 14 15 2 Unauthorized color A, F, I, J, O, R, S 0.0013–4938
Sudan II 1 Unauthorized color R
Sudan III 1 1 4 1 1 Unauthorized color F, J, S 0.1–181
Sudan IV 5 170 94 25 13 12 15 12 9 6 Unauthorized color A, F, I, J, L, S 0.01 –2105
Sudan 7B 1 Unauthorized color A, C, I, J, N, S 0.05
Sudan red G 1 1 1 Unauthorized color F, J, S 0.2–25.2
Toluidine red 1 1 2 Unauthorized color J, S 2.5–179
Victoria pure blue BO 1 Unauthorized substance G 0.0089
E 100 curcumin 1 1 1 1 Too high content, unauthorized use A, J, S 450–3200
E 102 tartrazine 3 36 10 7 12 5 7 3 Too high content, unauthorized A, B, C, G, I, J, M, N, O, R 1.2–6000
use, undeclared color
E 104 quinoline yellow 2 2 1 1 Too high content, unauthorized use A, C, G 70.6–128
E 110 sunset yellow FCF 1 2 11 7 15 16 11 11 7 2 Too high content, unauthorized A, C, D, G, I, J, K, L, M, N, O, R, S, T 5–2265
use, undeclared color
E 120 cochineal 1 1 4 4 Too high content, unauthorized use G, I, L, M, O 115–356
E 122 azorubine 7 8 2 2 5 2 6 7 Too high content, unauthorized A, B, C, G, I, J, K, L, M, N, T 15.6–314
use, undeclared color
E 123 amaranth 7 2 7 5 3 4 4 4 1 Unauthorized use, undeclared color B, C, E, H, J, K, M, N, S 1.2–3300
E 124 ponceau 4R 4 6 11 8 8 17 8 4 7 Too high content, unauthorized A, C, D, G, I, J, K, L, M, N, P, S 0.0027–1800
use, undeclared color
E 127 erythrosine 2 5 15 6 11 17 12 4 11 7 Unauthorized use A, B, C, D, E, G, H, I, J, K, M, N, O, R, S,W 1.6–145
E 129 allura red AC 2 2 7 8 4 5 2 3 1 Too high content, unauthorized A, C, D, E, G, I, J, L, M, N 1.5–850
use, undeclared color
E 131 patent blue V 1 1 Unauthorized use undeclared color C, I
E 132 indigotine/indigo carmine 1 1 1 1 1 Too high content, unauthorized C, E, G, I 14–309
use, undeclared color
E 133 brilliant blue FCF 3 2 2 4 2 2 Too high content, unauthorized A, B, C, E 91–2500
use, undeclared color
E 141i chlorophylls 1 Unauthorized use A
E 142 green S 1 Undeclared color C
E 150a plain caramel 1 1 Unauthorized use S, M
E 151 brilliant black BN 2 1 1 2 Too high content, undeclared color C, G 410–630
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Table 2. (Continued).
Number of notifications recorder by RASFF

Dye 2003 2004 2005 2006 2007 2008 2009 2010 2011 2012 Type of notification Product category2 Conc. [mg/kg –ppm]

E 153 vegetable carbon 1 Unauthorized use A


E 155 brown HT 1 1 Too high content, undeclared color C, G
E 160b annatto/bixin/norbixin 2 9 22 11 5 6 3 6 1 9 Too high content, unauthorized use A, C, F, G, J, M, S 0.6–3486
E 170 calcium carbonate 2 Unauthorized use H, S
E 171 titanium dioxide 19 7 17 5 Unauthorized use I 0.44–217
E 173 aluminium 1 Unauthorized use C
2
Product categories:
A—cereals and bakery products
B—cocoa and cocoa preparations, coffee, and tea
C—confectionery
D—crustaceans and products thereof
E—dietetic foods, food supplements, fortified foods
F—fats and oils
G—fish and products thereof
H—food additives
I—fruit and vegetables
J—herbs and spices
K—ices and desserts
L—meat and meat products (other than poultry)
M—non-alcoholic beverages
N—nuts, nut products, and seeds
O—other food product/mixed
P—poultry meat and poultry meat products
R—prepared dishes and snacks
S—soups, broths, sauces, and condiments
T—wine
U—food contact materials
W—milk and milk products
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION
535
536 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Table 3. Number of import alerts for each colour additive on “Detention Without malachite green in fish, the minimum required performance
Physical Examination and Guidance of Foods Containing Illegal and/or Undeclared limit (MRPL) for the method used for the detection of the sum
Colors” F&DA list as on 06/09/2013.
of malachite green and its leuco metabolite is set at 2 ppb in the
Nr of products on Import Alert EU according to Commission Decision 2004/25/EC.
Food color 45-02 as on 06/09/2013

Synthetic colors FD&C yellow No. 5. 2500


legal in the tartrazine 11. Food colors—Current issues
United States FD&C yellow No. 6 1905
sunset yellow 11.1. Synthetic colors
FD&C red No. 3. 416
erythrosine As a result of a large number of contamination cases of food
FD&C red No. 40. allura 1300
red with sudan dyes in the EU in 2003, the emergency measures
FD&C blue No. 1.brilliant 1359 were taken and all chilli, chilli products, curcuma, and palm oil
blue imported into the EU had to be screened for the presence of
FD&C blue No. 2 210
indigotine sudan I-IV dyes (Commission Decisions 2003/460/EC, 2004/
FD&C green No. 3 fast 24 92/EC, and 2005/402/EC). In 2005 and 2006, the Food Stand-
green FCF ards Agency (FSA) in the UK tested 893 samples of spices, sau-
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Citrus red No. 2 1


Natural colors Turmeric 33 ces, and oils for sudan dyes, para red, rhodamine B, orange II,
legal in the Annatto 9 red 2G, methyl yellow, and metanil yellow and found six to be
United States Astaxanthin 3 contaminated (FSA, 2006). Additionally, 18 samples contained
Betanin/beetroot 1
Carmine/cochineal 34 annatto/bixin/norbixin (E160b) a natural food color that
Carotene 45 should not be used in spices. Our own study on the application
Chlorophylls/copper 20 of the ELISA method for the detection of sudan I showed pres-
complexes of
chlorophylls ence of this contaminant in 3 samples (out of 85 tested) that
Iron oxides 13 were purchased within the EU (1 sample) and outside (2 sam-
Paprika color 9 ples) (Oplatowska et al., 2011c). The data from RASFF also
Riboflavin 2
Titanium dioxide 50 support the necessity for monitoring for the presence of sudan
Synthetic colors Acid red 52 16 dyes in food, as contamination events can occur, but not on the
illegal in the Acid yellow G 1 same scale as between 2003 and 2005. There are also a number
United States Amaranth 291
Brilliant black BN 22 of dyes with similar properties that might be illegally used in
Brown HT 5 food as a replacement for monitored sudan dyes. The com-
Carmoisine 1072 pounds such as metanil yellow, methyl yellow, rhodamine B,
Chrysoin S 6
Green S 33 toluidine red, and other sudan-similar azo dyes should be also
Lake red CBA 6 included in the screening programmes to ensure safe food for
Light green SF 3 the consumer.
Malachite green 12(rice and tapioca)
+35(seafood) A number of commercial companies offer screening services for
Orange II 24 several synthetic dyes. However, there is still a need for the develop-
Patent blue V 82 ment of multianalyte methods that could target a large range of sus-
Phloxine B 11
Polar yellow 5G 5 pect compounds. Such trends are currently observed in mycotoxin
Ponceau 4R 1162 analysis (Varga et al., 2013) and veterinary drug residues (Smith
Ponceau 6R 1 et al., 2009). Further expansion of the existing tools for fast, low-
Ponceau SX 14
Quinoline yellow 187 cost screening methods such as ELISA (limited to sudan dyes, para
Quinoline yellow spirit 10 red, methyl yellow, rhodamine B, orange II, chrysoidine, and tri-
soluble phenylmethane dyes thus far) would serve to provide further data
Red 2 G 6
Rhodamine B 99 on the occurrence of these contaminants in foods. The list of possi-
Natural colors Anthocyanin 21 ble targets is close to impossible to determine as there is such a large
illegal in the Calcium carbonate 6 number of synthetic dyes used in industry and widely available
United States Carbon black, charcoal, 134
vegetable carbon nowadays. New dyes are being detected in food, for example, in
Carthamin 13 2012 Ruf et al. (2012) reported the presence of common industrial
Gardenia blue pigment 7 azo-dye basic red 46 in sumac spice sample during the routine anal-
Gardenia yellow 17
pigment ysis for sudan dyes. Studies performed in countries from which the
dye-contaminated food is often imported can provide some back-

Import Alert 16-124 (F&DA, 2013c). ground on the targets that the analytical methods should focus on.
One such study in India reported the presence of a number of ille-
(Premier Analytical Services, 2013), or QTS Analytical for 14 gal dyes in colored food commodities purchased from urban and
illegal dyes (QTS Analytical, 2012). rural areas (Tripathi et al., 2007). Thirty-one percent of samples
Generally, no safe level of the presence of illegal dyes in were found to contain illegal dyes: metanil yellow, rhodamine B,
foods has been established; however the FSA in the UK has rec- orange II, sudan dyes, auramine, malachite green, amaranth, and
ommended a limit 0.5 ppm for products containing illegal dyes quinoline yellow (the last two are not permitted in India), with
to be withdrawn from the market (FSA, 2007). With regards more contaminants found in rural area (38% of the total samples,
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 537

Table 4. Detection methods for synthetic food colors.

Color CI number Detection methods

Acid blue 1 42045 Liquid chromatography—Yoshioka and Ichihashi, 2008


Acid green 9 42100 Liquid chromatography – Yoshioka and Ichihashi, 2008
Acid green 25 61570 Liquid chromatography—Feng et al., 2011
Acid red 13 (fast red E) 16045 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Acid red 52 (sulforhodamine B) 45100 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Acid violet 7 18055 Liquid chromatography—Yoshioka and Ichihashi, 2008
Acid violet 17 42650 Liquid chromatography—Feng et al., 2011
Acid yellow 9 (fast yellow AB) 13015 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Alizarin yellow GG 14025 Liquid chromatography—Feng et al., 2011
Amido black 10B (acid black 1) 20470 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Astrazon orange G (basic orange 21) 48035 Liquid chromatography—Fang et al., 2013b
Astrazon orange R (basic orange 22) 48040 Liquid chromatography—Fang et al., 2013b
Auramine O (basic flavine O) 41000 Liquid chromatography—Feng et al., 2011
Azocarmine B 50090 Liquid chromatography—Bonan et al., 2013
Azocarmine G 50085 Liquid chromatography—Bonan et al., 2013
Azure B 52010 Liquid chromatography—Tarbin et al., 2008
Benzyl violet 4B 42640 Liquid chromatography—Yoshioka and Ichihashi, 2008
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Brilliant black PN 28440 Liquid chromatography—Yoshioka and Ichihashi, 2008


Brilliant green 42040 Liquid chromatography—Andersen et al., 2007, 2009; Tarbin et al., 2008; Hurtaud– Pessel et al.,
2011
ELISA—Oplatowska et al., 2011a; Shen et al., 2011
Chrysoidine (basic orange2) 11270 Liquid chromatography—Gui et al., 2010; Reyns et al., 2010; Feng et al., 2011; Zhao et al., 2012;
Fang et al., 2013a, 2013b
Gas chromatography—Wang et al., 2008
Chemiluminescence sensor with magnetic molecularly imprinted polymer—Lu et al., 2012
ELISA—Lei et al., 2011
Chrysoine (acid orange 6, tropaeolin O, 14270 Liquid chromatography—Yoshioka and Ichihashi, 2008; Fang et al., 2013b
resorcinol yellow)
Crystal violet and/or leuco crystal violet 42555 Liquid chromatography—Rushing et al., 1995; Rushing and Hansen, 1997; Rushing and
Thompson, 1997; Tarbin et al., 1998; Andersen et al., 2007; Dowling et al., 2007; Wu et al.,
2007; 2008; Dowling et al., 2009; Long et al., 2009; Hurtaud-Pessel et al., 2011; Tao et al.,
2011; Ascari et al., 2012
Spectrophotometry—Safarik and Safarikova, 2002
ELISA—Yang et al., 2007; Oplatowska et al., 2011a; Shen et al., 2011
Disperse blue 106 111935 Liquid chromatography—Zhao et al., 2012
Disperse blue 124 111938 Liquid chromatography—Zhao et al., 2012
Disperse orange 3 11005 Liquid chromatography—Zhao et al., 2012
Disperse orange 11 60700 Liquid chromatography—Zhao et al., 2012
Disperse orange 37 11132 Liquid chromatography—Zhao et al., 2012
Disperse red 1 1110 Liquid chromatography—Zhao et al., 2012
Disperse yellow 3 11855 Liquid chromatography—Zhao et al., 2012
Eosine Y 45380 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Ethyl violet 42600 Liquid chromatography—Tarbin et al., 2008
Fast green FCF 42053 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011; Harp et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Huang et al., 2002, 2003, 2005; Jager et al., 2005;
Lee et al., 2008
Fast red E 16045 Liquid chromatography—Yoshioka and Ichihashi, 2008
Guinea green B 42085 Liquid chromatography—Feng et al., 2011
Light green SF 42095 Liquid chromatography—Feng et al., 2011
Malachite green and /or leuco malachite green 42000 Liquid chromatography—Allen et al., 1994; Hajee and Haagsma, 1995; Turnipseed et al., 1995;
Roybal et al., 1995; Rushing and Hansen, 1997; Rushing and Thompson, 1997; Doerge at al.,
1998; Tarbin et al., 1998; Bergwerff and Scherpenisse, 2003; Andersen et al., 2004; Mitrowska
and Posyniak, 2004; Scherpenisse and Bergwerff, 2005; Valle et al., 2005; Andersen et al.,
2006; Lee et al., 2006; Dowling et al., 2007; Halme et al., 2007; Wu et al., 2007; Mitrowska
et al., 2008; Tarbin et al., 2008; Andersen et al., 2009; Long et al., 2009; Smith et al., 2009;
Martınez Bueno et al., 2010; Hurtaud-Pessel et al., 2011; Liu et al., 2011; Tao et al., 2011; Ascari
et al., 2012; Hashimoto et al., 2012; Chen et al., 2013; Nebot et al., 2013
Spectrophotometry—Safarik and Safarikova, 2002
ELISA—Yang et al., 2007; Xing et al., 2009; Oplatowska et al., 2011a; Shen et al., 2011; Singh
et al., 2011
Martius yellow 10315 Liquid chromatography—Yoshioka and Ichihashi, 2008
Metanil yellow 13065 Liquid chromatography—Fuh and Chia, 2002; Feng et al., 2011; Zhao et al., 2012; Bonan et al.,
2013
Methylene blue 52015 Liquid chromatography—Tarbin et al., 2008; Zhao et al., 2012
Methyl orange (acid orange 52) 13025 Liquid chromatography—Fang et al., 2013b
Methyl yellow (butter yellow, sudan yellow) 11020 Liquid chromatography—Sun et al., 2007; Feng et al., 2011; Zhao et al., 2012
ELISA—Oplatowska and Elliott, 2011
Napthol yellow S 10316 Liquid chromatography—Yoshioka and Ichihashi, 2008
New methylene blue 52030 Liquid chromatography—Tarbin et al., 2008
New red Liquid chromatography—Feng et al., 2011
Nile blue A 51180 Liquid chromatography—Tarbin et al., 2008
Orange I (acid orange 20) 14600 Liquid chromatography—Fuh and Chia, 2002; Yoshioka and Ichihashi, 2008; Fang et al., 2013b
(Continued on next page)
538 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Table 4. (Continued).
Color CI number Detection methods

Orange II (acid orange 7) 15510 Liquid chromatography—Fuh and Chia, 2002; Yoshioka and Ichihashi, 2008; Feng et al., 2011;
Zhao et al., 2012; Bonan et al., 2013; Fang et al., 2013b; Zou et al., 2013;
ELISA—Xue et al., 2012
Orange G 16230 Liquid chromatography—Yoshioka and Ichihashi, 2008
Orange RN 15970 Liquid chromatography—Yoshioka and Ichihashi, 2008
Para red 12070 Liquid chromatography—Stuart, 2006; Botek et al., 2007; Ertaş et al., 2007; Sun et al., 2007;
Uematsu et al., 2007; Mazzotti et al., 2008; Fan et al., 2009; Pardo et al., 2009; Liu et al., 2011;
Zhao et al., 2012
ELISA—Ju et al., 2008; Xu et al., 2010a; Chang et al., 2011; Liu et al., 2012; Qi et al., 2012; Shan
et al., 2012; Wang et al., 2012
Pararosaniline 42500 Liquid chromatography—Tarbin et al., 2008
Phloxine B 45410 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Ponceau 2R 16150 Liquid chromatography—Fuh and Chia, 2002; Yoshioka and Ichihashi, 2008; Feng et al., 2011;
Bonan et al., 2013
Ponceau 3R 16155 Liquid chromatography—Fuh and Chia, 2002; Yoshioka and Ichihashi, 2008; Feng et al., 2011
Ponceau 6R 16290 Liquid chromatography—Yoshioka and Ichihashi, 2008; Bonan et al., 2013
Ponceau SX 14700 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
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Ponceau xylidine 16150 Liquid chromatography—Zou et al., 2013


Quinoline yellow spirit soluble 47000 Spectrophotometry—Capitan et al., 1996
Red 2G (acid red 1, azophloxine) 18050 Liquid chromatography—Kirschbaum et al., 2003, 2006; Minioti et al., 2007; Yoshioka and
Ichihashi, 2008; Feng et al., 2011; Bonan et al., 2013; Zou et al., 2013
Capillary electrophoresis—Ryvolova et al., 2007
Red 10B 17200 Liquid chromatography—Yoshioka and Ichihashi, 2008
Rhodamine B 45170 Liquid chromatography—Stuart, 2006; Botek et al., 2007; Feng et al., 2011; Liu et al., 2011; Zhao
et al., 2012
ELISA—Oplatowska and Elliott, 2011
Rhodamine 6G 45160 Liquid chromatography—Tarbin et al., 2008; Liu et al., 2011
Rose bengal 45440 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Sudan I 12055 Liquid chromatography—Di Donna et al., 2004; Calbiani et al., 2004a, 2004b; Tateo and Bononi,
2004; Mazzetti et al., 2004; Puoci et al., 2005; Cornet et al., 2006; Stuart, 2006; Ma et al., 2006;
Zhang et al., 2006; Botek et al., 2007; Ertaş et al., 2007; He et al., 2007; Liu et al., 2007a;
Uematsu et al., 2007; Sun et al., 2007; Chailapakul et al., 2008; Mazzetti et al., 2008; Yu et al.,
2008; Fan et al., 2009; Murty et al., 2009; Pardo et al., 2009; Liu et al., 2011; Zhao et al., 2012;
Schummer et al., 2013
Gas chromatography—He et al., 2007
Capillary electrophoresis—Mejia et al., 2007
Voltammetry—Du et al., 2007; Gan et al., 2008; Lin et al., 2008; Mo et al., 2010
Amperometry—Liu et al., 2007b
Spectrophotometry—Capitan et al., 1996
Chemiluminescence—Liu et al., 2007c
Plasmon resonance light scattering—Wu et al., 2006
ELISA—Han et al., 2007; Ju et al., 2008; Anfossi et al., 2009; Wang et al., 2009; Xu et al., 2010a,
2010b; Chang et al., 2011; Wang et al., 2011; Xiao et al., 2011; Oplatowska et al., 2011c; Liu
et al., 2012; Qi et al., 2012; Shan et al., 2012
Flow injection chemiluminescence—Chen et al., 2010
Sudan II 12140 Liquid chromatography—Tateo and Bononi, 2004; Calbiani et al., 2004a, 2004b; Cornet et al.,
2006; Ma et al., 2006; Stuart, 2006; Zhang et al., 2006; Botek et al., 2007; Ertaş et al., 2007; He
et al., 2007; Sun et al., 2007; Uematsu et al., 2007; Liu et al., 2007a; Chailapakul et al., 2008;
Mazzotti et al., 2008; Yu et al., 2008; Fan et al., 2009; Murty et al., 2009; Pardo et al., 2009; Liu
et al., 2011; Zhao et al., 2012; Schummer et al., 2013
Gas chromatography—He et al., 2007
Capillary electrophoresis—Mejia et al., 2007
Amperometry—Liu et al., 2007b
Plasmon resonance light scattering—Wu et al., 2006
ELISA—Anfossi et al., 2009; Chang et al., 2011; Liu et al., 2012; Qi et al., 2012; Shan et al., 2012
Sudan III 26100 Liquid chromatography—Calbiani et al., 2004a, 2004b; Cornet et al., 2006; Ma et al., 2006;
Stuart, 2006; Zhang et al., 2006; Botek et al., 2007; Ertaş et al., 2007; He et al., 2007; Sun et al.,
2007; Uematsu et al., 2007; Liu et al., 2007a; Chailapakul et al., 2008; Mazzotti et al., 2008; Yu
et al., 2008; Fan et al., 2009; Murty et al., 2009; Pardo et al., 2009; Liu et al., 2011; Zhao et al.,
2012; Schummer et al., 2013
Gas chromatography—He et al., 2007
Capillary electrophoresis—Mejia et al., 2006
Amperometry—Liu et al., 2007b
Plasmon resonance light scattering—We et al., 2006
ELISA—Ju et al., 2008; Liu et al., 2008; Chang et al., 2011; Liu et al., 2012; Qi et al., 2012; Shan
et al., 2012
Sudan IV 26105 Liquid chromatography—Calbiani et al., 2004a, 2004b; Cornet et al., 2006; Ma et al., 2006;
Stuart, 2006; Zhang et al., 2006; Botek et al., 2007; Ertaş et al., 2007; He et al., 2007; Sun et al.,
2007; Uematsu et al., 2007; Liu et al., 2007a; Chailapakul et al., 2008; Mazzotti et al., 2008; Yu
et al., 2008; Fan et al., 2009; Murty et al., 2009; Pardo et al., 2009; Xinyi et al., 2009; Liu et al.,
2011; Zhao et al., 2012; Schummer et al., 2013
Gas chromatography—He et al., 2007
(Continued on next page)
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 539

Table 4. (Continued).
Color CI number Detection methods

Capillary electrophoresis—Mejia et al., 2007


Amperometry—Liu et al., 2007b
Plasmon resonance light scattering—Wu et al., 2006
ELISA—Chang et al., 2011; Liu et al., 2012; Qi et al., 2012; Shan et al., 2012
Sudan blue 2 61554 Liquid chromatography—Zhao et al., 2012
Sudan orange G 11920 Liquid chromatography—Botek et al., 2007; Sun et al., 2007; Pardo et al., 2009; Liu et al., 2011;
Zhao et al., 2012
Sudan red B 26110 Liquid chromatography—Sun et al., 2007
Sudan red 7B 26050 Liquid chromatography—Botek et al., 2007; Sun et al., 2007; Pardo et al., 2009; Liu et al., 2011;
Zhao et al., 2012
Sudan red G 12150 Liquid chromatography—Sun et al., 2007; Liu et al., 2011; Zhao et al., 2012
ELISA—Chang et al., 2011; Liu et al., 2011; 2012; Qi et al., 2012; Shan et al., 2012
Toluidine red 12120 Liquid chromatography—Liu et al., 2011; Zhao et al., 2012
Uranine 45350 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
Victoria blue B 44045 Liquid chromatography—Tarbin et al., 2008
Victoria pure blue BO 42595 Liquid chromatography—Tarbin et al., 2008
Victoria blue R 44040 Liquid chromatography—Tarbin et al., 2008
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Yellow 2G (acid yellow 17) 18965 Liquid chromatography—Yoshioka and Ichihashi, 2008; Feng et al., 2011
E 102 tartrazine 19140 Liquid chromatography—Chen et al., 1998; Fuh and Chia, 2002; Kirschbaum et al., 2003;
Gonzalez et al., 2003a, 2003b; Gianotti et al., 2005; Garcıa-Falcon and Simal-Gandara, 2005;
Kirschbaum et al., 2006; Ma et al., 2006; Vidotti et al., 2006; Minioti et al., 2007; Alves et al.,
2008; Yoshioka and Ichihashi, 2008; Culzoni et al., 2009; Feng et al., 2011; Khanavi et al., 2012;
Bonan et al., 2013; Harp et al., 2013; Hajimahmoodi et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Perez-Urquiza and Beltran, 2000; Huang et al., 2002,
2003, 2005; Jager et al., 2005; Lee et al., 2008
Voltammetry—Ni et al., 1996, 1997; Silva et al., 2007; Song et al., 2010; Ghoreishi et al., 2011,
2012; Medeiros et al., 2012a, 2012b
Spectrophotometry—Ni and Gong, 1997; Capitan-Vallvey et al., 1998; Vidotti et al., 2005; Llamas
et al., 2009; Ni et al., 2009; Aktas and Ertokus, 2011
Photoacoustic spectroscopy—Coelho et al., 2010
ELISA—Lei et al., 2013
E 104 quinoline yellow 47005 Liquid chromatography—Kirschbaum et al., 2003; Garcıa-Falcon and Simal-Gandara, 2005;
Gianotti et al., 2005; Kirschbaum et al., 2006; Minioti et al., 2007; Yoshioka and Ichihashi, 2008;
Feng et al., 2011; Khanavi et al., 2012; Bonan et al., 2013; Hajimahmoodi et al., 2013
Spectrophotometry—Capitan et al., 1996
E 110 sunset yellow FCF 15985 Liquid chromatography—Chen et al., 1998; Fuh and Chia, 2002; Kirschbaum et al., 2003; Garcıa-
Falcon and Simal-Gandara, 2005; Gianotti et al., 2005; Kirschbaum et al., 2006; Ma et al., 2006;
Vidotti et al., 2006; Minioti et al., 2007; Alves et al., 2008; Yoshioka and Ichihashi, 2008;
Culzoni et al., 2009; Feng et al., 2011; Khanavi et al., 2012; Bonan et al., 2013; Hajimahmoodi
et al., 2013; Harp et al., 2013; Zou et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Perez-Urquiza and Beltran, 2000; Huang et al., 2002;
Del Giovine and Bocca, 2003; Huang et al., 2003, Huang et al., 2005; Jager et al., 2005; Lee
et al., 2008
Voltammetry—Ni et al., 1996; Nevado et al., 1997; Ni and Bai, 1997; Ni et al., 1997; Silva et al.,
2007; Song, 2010; Ghoreishi et al., 2012; Medeiros et al., 2012a, 2012b
Spectrophotometry—Capitan et al., 1996; Ni and Gong, 1997; Capitan-Vallvey et al., 1998;
Vidotti et al., 2005; Llamas et al., 2009; Ni et al., 2009; Aktas and Ertokus, 2011
Photoacoustic spectroscopy—Coelho et al., 2010
ELISA—Xing et al., 2012
E 122 azorubine 14720 Liquid chromatography—Gennaro et al., 1997; Kirschbaum et al., 2003; Garcıa-Falcon and
Simal-Gandara, 2005; Gianotti et al., 2005; Kirschbaum et al., 2006; Minioti et al., 2007;
Yoshioka and Ichihashi, 2008; Feng et al., 2011; Khanavi et al., 2012; Bonan et al., 2013;
Hajimahmoodi et al., 2013
Capillary electrophoresis—Del Giovine and Bocca, 2003; Jager et al., 2005; Ryvolova et al., 2007
Differential pulse polarography—Chanlon et al., 2005
E 123 amaranth 16185 Liquid chromatography—Gennaro et al., 1997; Chen et al., 1998; Fuh and Chia, 2002;
Kirschbaum et al., 2003; Gianotti et al., 2005; Kirschbaum et al., 2006; Ma et al., 2006; Minioti
et al., 2007; Alves et al., 2008; Yoshioka and Ichihashi, 2008; Culzoni et al., 2009; Feng et al.,
2011; Bonan et al., 2013
Capillary electrophoresis—Perez-Urquiza and Beltran, 2000; Jager et al., 2005; Ryvolova et al.,
2007; Lee et al., 2008
Voltammetry – Ni et al., 1996, 1997; Ni and Bai, 1997
Spectrophotometry—Nevado et al., 1995; Ni and Gong, 1997; Vidotti et al., 2005; Llamas et al.,
2009; Ni et al., 2009
E 124 ponceau 4R 16255 Liquid chromatography—Gennaro et al., 1997; Chen et al., 1998; Fuh and Chia, 2002;
Kirschbaum et al., 2003; Garcıa-Falcon and Simal-Gandara, 2005; Gianotti et al., 2005;
Kirschbaum et al., 2006; Ma et al., 2006; Minioti et al., 2007; Yoshioka and Ichihashi, 2008;
Feng et al., 2011; Khanavi et al., 2012; Bonan et al., 2013; Hajimahmoodi et al., 2013; Zou
et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Perez-Urquiza and Beltran, 2000; Huang et al., 2002,
2003, Del Giovine and Bocca, 2003; 2005; Jager et al., 2005; Ryvolova et al., 2007; Lee et al.,
2008
Voltammetry—Ni et al., 1996, 1997

(Continued on next page)


540 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Table 4. (Continued).
Color CI number Detection methods

Spectrophotometry—Nevado et al., 1995; Ni and Gong, 1997; Capitan-Vallvey et al., 1998; Ni


et al., 2009
Differential pulse polarography—Chanlon et al., 2005
E 127 erythrosine 45430 Liquid chromatography—Kirschbaum et al., 2003; Gonzalez et al., 2003a; Kirschbaum et al.,
2006; Minioti et al., 2007; Yoshioka and Ichihashi, 2008; Feng et al., 2011; Harp et al., 2013;
Zou et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Jager et al., 2005; Ryvolova et al., 2007; Lee et al.,
2008
E 129 allura red AC 16035 Liquid chromatography—Chen et al., 1998; Fuh and Chia, 2002; Kirschbaum et al., 2003, 2006;
Minioti et al., 2007; Alves et al., 2008; Yoshioka and Ichihashi, 2008; Feng et al., 2011; Khanavi
et al., 2012; Bonan et al., 2013; Hajimahmoodi et al., 2013; Harp et al., 2013; Zou et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Perez-Urquiza and Beltran, 2000; Huang et al., 2002,
2003, 2005; Jager et al., 2005; Lee et al., 2008
Voltammetry—Silva et al., 2007
Spectrophotometry—Aktas and Ertokus, 2011
Differential pulse polarography—Chanlon et al., 2005
E 131 patent blue V 42051 Liquid chromatography—Kirschbaum et al., 2003, 2006; Gianotti et al., 2005; Minioti et al.,
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2007; Yoshioka and Ichihashi, 2008; Feng et al., 2011; Bonan et al., 2013
Capillary electrophoresis—Perez-Urquiza and Beltran, 2000; Jager et al., 2005; Dossi et al., 2007
E 132 indigotine/indigo carmine 73015 Liquid chromatography—Chen et al., 1998; Gonzalez et al., 2003a, 2003b; Kirschbaum et al.,
2003, 2006; Minioti et al., 2007; Yoshioka and Ichihashi, 2008; Feng et al., 2011; Khanavi et al.,
2012; Bonan et al., 2013; Hajimahmoodi et al., 2013; Harp et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Huang et al., 2002, 2003, 2005; Jager et al., 2005;
Lee et al., 2008
E 133 brilliant blue FCF 42090 Liquid chromatography—Chen et al., 1998; Kirschbaum et al., 2003; Gonzalez et al., 2003a,
2003b; Gianotti et al., 2005; Kirschbaum et al., 2006; Vidotti et al., 2006; Minioti et al., 2007;
Alves et al., 2008; Yoshioka and Ichihashi, 2008; Feng et al., 2011; Khanavi et al., 2012; Bonan
et al., 2013; Harp et al., 2013; Hajimahmoodi et al., 2013
Capillary electrophoresis—Kuo et al., 1998; Huang et al., 2002, 2003, 2005; Jager et al., 2005;
Lee et al., 2008
Voltammetry—Ghoreishi et al., 2011; Medeiros et al., 2012a, 2012b
Spectrophotometry—Ni and Gong, 1997; Vidotti et al., 2005; Ni et al., 2009
Photoacoustic spectroscopy—Coelho et al., 2010
E 142 green S 44090 Liquid chromatography—Kirschbaum et al., 2003; Gonzalez et al., 2003a, 2003b; 2006; Minioti
et al., 2007; Yoshioka and Ichihashi, 2008; Feng et al., 2011
Capillary electrophoresis—Dossi et al., 2007
E 151 brilliant Black BN 28440 Liquid chromatography—Gonzalez et al., 2003a, 2003b; Kirschbaum et al., 2003, 2006

while 25% in urban area) probably due to the less frequent was found in 9 out of 51 fishery products that should not con-
sampling and analysis of samples. This high level occurrence of tain this dye according to the EU legislation (Bonan et al.,
illegal synthetic colors shows the potential scale of the problem 2013). Carcinogenic chrysoidine has been demonstrated to be
in Asian countries and indeed across the Developing World. used illegally as a dye in soybean milk or to dye low-cost fish to
Another Indian study (Rao and Sudershan, 2008) reported the imitate expensive and superior in quality yellow-fin tuna
increase in usage of some permitted synthetic colors in food (Wang et al., 2008; Reyns et al., 2010; Gui et al., 2010). Chrysoi-
that may lead to exceeding the ADIs. The illegal dyes (namely, dine has also antimicrobial and antiseptic properties and as
fast red, amaranth, rhodamine B, orange II, and auramine) such it has been applied to disinfect fish skin in some Asian
were also identified in some foods analyzed. In the study per- countries (Reyns et al., 2010).
formed by Dixit et al. (2013) the illegal synthetic colours such
as rhodamine B, metanil yellow, orange II, and malachite green
11.2. Dyes—Illegal veterinary drugs
were found in 16.4% food samples collected in different regions
of India in addition to excessive amount of legal colorants iden- Monitoring programs for carcinogenic triphenylmethane
tified in 58% of samples. Due to the common occurrence of dyes: malachite green and crystal violet are already in place
illegal dyes in food the Times of India advices how to detect in Europe and the United States. However, there are a
food adulteration with illegal dyes in ordinary kitchen (Times number of dyes belonging to this group with similar prop-
of India, 2012). The author suggests that illegal metanil yellow erties that can be used as alternatives and may not be
in turmeric can be exposed by dissolving spices in water and detected in these monitoring programmes. Tarbin et al.
adding any commonly available acid as metanil yellow should (2008) suggested 11 other compounds belonging to triaryl-
turn purple, violet, or pink under acidic conditions. The pres- methanes, xanthenes, and phenothiazine groups that should
ence of malachite green on green vegetables can be detected by be under suspicion, i.e., brilliant green, ethyl violet, pararos-
simply placing food on moistened white paper. The adultera- aniline, victoria blue B, victoria blue R, victoria pure blue
tion with malachite green is indicated by formation of the col- BO, rhodamine 6G, methylene blue, azure B, new methy-
ored impressions. lene blue, and nile blue. One of these compounds—victoria
Dyes can be also added illegally to foodstuffs to compensate pure blue BO appeared on RASFF in 2010 as it was found
for their low quality. In a recent study, the synthetic dye E154 in fish imported from Vietnam.
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 541

11.3. Color migration The sudan scare in 2003 and contamination of hundreds of
products with illegal sudan dyes demonstrates the need for rig-
The migration of a color from the package material or other
orous monitoring programs and identifying and targeting of
food contact materials has been recorded on RASFF since 2005
possible hazards. Currently, a number of analytical methods
(RASFF online database). RASFF does not generally give details
have been developed for the analysis of food colors and a num-
about the identity of the dye that was detected in food as a
ber of companies across Europe and the United States provide
result of the migration. These are most probably dyes used in
testing services for detecting illegal dyes present in foods. Nev-
industrial applications, for example, dying cutlery, napkins, or
ertheless, there is still a clear need for additional research and
wrappings and should not be consumed by humans. A recent
monitoring activities to better protect the consumer. Therefore,
study demonstrated the migration of synthetic color brilliant
another challenge in the area of food colors is identification of
green from green paper towels (Oplatowska et al., 2011b). Bril-
known and emerging dye adulterants/contaminants in food,
liant green is a triphenylmethane dye that is likely to have simi-
not only in the Developed World but as a matter of priority in
larly toxic properties as the known illegal veterinary drug
the Developing World is needed. To support this need the
malachite green. A measurable amount of the paper towel dye
availability of rapid and low cost multicolorant screening and
was shown to migrate from the towel through the skin when
confirmatory methods is identified as a priority.
the towel was used for hand drying. Additionally, it was also
Further exposure assessments of legal synthetic colors, espe-
demonstrated that large amounts of color can accumulate in
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cially in children are required to better understand the link


food (fish was used as a model) when towels containing dye
between consumption and adverse health effects. Without this
were used for wrapping. This study raised a concern about the
data the ability to protect the consumer, especially the most
safety of use of dyed paper towels for hygiene purposes and in
vulnerable (children) is highly compromised.
food preparation area.
A previously unidentified mean of exposure to legal syn-
thetic colors was demonstrated in a study performed by Lucova References
et al. (2013). Patent blue V (E131) and brilliant blue (E133)
Abraham, K., Gurtler, R., Berg, K., Heinemeyer, G., Lampen, A. and Appel,
were shown to directly enter the epithelium and then possibly K. E. (2011). Toxicology and risk assessment of 5-hydroxymethylfurfu-
the bloodstream through the tongue from the saliva when used, ral in food. Mol. Nutr. Food Res. 55:667–678.
for example, in lollipops. These dyes could also penetrate the Aktas, A. H. and Ertokus, G. P. (2011). Spectral simultaneous determina-
shaven skin when used in aftershave products. This type of tion of tartazine, allura red, sunset yellow and caramel in drink sample
exposure does not include gastrointestinal tract degradation by chemometric method. Rev. Anal. Chem. 29:107–116.
Allen, J., Gofus, J. and Meinertz, J. (1994). Determination of malachite
and result in direct access of the dyes to the systemic circula- green residues in the eggs, fry and adult muscle tissue of rainbow trout.
tion. The authors concluded that due to the systemic availabil- J. AOAC Int. 77:553–557.
ity these compounds should not be used in topical products Alves, S. P., Brum, D. M., de Andrade, E.  C. B. and Netto, A. D. P. (2008).
intended for use on slightly damaged skin and for confection- Determination of synthetic dyes in selected foodstuffs by high perfor-
ary and lollipops for licking. Currently E131, E133, and other mance liquid chromatography with UV-DAD detection. Food Chem.
107:489–496.
synthetic dyes are commonly used in cosmetics, oral mouth- Andersen, W. C., Roybal, J. E. and Turnipseed, S. B. (2004). Determination
washes, pharmaceutical lozenges, and confectionary. of malachite green and leucomalachite green ins with in-situ oxidation
and liquid chromatography with visible detection. F&DA Laboratory
Information Bulletin No. 4334.
12. Conclusions and summary Andersen, W. C., Turnipseed, S. B., Karbiwnyk, C. M., Lee, R. H., Clark, S.
B., Rowe, W. D., Madson, M. R. and Miller, K. E. (2007). Quantitative
The use of synthetic colors in food has resulted in a substantial and confirmatory analyses of crystal violet (gentian violet) and brilliant
amount of negative press in recent years due to the possible green in fish. F&DA Laboratory Information Bulletin No. 4395. Avail-
able at http://www.fda.gov/Food/FoodScienceResearch/LaboratoryMe
harmful side effects. One of the most important issues concern- thods/ucm071574.htm
ing the legal synthetic food colors is that there is still no defini- Andersen, W. C., Turnipseed, S. B., Karbiwnyk, C. M., Lee, R. H., Clark, S.
tive answer if these dyes play any role in hyperactive behavior B., Rowe, W. D., Madson, M. R. and Miller, K. E. (2009). Multiresidue
in children. However, due to the current suspicions there is a method for the triphenylmethane dyes in fish: Malachite green, crystal
trend to remove them from the food supply chain. The volun- (gentian) violet, and brilliant green. Anal. Chim. Acta 637:279–289.
Andersen, W. C., Turnipseed, S. B. and Roybal, J. E. (2006). Quantitative
tary withdrawal action in the UK supported by the Food and and confirmatory analyses of malachite green and leucomalachite green
Standards Agency has already resulted in major food suppliers residues in fish and shrimp. J. Agric. Food Chem. 54:4517–4523.
changing from synthetic colors to natural products, especially Anfossi, L., Baggiani, C., Giovannoli, C. and Giraudi, G. (2009). Develop-
in confectionery. However, the replacement is not always ment of enzyme-linked immunosorbent assays for sudan dyes in chilli
straightforward and not all natural colors are completely safe. powder, ketchup and egg yolk. Food Addit. Contam. 26:800–807.
Arnold, D., LeBizec, B. and Ellis, R. (2009). Malachite green in Residue
Food globalization has resulted in humans consuming foods evaluation of certain veterinary drugs. FAO JECFA Monographs 6.
from many different parts of the world. Another important Available from ftp://ftp.fao.org/docrep/fao/011/i0659e/i0659e.pdf.
issue is the lack of uniform regulations on food colors what Accessed August 1, 2012.
causes disruption to the international trade. Additionally, due Arnold, L.A., Lofthouse, N. and Hurt, E. (2012). Artificial food colors and
to the lack of uniform control policies worldwide, the distinct attention-deficit/hyperactivity symptoms: Conclusions to dye for. Neu-
rotherapeutics 9:599–609.
possibility of illegal and harmful chemicals being present in Ascari, J., Dracz, S., Santos, F. A., Lima, J. A., Diniz, M. H. and Vargas, E.
foods locally produced or imported cannot be ruled out and A. (2012). Validation of an LC-MS/MS method for malachite green
indeed is quite likely, particularly in the Developing World. (MG), leucomalachite green (LMG), crystal violet (CV) and
542 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

leucocrystal violet (LCV) residues in fish and shrimp. Food Addit. Con- Coelho, T. M., Vidotti, E. C., Rollemberg, M. C., Medina, N., Baesso, M. L.,
tam. Pt. A 29:602–608. Cella, N. and Bento, C. (2010). Photoacoustic spectroscopy as a tool for
Baldwin, J. L., Chou, A. H. and Solomon, W. R. (1997). Popsicle-Induced determination of food dyes: Comparison with first derivative spectro-
Anaphylaxis Due to Carmine Dye Allergy. Ann. Allergy, Asthma photometry. Talanta 81:202–207.
Immunol. 79:415–419. Commission Decision (2004/25/EC). Commission Decision of 22 Decem-
Bateman, B., Warner, J. O., Hutchinson, E., Dean, T., Rowlandson, P., ber 2003 amending Decision 2002/657/EC as regards the setting of
Gant, C., Grundy, J., Fitzgerald, C. and Stevenson, J. (2004). The effects minimum required performance limits (MRPLs) for certain residues in
of a double blind, placebo controlled, artificial food colourings and food of animal origin. Off. J. Eur. Union L 6:38–39.
benzoate preservative challenge on hyperactivity in a general popula- Commission Regulation (EC) No 884 (2007). Commission Regulation
tion sample of preschool children. Arch. Dis. Childhood. 89:506–511. (EC) No 884/2007 of 26 July 2007 on emergency measures suspending
Bergwerff, A. and Scherpenisse, P. (2003). Determination of residues of the use of E 128 red 2G as food colour. Off. J. Eur. Union L 195:8–9.
malachite green in aquatic animals. J. Chromatogr. B 788:351–359. Commission Regulation (EC) No 775 (2008). Commission Regulation
Bonan, S., Fedrizzi, G., Menotta, S. and Elisabetta, C. (2013). Simultaneous (EC) No 775/2008 of 4 August 2008 establishing maximum residue
determination of synthetic dyes in foodstuffs and beverages by high- limits for the feed additive canthaxanthin in addition to the conditions
performance liquid chromatography coupled with diode-array detec- provided for in Directive 2003/7/EC. Off. J. Eur. Union L 207:5–6.
tor. Dyes Pigments 99:36–40. Commission Regulation (EU) No 257 (2010). Commission Regulation
Botek, P., Poustka, J. and Hajslova, J. (2007). Determination of banned (EU) No 257/2010 of 25 March 2010 setting up a programme for the
dyes in spices by liquid chromatography – mass spectrometry. Czech J. re-evaluation of approved food additives in accordance with Regulation
Food Sci. 25:17–24. (EC) No 1333/2008 of the European Parliament and of the Council on
Downloaded by [Universidad Nacional Colombia] at 16:11 05 September 2017

Breithaupt, D. E. (2004). Simultaneous HPLC determination of carote- food additives. Off. J. Eur. Union L 80:19–27.
noids used as food coloring additives: Applicability of accelerated sol- Commission Regulation (EU) No 1129 (2011). Commission Regulation (EU)
vent extraction. Food Chem. 86:449–456. No 1129/2011 of 11 November 2011 amending Annex II to Regulation
Calbiani, F., Careri, M., Elviri, L., Mangia, A., Pistara, L. and Zagnoni, I. (EC) No 1333/2008 of the European Parliament and of the Council by
(2004a). Development and in-house validation of a liquid chromatog- establishing a Union list of food additives. Off. J. Eur. Union L 295:1–177.
raphy–electrospray–tandem mass spectrometry method for the simul- Committee on Toxicity of Chemicals in Food, Consumer Products and the
taneous determination of sudan I, sudan II, sudan III and sudan IV in Environment (COT) (2007). Statement on research project (T07040)
hot chilli products. J. Chromatogr. A 1042:123–130. investigating the effect of mixtures of certain food colours and a preser-
Calbiani, F., Careri, M., Elviri, L., Mangia, A. and Zagnoni, I. (2004b). vative on behaviour in children. Available from http://cot.food.gov.uk/
Accurate mass measurements for the confirmation of sudan azo-dyes pdfs/colpreschil.pdf. Accessed June 1, 2012.
in hot chilli products by capillary liquid chromatography–electrospray Cornet, V., Govaert, Y., Moens, G., Van Loco, J. and Degroodt, J. (2006).
tandem quadrupole orthogonal-acceleration time of flight mass spec- Development of a fast analytical method for the determination of
trometry. J. Chromatogr. A 1058:127–135. sudan dyes in chili- and curry-containing foodstuffs by high-perfor-
Capitan, F., Capitan-Vallvey, L. F., Fernandez, M. D., de Orbe, I. and Avi- mance liquid chromatography-photodiode array detection. J. Agric.
dad, R. (1996). Determination of colorant matters mixtures in foods by Food Chem. 54:639–644.
solid-phase spectrophotometry. Anal. Chim. Acta 33:141–148. Council Directive 62/2645/EEC of 23 October 1962 on the approximation
Capitan-Vallvey, L. F., Fernandez, M. D., de Orbe, I. and Avidad, R. (1998). of the rules of the Member States concerning the colouring matters
Simultaneous determination of the colorants tartrazine, ponceau 4R authorized for use in foodstuffs intended for human consumption. Off.
and sunset yellow FCF in foodstuffs by solid phase spectrophotometry J. Eur. Commun. 115:2645–2654.
using partial least squares multivariate calibration. Talanta 47:861–868. Council Directive 76/399/EEC of 6 April 1976 making a fifth amendment
CBSNews (2012). “Starbucks Strawberry Frappuccinos dyed with crushed to the Council Directive of 23 October 1962 on the approximation of
up cochineal bugs, report says,” Available from http://www.cbsnews. the rules of the Member States concerning the colouring matters autho-
com/8301-504763_162-57405140-10391704/starbucks-strawberry-frap rized for use in foodstuffs intended for human consumption. Off. J.
puccinos-dyed-with-crushed-up-cochineal-bugs-report-says. Accessed Eur. Commun. L 108:19–20.
June 1, 2013. Culp, S. J., Beland, F. A., Heflich, R. H., Benson, R. W., Blankenship, L. R.,
Ceyhan, B. M., Gultekin, F., Doguc, D. K. and Kulac, E. (2013). Effects of Webb, P. J., Mellick, P. W., Trotter, R. W., Shelton, S. D., Greenlees, K.
maternally exposed coloring food additives on receptor expressions J. and Manjanatha, M. G. (2002). Mutagenicity and carcinogenicity in
related to learning and memory in rats. Food Chem. Toxicol. 56:145–148. relation to DNA adduct formation in rats fed leucomalachite green.
Chailapakul, O., Wonsawat, W., Siangproh, W., Grudpan, K., Zhao, Y. and Mutat. Res. 506–507:55–63.
Zhu, Z. (2008). Analysis of sudan I, sudan II, sudan III, and sudan IV Culp, S. J., Blankenship, L. R., Kusewitt, D. F., Doerge, D. R., Mulligan, L.
in food by HPLC with electrochemical detection: Comparison of glassy T. and Beland, F. A. (1999). Toxicity and metabolism of malachite
carbon electrode with carbon nanotube-ionic liquid gel modified elec- green and leucomalachite green during short-term feeding to fischer
trode. Food Chem. 109:876–882. 344 rats and B6C3F1 mice. Chem. Biol. Interact. 122:153–170.
Chang, X. C., Hu, X. Z., Li, Y. Q., Shang, Y. J., Liu, Y. Z., Feng, G. and Culp, S. J., Mellick, P. W., Trotter, R. W., Greenlees, K. J., Kodell, R. L. and
Wang, J. P. (2011). Multi-determination of Para red and Sudan dyes in Beland, F. A. (2006). Carcinogenicity of malachite green chloride and
egg by a broad specific antibody based enzyme linked immunosorbent leucomalachite green in B6C3F1 mice and F344 rats. Food Chem. Toxi-
assay. Food Control. 22:1770–1775. col. 44:1204–1212.
Chanlon, S., Joly-Pottuz, L., Chatelut, M., Vittori, O. and Cretier, J. L. Culzoni, M. J., Schenone, A. V., Llamas, N. E., Garrido, M., Di Nezio, M. S.,
(2005). Determination of carmoisine, allura red and ponceau 4R in Fernandez, B. S. and Goicoechea, H. C. (2009). Fast chromatographic
sweets and soft drinks by differential pulse polarography. J. Food Com- method for the determination of dyes in beverages by using high per-
posit. Anal. 18:503–515. formance liquid chromatography — diode array detection data and
Chen, D., Song, Z. and Yue, Q. (2010). Sensitive assay for picogram levels second order algorithms. J. Chromatogr. A 1216:7063–7070.
of sudan I in chilli foodstuffs by flow injection chemiluminescence. Del Giovine, L. and Bocca, A. P. (2003). Determination of synthetic dyes in
Anal. Method. 2:1316–1319. ice-cream by capillary electrophoresis. Food Control. 14:131–135.
Chen, L., Lu, Y., Li, S., Lin, X., Xu, Z. and Dai, Z., (2013). Application of Di Donna, L., Maiuolo, L., Mazzotti, F., De Luca, D. and Sindona, G.
graphene-based solid-phase extraction for ultra-fast determination of (2004). Assay of sudan I contamination of foodstuff by atmospheric
malachite green and its metabolite in fish tissues. Food Chem. pressure chemical ionization tandem mass spectrometry and isotope
141:1383–1389. dilution. Anal. Chem. 76:5104–5108.
Chen, Q., Mou, S., Hou, X., Riviello, J. M. and Ni, Z. (1998). Determination Dixit, S., Khanna S. K. and Das, M. (2013). All India survey for analyses of
of eight synthetic food colorants in drinks by high-performance ion colors in sweets and savories: Exposure risk in Indian population. J.
chromatography. J. Chromatogr. A 827:73–81. Food Sci. 78:T642–T647.
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 543

Doerge, D. R., Churchwell, M. I., Gehring, T. A., Pu, Y. M. and Plakas, S. powder, chilli oil and food additive combined with high performance
M. (1998). Analysis of malachite green and metabolites in fish using liquid chromatography. Anal. Chim. Acta 650:65–69.
liquid chromatography atmospheric pressure chemical ionization mass Fang, G., Feng, J., Yan, Y., Liu, C. and Wang, S. (2014). Highly selective
spectrometry. Rapid Commun. Mass Spectrom. 12:1625–1634. determination of chrysoidine in foods through a surface molecularly
Dossi, N., Toniolo, R., Pizzariello, A., Susmel, S., Perennes, F. and Bontem- imprinted sol-gel polymer solid-phase extraction coupled with HPLC.
pelli, G. (2007). A capillary electrophoresis microsystem for the rapid Food Anal. Method. 7:345–351.
in-channel amperometric detection of synthetic dyes in food. J. Elec- Fang, G., Wu, Y., Dong, X., Liu, C., He, S. and Wang, S. (2013b). Simulta-
troanal. Chem. 601:1–7. neous determination of banned acid orange dyes and basic orange dyes
Dowling, G., Mulder, P., Duffy, C., Regan, L. and Smyth, M. (2007). Con- in foodstuffs by liquid chromatography¡tandem electrospray ioniza-
firmatory analysis of malachite green, leucomalachite green, crystal vio- tion mass spectrometry via negative/positive ion switching mode. J
let and leucocrystal violet in salmon by liquid chromatography-tandem Agric. Food Chem. 61:3834–3841.
mass spectrometry. Anal. Chim. Acta 586:411–419. Feingold, B. F. (1975). Hiperkinesis and learning disabilities linked to arti-
Downham, A. and Collins, P. (2000). Colouring our foods in the last and ficial food flavours and colours. Am. J. Nur. 75:797–803.
next millennium. Int. J. Food Sci. Technol. 35:5–22. Feng, F., Zhao, Y., Yong, W., Sun, L., Jiang, G. and Chu, X. (2011). Highly
Du, M., Han, X., Zhou, Z. and Wu, S. (2007). Determination of sudan I in sensitive and accurate screening of 40 dyes in soft drinks by liquid
hot chili powder by using an activated glassy carbon electrode. Food chromatography–electrospray tandem mass spectrometry. J. Chroma-
Chem. 105:883–888. togr. B 879:1813–1818.
Electronic Code of Federal Regulations (e-CFR). (2009). Available from Food and Drug Administration (F&DA) (2011a). Available from
http://ecfr.gpoaccess.gov. Accessed November 1, 2012. http://www.fda.gov/AdvisoryCommittees/CommitteesMeetingMateri
Downloaded by [Universidad Nacional Colombia] at 16:11 05 September 2017


Ertaş, E., Ozer, H. and Alasalvar, C. (2007). A rapid HPLC method for als/FoodAdvisoryCommittee/ucm250901.htm. Food Advisory Com-
determination of sudan dyes and para red in red chilli pepper. Food mittee Meeting Minutes March 30-31, 2011. Certified Color Additives
Chem. 105:756–760. in Food and Possible Association with Attention Deficit Hyperactivity
Eurofins. (2013). Sudan dyes in spices in food. Available from http://www. Disorder in Children. Accessed November 1, 2012.
eurofins.de/media/2717988/sudan_dyes_in_food.pdf. Accessed June 1, Food and Drug Administration (2011b). Background document for the
2013. Food Advisory Committee: Certified color additives in food and possi-
European Food Safety Authority (EFSA). (2005). Opinion of the Scientific ble association with attention deficit hyperactivity disorder in children,
Panel on Food Additives, Flavourings, Processing Aids and Materials March 30–31, 2011. Available from http://www.fda.gov/downloads/
in Contact with Food on a request from the Commission to review the AdvisoryCommittees/CommitteesMeetingMaterials/FoodAdvisory
toxicology of a number of dyes illegally present in food in the EU. Committee/UCM248549.pdf. Accessed February 1, 2013.
EFSA J. 263:1–71. Food and Drug Administration (2013a). Listing of color additives exempt
European Food Safety Authority (EFSA). (2007). Opinion of the Scientific from certification; Spirulina extract. Fed. Reg. 78:49177–49120 Avail-
Panel on Food Additives, Flavourings, Processing Aids and Materials able from https://federalregister.gov/a/2013-19550. Accessed Septem-
in Contact with Food on the food colour red 2G (E128) based in a ber 9, 2013.
request from the Commission related to the re-evaluation of all permit- Food and Drug Administration (2013b). Detention without physical exam-
ted food additives. EFSA J. 515:1–28. ination and guidance of foods containing illegal and/or undeclared col-
European Food Safety Authority (EFSA). (2008). Assessment of the results ors. Import Alert 45-02, last updated 09/06/2013. Available from
of the study by McCann et al. (2007) on the effect of some colours and http://www.accessdata.fda.gov/cms_ia/importalert_118.html. Accessed
sodium benzoate on children’s behaviour. Scientific Opinion of the September 7, 2013.
Panel on Food Additives, Flavouring, Processing Aids and Food Con- Food and Drug Administration (2013c). Detention without physical exam-
tact Materials. EFSA J. 660:1–54. ination of aquaculture seafood products due to unapproved drugs.
European Food Safety Authority (EFSA). (2009a). Scientific opinion on the Import Alert 16-124. Last updated 09/06/2013. Available from http://
re-evaluation of allura red AC (E 129) as a food additive. EFSA J. www.accessdata.fda.gov/cms_ia/importalert_27.html. Accessed Sep-
7(11):1327,1–39. tember 7, 2013.
European Food Safety Authority (EFSA). (2009b). Scientific opinion on the Food Navigator (2010). Spirulina faces legal questions. Available from
re-evaluation of ponceau 4R (E 124) as a food additive. EFSA J. http://www.foodnavigator.com/Legislation/Spirulina-faces-legal-ques
7(11):1328,1–39. tions. Accessed June 1, 2013.
European Food Safety Authority (EFSA). (2009c). Scientific opinion on Food Navigator (2011). Available from http://www.foodnavigator.com/Sci
the re-evaluation of quinoline yellow (E 104) as a food additive. ence-Nutrition/Wild-adds-Spirulina-derived-blue-hue-to-colouring-
EFSA J. 7(11):1329,1–40. foodstuffs-portfolio. Wild adds Spirulina-derived blue hue to colouring
European Food Safety Authority (EFSA). (2009d). Scientific opinion on the foodstuffs portfolio. Accessed June 1, 2013.
re-evaluation of sunset yellow FCF (E 110) as a food additive. EFSA J. Food Standards Agency (FSA). (2006). Study on illegal dyes in imported
7(11):1330,1–44. foods. Available from http://www.food.gov.uk/multimedia/pdfs/illegal
European Food Safety Authority (EFSA). (2009e). Scientific opinion on the dyereport.pdf. Accessed June 1, 2012.
re-evaluation tartrazine (E 102). EFSA J. 7(11):1331,1–52. Food Standards Agency (FSA). (2007). Report of the sudan I review panel.
European Food Safety Authority (EFSA). (2009f). Scientific opinion on the Available from www.food.gov.uk/multimedia/pdfs/sudanreview.pdf.
re-evaluation of azorubine/Carmoisine (E 122) as a food additive. Accessed June 1, 2012.
EFSA J. 7(11):1332,1–40. Food Standards Agency (FSA). (2008a). Food additives and hyperactivity.
European Food Safety Authority (EFSA). (2010). Scientific opinion on the 10 April 2008. Available from http://www.food.gov.uk/multimedia/
re-evaluation of canthaxanthin (E161g) as a food additive. EFSA J. pdfs/board/fsa080404a.pdf. Accessed November 1, 2012.
8(10):1852,1–42 Food Standards Agency (FSA). (2008b). Board discuses colours advice.
European Food Safety Authority (EFSA). (2011). Scientific opinion on the Available from http://www.food.gov.uk/news/newsarchive/2008/apr/
re-evaluation of caramel colours (E 150 a,b,c,d) as food additives. EFSA coloursadvice. Accessed June 1, 2012.
J. 9(3):2004, 1–103 Food Standards Agency (FSA). (2011). Guidelines on approaches to the
European Food Safety Authority (EFSA). (2013). Statement on Allura Red replacement of Tartrazine, Allura Red, Ponceau 4R, Quinoline Yellow,
AC and other sulphonated mono azo dyes authorised as food and feed Sunset Yellow and Carmoisine in food and beverages. Available from
additives. EFSA J. 11(6):3234, 1–25. http://www.food.gov.uk/multimedia/pdfs/publication/guidelinessoton
European Parliament and Council Directive 94/36/EC of 30 June 1994 on sixcolours.pdf. Accessed June 1, 2013.
colours for use in foodstuffs. Off. J. Eur. Union. L 237:13–29. Fuh, M. and Chia, K. (2002). Determination of sulphonated azo dyes in
Fan, Y., Chen, M., Shentu, C., El-Sepai, F., Wang, K., Zhu, Y. and Ye, M. food by ion-pair liquid chromatography with photodiode array and
(2009). Ionic liquids extraction of para red and sudan dyes from chilli electrospray mass spectrometry detection. Talanta 56:663–671.
544 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Gan, T., Li, K. and Wu, K. (2008). Multi-wall carbon nanotube-based elec- Huang, H., Shih, Y. and Chen, Y. (2002). Determining eight colorants in
trochemical sensor for sensitive determination of sudan I. Sensors milk beverages by capillary electrophoresis. J. Chromatogr. A 959:317–
Actuators B-Chem. 132:134–139. 325.
Garcıa-Falcon, M. and Simal-Gandara, J. (2005). Determination of food Hurtaud-Pessel, D., Cou€edor, P. and Verdon, E. (2011). Liquid chromatog-
dyes in soft drinks containing natural pigments by liquid chromatogra- raphy-tandem mass spectrometry method for the determination of dye
phy with minimal clean-up. Food Control. 16:293–297. residues in aquaculture products: Development and validation. J. Chro-
Gennaro, M., Gioannini, E., Angelino, S., Aigotti, R. and Giacosa, D. matogr. A 1218:1632–1645.
(1997). Identification and determination of red dyes in confectionery International Agency for Research on Cancer (IARC). (1975). IARC
by ion-interaction high-performance liquid chromatography. J. Chro- monographs on the evaluation of carcinogenic risks to humans. Some
matogr. A 767:87–92. aromatic azo compunds. Vol. 8. Available from http://monographs.
Ghoreishi, S. M., Behpour, M. and Golestaneh, M. (2011). Simultaneous iarc.fr/ENG/Monographs/vol8/volume8.pdf. Accessed June 1, 2009.
voltammetric determination of Brilliant Blue and Tartrazine in real International Agency for Research on Cancer (IARC). (1978). IARC
samples at the surface of a multi-walled carbon nanotube paste elec- monographs on the evaluation of carcinogenic risks to humans. Some
trode. Anal. Method. 3:2842–2847. aromatic amines and related nitro compunds (hair dyes, colouring
Ghoreishi, S. M., Behpour, M. and Golestaneh, M. (2012). Simulta- agents and miscellenous industrial chemcals). Vol. 16. Available
neous determination of Sunset yellow and Tartrazine in soft drinks from http://monographs.iarc.fr/ENG/Monographs/vol16/volume16.
using gold nanoparticles carbon paste electrode. Food Chem. pdf, Accessed June 1, 2009.
132:637–641. Jacobson, M.F. (2012). Carcinogenicity and regulation of caramel color-
Gianotti, V., Angioi, S., Gosetti, F., Marengo, E. and Gennaro, M. C. ings. Int. J. Occup. Environ. Health. 18:254–259.
Downloaded by [Universidad Nacional Colombia] at 16:11 05 September 2017

(2005). Chemometrically assisted development of IP-RP-HPLC and Jager, A. V., Tonin, F. G. and Tavares, M. F. M. (2005). Optimizing the sepa-
spectrophotometric methods for the identification and determination ration of food dyes by capillary electrophoresis. J. Sep. Sci. 28:957–965.
of synthetic dyes in commercial soft drinks. J. Liq. Chromatogr. Related Japan External Trade Organization (JETO). (2006). Food sanitation law
Technol. 28:923–937. in Japan. Available from http://www.foodluh.org/en/pdf/Food%20
Giorgi, L. and Lindner, L. F. (2009). The contemporary governance of food Sanitation%20Law%20in%20Japan.pdf. Accessed May 1, 2013.
safety: Taking stock and looking ahead. Qual. Assur. Saf. Crops. Foods. Joint FAO/WHO Expert Committee on Food Additives (JECFA). (2009).
1:36–49. Environmental Health Criteria 240. Principles and methods for the risk
Golka, K., Kopps, S. and Myslak, Z. W. (2004). Carcinogenicity of azo colo- asessment of chemicals in food. Annex 1. Glossary of terms. Available
rants: Influence of solubility and bioavailability. Toxicol. Lett. 151:203– from http://whqlibdoc.who.int/ehc/WHO_EHC_240_13_eng_Annex1.
210. pdf. Accessed August 1, 2010.
Gonzalez, M., Gallego, M. and Valcarcel, M. (2003a). Determination of Ju, C., Tang, Y., Fan, H. and Chen, J. (2008). Enzyme-linked immunosor-
natural and synthetic colorants in prescreened dairy samples using liq- bent assay (ELISA) using a specific monoclonal antibody as a new tool
uid chromatography-diode array detection. Anal. Chem. 75:685–693. to detect sudan dyes and para red. Anal. Chim. Acta 621:200–206.
Gonzalez, M., Gallego, M. and Valcarcel, M. (2003b). Liquid chro- Khanavi, M., Hajimahmoodi, M., Ranjbar, A. M., Oveisi, M. R., Ardekani,
matographic determination of natural and synthetic colorants in lyoph- M. R. S. and Mogaddam, G. (2012). Development of a green chro-
ilized foods using an automatic solid-phase extraction system. J. Agric. matographic method for simultaneous determination of food colorants.
Food Chem. 51:2121–2129. Food Anal. Method. 5:408–415.
Gui, W., Xu, Y., Shou, L., Zhu, G. and Ren, Y. (2010). Liquid chromatogra- Kirschbaum, J., Krause, C. and Bruckner, H. (2006). Liquid chro-
phy–tandem mass spectrometry for the determination of chrysoidine matographic quantification of synthetic colorants in fish roe and caviar.
in yellow-fin tuna. Food Chem. 122:1230–1234. Eur. Food Res. Technol. 222:572–579.
Hajee, C. A. and Haagsma, N. (1995). Simultaneous determination of Kirschbaum, J., Krause, C., Pfalzgraf, S. and Bruckner, H. (2003). Develop-
malachite green and its metabolite leucomalachite green in eel plasma ment and evaluation of an HPLC-DAD method for determination of
using post-column oxidation. J. Chromatogr. B 669:219–227. synthetic food colorants. Chromatographia. 57:115–119.
Hajimahmoodi, M., Afsharimanesh, M., Moghaddam, G., Sadeghi, N., Kleter, G. A., Prandini, A., Filippi, L. and Marvin, H. J. (2009). Identifica-
Oveisi, M. R., Jannat, B., Pirhadi, E, Zamani Mazdeh, F. and Kanan, H. tion of potentially emerging food safety issues by analysis of reports
(2013). Determination of eight synthetic dyes in foodstuffs by green liq- published by the European Community’s Rapid Alert System for Food
uid chromatography. Food Addit. Contam. Pt A 30:780–785. and Feed (RASFF) during a four-year period. Food Chem. Toxicol.
Halme, K., Lindfors, E. and Peltonen, K. (2007). A confirmatory analysis of 47:932–950.
malachite green residues in rainbow trout with liquid chromatography- Kucharska, M. and Grabka, J. (2010). A review of chromatographic meth-
electrospray tandem mass spectrometry. J. Chromatogr. B 845:74–79. ods for determination of synthetic food dyes. Talanta. 80:1045–1051.
Han, D., Yu, M., Knopp, D., Niessner, R., Wu, M. and Deng, A. (2007). Kuo, K., Huang, H. and Hsieh, Y. (1998). High-performance capillary elec-
Development of a highly sensitive and specific enzyme-linked immu- trophoretic analysis of synthetic food colorants. Chromatographia.
nosorbent assay for detection of sudan I in food samples. J. Agric. Food 47:249–256.
Chem. 55:6424–6430. Lau, K., McLean, W. G., Williams, D. P., Howard, V. (2006). Synergistic
Harp, B. P., Miranda-Bermudez, E. and Barrows, J. N. (2013). Determina- interactions between commonly used food additives in a developmental
tion of seven certified color additives in food products using liquid neurotoxicity test. Toxicol. Sci. 90:178–187.
chromatography. J. Agric. Food Chem. 61:3726–3736. Lee, K.-S., Shiddiky, M. J. A., Park, S.-H., Park, D.-S. and Shim, Y.-B.
Hashimoto, J. C., Paschoal, J. A. R., Queiroz, S. C. N., Ferracini, V. L., Assa- (2008). Electrophoretic analysis of food dyes using a miniaturized
lin, M. R. and Reyes, F. G. R. (2012). A simple method for the determina- microfluidic system. Electrophoresis. 29:1910–1917.
tion of malachite green and leucomalachite green residues in fish by a Lee, K., Wu, J. and Cai, Z. (2006). Determination of malachite green
modified quechers extraction and LC/MS/MS. J. AOAC Int. 95:913–922. and leucomalachite green in edible goldfish muscle by liquid chro-
He, L., Su, Y., Fang, B., Shen, X., Zeng, Z. and Liu, Y. (2007). Determina- matography-ion trap mass spectrometry. J. Chromatogr. B 843:
tion of sudan dye residues in eggs by liquid chromatography and gas 247–251.
chromatography-mass spectrometry. Anal. Chim. Acta 594:139–146. Lei, H., Liu, J., Song, L., Shen, Y., Haughey, S. A., Guo, H., Yang, J., Xu, Z.,
Huang, H., Chiu, C., Sue, S. and Cheng, C. (2003). Analysis of food colo- Jiang, Y. and Sun, Y. (2011). Development of a highly sensitive and spe-
rants by capillary electrophoresis with large-volume sample stacking. J. cific immunoassay for determining chrysoidine, a banned dye, in soy-
Chromatogr. A 995:29–36. bean milk film. Molecules. 50:7043–7057.
Huang, H., Chuang, C., Chiu, C. and Chung, M. (2005). Determination of Lei, Y., Zhang, S., Fang, L., Hamid Akash, M. S., Shi, W., Sun, K., Xu, Y. and
food colorants by microemulsion electrokinetic chromatography. Elec- Chen, S. (2013). A sensitive and specific enzyme immunoassay for
trophoresis 26:867–877. detecting tartrazine in human urinary samples. Anal. Method. 5:925–930.
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 545

Li, Y., Wang, Y., Yang, H., Gao, Y., Zhao, H. and Deng, A. (2010). Estab- in the community: A randomised, double-blinded, placebo-controlled
lishment of an immunoaffinity chromatography for simultaneously trial. The Lancet. 370:1560–1567.
selective extraction of Sudan I, II, III and IV from food samples. J. Medeiros, R. a, Lourencao, B. C., Rocha-Filho, R. C. and Fatibello-Filho, O.
Chromatogr. A 1217:7840–7847. (2012a). Simultaneous voltammetric determination of synthetic colo-
Lin, H., Li, G. and Wu, K. (2008). Electrochemical determination of sudan rants in food using a cathodically pretreated boron-doped diamond
I using montmorillonite calcium modified carbon paste electrode. Food electrode. Talanta. 97:291–297.
Chem. 107:531–536. Medeiros, R. a, Lourencao, B. C., Rocha-Filho, R. C. and Fatibello-Filho, O.
Lineback, D. R., Pirlet, A., Van Der Kamp, J. and Wood, R. (2009). Global- (2012b). Flow injection simultaneous determination of synthetic colo-
ization, food safety issues & role of international standards. Qual. rants in food using multiple pulse amperometric detection with a
Assur. Saf. Crops Foods 1:23–27. boron-doped diamond electrode. Talanta. 99:883–889.
Littlefield, N. A., Blackwell, B.-N., Hewitt, C. C. and Gaylor, D. W. (1985). Mejia, E., Ding, Y. S., Mora, M. F. and Garcia, C. D. (2007). Determination
Chronic toxicity and carcinogenicity studies of gentian violet in mice. of banned sudan dyes in chili powder by capillary electrophoresis. Food
Fundam. Appl. Toxicol. 5:902–912. Chem. 102:1027–1033.
Liu, J., Zhang, H., Zhang, D., Gao, F. and Wang, J. (2012). Production of Minioti, K. S., Sakellariou, C. F. and Thomaidis, N. S. (2007). Determina-
the monoclonal antibody against Sudan 2 for immunoassay of Sudan tion of 13 synthetic food colorants in water-soluble foods by reversed-
dyes in egg. Anal. Biochem. 423:246–252. phase high-performance liquid chromatography coupled with diode-
Liu, R., Hei, W., He, P. and Li, Z. (2011). Simultaneous determination of array detector. Anal. Chim. Acta 583:103–110.
fifteen illegal dyes in animal feeds and poultry products by ultra-high Ministry of Health, Labour and Welfare, Japan. (2011). Inspection Results
performance liquid chromatography tandem mass spectrometry. J. of Imported Foods Monitoring and Guidance Plan for FY 2011. Avail-
Downloaded by [Universidad Nacional Colombia] at 16:11 05 September 2017

Chromatogr. B 879:2416–2422. able from http://www.mhlw.go.jp/english/topics/importedfoods/11/11-


Liu, S., Zhang, X., Lin, X., Wu, X., Fu, F. and Xie, Z. (2007b). Development 06.html. Accessed September 9, 2013.
of a new method for analysis of Sudan dyes by pressurized CEC with Ministry of Health People’s Republic of China. (2011). National Food
amperometric detection. Electrophoresis 28:1696–1703. Safety Standard, Standard for Uses of Food Additives GB2760-2011.
Liu, W., Zhao, W., Chen, J. and Yang, M. (2007a). A cloud point extraction English translation available from http://www.fas.usda.gov. Accessed
approach using Triton X-100 for the separation and preconcentration September 9, 2013.
of sudan dyes in chilli powder. Anal. Chim. Acta 605:41–45. Mishra, K. K., Dixit, S., Purshottam, S. K., Pandey, R. C., Das, M. and
Liu, Y., Song, Z., Dong, F. and Zhang, L. (2007c). Flow injection chemilu- Khanna, S. K. (2007). Exposure assessment to Sudan dyes through con-
minescence determination of sudan I in hot chilli sauce. J. Agric. Food sumption of artificially coloured chilli powders in India. Int. J. Food
Chem. 55:614–617. Sci. Technol. 42:1363–1366.
Lizaso, M. T., Moneo, I., Garcıa, B. E., Acero, S., Quirce, S. and Tabar, A. I. Mitrowska, K. and Posyniak, A. (2004). Determination of malachite green
(2000). Identification of allergens involved in occupational asthma due and its metabolite, leucomalachite green in fish muscle by liquid chro-
to carmine dye. Ann. Allergy, Asthma Immunol. 84:549–552. matography. J. AOAC Int. 7:173–176.
Llamas, N. E., Garrido, M., Di Nezio, M. S. and Fernandez Band, B. S. Mitrowska, K., Posyniak, A. and Zmudzki, J. (2008). Determination of
(2009). Second order advantage in the determination of amaranth, sun- malachite green and leucomalachite green residues in water using liq-
set yellow FCF and tartrazine by UV-vis and multivariate curve resolu- uid chromatography with visible and fluorescence detection and confir-
tion-alternating least squares. Anal. Chim. Acta 655:38–42. mation by tandem mass spectrometry. J. Chromatogr. A 1207:94–100.
Long, C., Mai, Z., Yang, Y., Zhu, B., Xu, X., Lu, L. and Zou, X. (2009). Mo, Z., Zhang, Y., Zhao, F., Xiao, F., Guo, G. and Zeng, B. (2010). Sensitive
Determination of multi-residue for malachite green, gentian violet and voltammetric determination of Sudan I in food samples by using gem-
their metabolites in aquatic products by high-performance liquid chro- ini surfactant–ionic liquid–multiwalled carbon nanotube composite
matography coupled with molecularly imprinted solid-phase extrac- film modified glassy carbon electrodes. Food Chem. 121:233–237.
tion. J. Chromatogr. A 1216:2275–2281. Murty, M. R. V. S., Chary, N. S., Prabhakar, S., Raju, N. P. and Vairamani,
Lu, F., Sun, M., Fan, L., Qiu, H., Li, X. and Luo, C. (2012). Flow injection M. (2009). Simultaneous quantitative determination of Sudan dyes
chemiluminescence sensor based on core–shell magnetic molecularly using liquid chromatography – atmospheric pressure photoionization
imprinted nanoparticles for determination of chrysoidine in food sam- – tandem mass spectrometry. Food Chem. 115:1556–1562.
ples. Sensors Actuators B-Chem. 173:591–598. National Toxicology Program (NTP). (1982). Study data for sudan I.
Lucova, M., Hojerova, J., Pazourekov, A. S. and Klimova, Z. (2013). Available from <http://ntp-apps.niehs.nih.gov/ntp_tox/index.cfm?
Absorption of triphenylmethane dyes brilliant blue and patent blue searchtermD842-07-9&fuseactionDntpsearch.searchresults>. Accessed
through intact skin, shaven skin and lingual mucosa from daily life February 1, 2010.
products. Food Chem. Toxicol. 52:19–27. Nebot, C., Iglesias, A., Barreiro, R., Miranda, J. M., Vazquez, B., Franco, C.
Ma, M., Luo, X., Chen, B., Su, S. and Yao, S. (2006). Simultaneous determi- M. and Cepeda, A. (2013). A simple and rapid method for the identifi-
nation of water-soluble and fat-soluble synthetic colorants in foodstuff cation and quantification of malachite green and its metabolite in hake
by high-performance liquid chromatography–diode array detection– by HPLC-MS/MS. Food Control. 31:102–107.
electrospray mass spectrometry. J. Chromatogr. A 1103:170–176. Nevado, J. J., Cabanillas, C. G. and Salcedo, A. M. (1995). Simultaneous
Martınez Bueno, M. J., Herrera, S., Ucles, A., Ag€uera, A., Hernando, M. D., spectrophotometric determination of three food dyes by using the first
Shimelis, O., Rudolfsson, M. and Fernandez-Alba, A. R. (2010). Deter- derivative of ratio spectra. Talanta. 42:2043–2051.
mination of malachite green residues in fish using molecularly Nevado, J. J. B., Flores, J. R. and Llerena, M. J. V. (1997). Square wave
imprinted solid-phase extraction followed by liquid chromatography- adsorptive voltammetric determination of sunset yellow. Talanta.
linear ion trap mass spectrometry. Anal. Chim. Acta 665:47–54. 44:467–474.
Mazzetti, M., Fascioli, R., Mazzoncini, I., Spinelli, G., Morelli, I. and Bertoli, Ni, Y. and Bai, J. (1997). Simultaneous determination of amaranth and
A. (2004). Determination of 1-phenylazo-2-naphthol (sudan I) in chilli sunset yellow by ratio derivative voltammetry. Talanta. 44:105–109.
powder and in chilli-containing food products by GPC clean-up and Ni, Y., Bai, J. and Jin, L. (1996). Simultaneous adsorptive voltammetric
HPLC with LC/MS confirmation. Food Addit. Contam. 21:935–941. analysis of mixed colorants by multivariate calibration approach. Anal.
Mazzotti, F., Di Donna, L., Maiuolo, L., Napoli, A., Salerno, R., Sajjad, A. Chim. Acta 329:65–72.
and Sindona, G. (2008). Assay of the set of all sudan azodye (I, II, III, Ni, Y., Bai, J. and Jin, L. (1997). Multicomponent chemometric determina-
IV, and para-red) contaminating agents by liquid Chromatogra- tion of colorant mixtures by voltammetry. Anal. Lett. 30:1761–1777.
phy¡Tandem mass spectrometry and isotope dilution methodology. J. Ni, Y. and Gong, X. (1997). Simultaneous spectrophotometric determina-
Agric. Food Chem. 56:63–67. tion of mixtures of food colorants. Anal. Chim. Acta 354:163–171.
McCann, D., Barrett, A., Cooper, A., Crumpler, D., Dalen, L., Grimshaw, Ni, Y., Wang, Y. and Kokot, S. (2009). Simultaneous kinetic spectrophoto-
K., Kitchin, E., Lok, K., Porteous, L. and Prince, E. (2007). Food addi- metric analysis of five synthetic food colorants with the aid of chemo-
tives and hyperactive behaviour in 3-year-old and 8/9-year-old children metrics. Talanta. 78:432–441.
546 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Nigg, J. T., Lewis, K., Edinger, T. and Falk, M. (2012). Meta-analysis of atten- Rapid Alert System For Food and Feed (RASFF). Online database.
tion-deficit/hyperactivity disorder or attention-deficit/hyperactivity disorder Available from <https://webgate.ec.europa.eu/rasff-window/portal/>.
symptoms, restriction diet, and synthetic food color additives. J. Am. Acad. Accessed 1 September 2013.
Child Adolesc. Psychiatry 51:86–97. Rebane, R., Leito, I., Yurchenko, S. and Herodes, K. (2010). A review of
Nordic Council of Ministers. (2002). Food additives in Europe 2000 Status analytical techniques for determination of Sudan I – IV dyes in food
of safety assessments of food additives presently permitted in the EU. matrixes. J. Chromatogr. A 1217:2747–2757.
TermaNord 560. Available from <http://www.norden.org/en/publica Regulation (EC) No 1925/2006 of the European Parliament and of the
tions/publications/2002-560/at_download/publicationfile>. Accessed Council of 20 December 2006 on the addition of vitamins and
June 1, 2010. minerals and of certain other substances to foods. Off. J. Eur.
Oplatowska, M., Connolly, L., Stevenson, P., Stead, S. and Elliott, C. T. Union L 404:26–38.
(2011a). Development and validation of a fast monoclonal based dis- Regulation (EC) No 1333/2008 of the European Parliament and the Coun-
equilibrium enzyme-linked immunosorbent assay for the detection of cil of 16 December 2008 on food additives. Off. J. Eur. Union L 354:16–
triphenylmethane dyes and their metabolites in fish. Anal. Chim. Acta 33.
698:51–60. Reyns, T., Fraselle, S., Laza, D. and Loco, J. V. (2010). Rapid method for the
Oplatowska, M., Donnelly, R. F., Majithiya, R. J., Glenn Kennedy, D. and confi rmatory analysis of chrysoidine in aquaculture products by ultra-
Elliott, C. T. (2011b). The potential for human exposure, direct and performance liquid chromatography – tandem mass spectrometry.
indirect, to the suspected carcinogenic triphenylmethane dye Brilliant Biomed. Chromatogr. 24:982–989.
Green from green paper towels. Food Chem. Toxicol. 49:1870–1876. Roybal, J. E., Allen, P. P., Munns, R. K., Holland, D. C., Hurlbut, J. A. and
Oplatowska, M. and Elliott, C. T. (2011). Development and validation of Long, A. R. (1995). Determination of malachite green and its metabo-
Downloaded by [Universidad Nacional Colombia] at 16:11 05 September 2017

rapid disequilibrium enzyme-linked immunosorbent assays for the lite, leucomalachite green in catfish (Ictalurus punctatus) tissue bu liq-
detection of Methyl Yellow and Rhodamine B dyes in foods. The Ana- uid chromatography with visible detection. Residues Trace Elements
lyst. 136:2403–2410. 78:453–457.
Oplatowska, M., Stevenson, P. J., Schulz, C., Hartig, L. and Elliott, C. T. Ruf, J., Walter, P., Kandler, H. and Kaufmann, A. (2012). Discovery and
(2011c). Development of a simple gel permeation clean-up procedure structural elucidation of the illegal azo dye Basic Red 46 in sumac spice.
coupled to a rapid disequilibrium enzyme-linked immunosorbent assay Food Addit. Contam. Pt A 29:897–890.
(ELISA) for the detection of Sudan I dye in spices and sauces. Anal. Rushing, L. G. and Hansen, E. B. (1997). Confirmation of malachite green,
Bioanal. Chem. 401:1411–1422. gentian violet and their leuco analogs in catfish and trout tissue by
Oreopoulou, V., Psimouli, V., Tsimogiannis, D., Anh, T. K., Tu, N. M., high-performance liquid chromatography utilizing electrochemistry
Uygun, U., Koksel, H., Gokmen, V., Crews, C., Tomoskozi, S., Domo- with ultraviolet-visible diode array detection and fluorescence detec-
tor, L., Balazs, G., Zhang, L., Liu, H., Cui, Y., Liu, B., Wenping, D., tion. J. Chromatogr. B 700:223–231.
Xingguo, W., Weining, H., Ozer, H., Zhongdong, L. and El-Nawawy, Rushing, L. G. and Thompson, H. C. (1997). Simultaneous determination
M. (2009). Assessing food additives: The good, the bad and the ugly. of malachite green, gentian violet and their leuco metabolites in catfish
Qual. Assur. Saf. Crops Foods 1:101–110. or trout tissue by high-performance liquid chromatography with visible
Pardo, O., Yusa, V., Le on, N. and Pastor, A. (2009). Development of a detection. J. Chromatogr. B 688:325–330.
method for the analysis of seven banned azo-dyes in chilli and hot chilli Rushing, L. G., Webb, S. F. and Thompson, H. C. (1995). Determination of
food samples by pressurised liquid extraction and liquid chromatogra- leucogentian violet and gentian violet in catfish tissue by high-perfor-
phy with electrospray ionization-tandem mass spectrometry. Talanta. mance liquid chromatography with visible detection. J. Chromatogr. B
78:178–186. 674:125–131.
Pemberton, R. M., Hart, J. P. and Mottram, T. T. (2001). An electrochemi- Ryvolova, M., Taborsky, P., Vrabel, P., Krasensky, P. and Preisler, J. (2007).
cal immunosensor for milk progesterone using a continuous flow sys- Sensitive determination of erythrosine and other red food colorants
tem. Biosens. Bioelectron. 16:715–723. using capillary electrophoresis with laser-induced fluorescence detec-
Perez-Urquiza, M. and Beltran, J. L. (2000). Determination of dyes in food- tion. J. Appl. Behav. Anal. 1141:206–211.
stuffs by capillary zone electrophoresis. J. Chromatogr. A 898:271–275. Safarık, I. and Safarikova, M. (2002). Detection of low concentrations of
Perva-Uzunalic, A., Skerget, M., Weinreich, B. and Zeljko,  K. (2004). malachite green and crystal violet in water. Water Res. 36:196–200.
Extraction of chilli pepper (var. Byedige) with supercritical CO2: Effect Scherpenisse, P. and Bergwerff, A. (2005). Determination of residues of
of pressure and temperature on capsaicinoid and colour extraction effi- malachite green in finfish by liquid chromatography tandem mass
ciency. Food Chem. 87:51–58. spectrometry. Anal. Chim. Acta 529:173–177.
Pielesz, A., Baranowska, I., Rybak, A. and Wlochowicz, A. (2002). Detec- Schummer, C., Sassel, J., Bonenberger, P. and Moris, G. (2013). Low-Level
tion and determination of aromatic amines as products of reductive Detections of Sudan I, II, III and IV in Spices and Chili-Containing Food-
splitting froms azo dyes. Ecotoxicol. Environ. Saf. 53:42–47. stuffs Using UPLC-ESI-MS/MS. J. Agric. Food Chem. 61:2284–2289.
Pinheiro, H., Touraud, E. and Thomas, O. (2004). Aromatic amines from Scotter, M. J. (2011a). Emerging and persistent issues with artificial food
azo dye reduction: Status review with emphasis on direct UV spectro- colours: Natural colour additives as alternatives to synthetic colours in
photometric detection in textile industry wastewaters. Dyes Pigments food and drink. Qual. Assur. Saf. Crops Foods 3:28–39.
61:121–139. Scotter, M. J. (2011b). Methods for the determination of European Union-
Premier Analytical Services. (2013). Illegal dye testing. Available permitted added natural colours in foods: A review. Food Addit. Con-
from <http://www.rhmtech.co.uk/info-sheets/illegal-dye-testing.html>. tam. Pt. A 28:527–596.
Accessed June 1, 2013. Shan, W. C., Xi, J. Z., Sun, J., Zhang, Y. J. and Wang, J. P. (2012). Produc-
Puoci, F., Garreffa, C., Iemma, F., Muzzalupo, R., Spizzirri, U. G. and Picci, tion of the monoclonal antibody against Sudan 4 for multi-immunoas-
N. (2005). Molecularly imprinted solid phase extraction for detection say of Sudan dyes in egg. Food Control. 27:146–152.
of sudan I in food matrices. Food Chem. 93:349–353. Shen, Y.-D., Deng, X.-F., Xu, Z.-L., Wang, Y., Lei, H.-T., Wang, H., Yang,
Qi, Y. H., Shan, W. C., Liu, Y. Z., Zhang, Y. J. and Wang, J. P. (2012). J.-Y., Xiao, Z.-L. and Sun, Y.-M. (2011). Simultaneous determination of
Production of the polyclonal antibody against sudan 3 and Immu- malachite green, brilliant green and crystal violet in grass carp tissues
noassay of sudan dyes in food samples. J. Agric. Food Chem. by a broad-specificity indirect competitive enzyme-linked immunosor-
60:2116–2122. bent assay. Anal. Chim. Acta. 707:148–154.
QTS Analytical. (2012). Illegal dye testing. Available from <http://www. Silva, M. L., Garcia, M. B., Lima, J. L. and Barrado, E. (2007). Voltam-
qtsanalytical.com/illegal-dye-testing/?utm_sourceDrss&utm_mediumD metric determination of food colorants using a polyallylamine
rss&utm_campaignDillegal-dye-testing>. Accessed June 1, 2013. modified tubular electrode in a multicommutated flow system.
Rao, P. and Sudershan, R. (2008). Risk assessment of synthetic food col- Talanta. 72:282–288.
ours: A case study in Hyderabad, India. Int. J. Food Saf. Nutr. Pub. Singh, G., Koerner, T., Gelinas, J.-M., Abbott, M., Brady, B., Huet, A.-C.,
Health. 1:68–87. Charlier, C., Delahaut, P. and Godefroy, S. B. (2011). Design and
CRITICAL REVIEWS IN FOOD SCIENCE AND NUTRITION 547

characterization of a direct ELISA for the detection and quantification Vidotti, E. C., Cancino, J. C., Oliveira, C. C. and Rollemberg, M. C. E.
of leucomalachite green. Food Addit. Contam. Pt. A 28:731–739. (2005). Simultaneous determination of food dyes by first derivative
Smith, S., Gieseker, C., Reimschuessel, R., Decker, C.-S. and Carson, M. C. spectrophotometry with sorption onto polyurethane foam. Anal. Sci.
(2009). Simultaneous screening and confirmation of multiple classes of 21:149–153.
drug residues in fish by liquid chromatography-ion trap mass spec- Vidotti, E. C., Costa, W. F. and Oliveira, C. (2006). Development of a green
trometry. J. Chromatogr. A 1216:8224–8232. chromatographic method for determination of colorants in food sam-
Song, Y.-Z. (2010). Electrochemical reduction of sunset yellow at a multi- ples. Talanta 68:516–521.
walled carbon nanotube (MWCNT)-modified glassy carbon electrode Wang, J., Wei, K., Li, H., Li, Q. X., Li, J. and Xu, T. (2012). A sensitive and
and its analytical application. Can. J. Chem. 88:676–681. selective enzyme-linked immunosorbent assay for the analysis of para
Song, Y. Z., Xu, J. M., Lv, J. S., Zhong, H., Ye, Y. and Xie, J. M. red in foods. Analyst 137:2136–2142.
(2010). Electrochemical reduction of tartrazine at multi-walled car- Wang, X., Song, G., Wu, W., Zhao, J. and Hu, Y. (2008). Determination of
bon nanotube-modified pyrolytic graphite electrod. Ind. J. Chem. food colorant, chrysoidine, in fish by GC-MS. Chromatographia
49A:1030–1034. 68:659–662.
Stuart, B. (2006). Analysis of illegal dyes in chilli powder by LC-UV. Statu- Wang, Y., Wei, D., Yang, H., Yang, Y., Xing, W., Li, Y. and Deng, A.
tory analysis government chemist programme ad hoc project 1. LGC (2009). Development of a highly sensitive and specific
Limited. Available from <http://www.governmentchemist.org.uk/ monoclonal antibody-based enzyme-linked immunosorbent assay
dm_documents/Aanlysis%20of%20illegal%20dyes%20in%20chilli% (ELISA) for detection of sudan I in food samples. Talanta
20powder%20by%20LC-UV_3nhSP.pdf>. Accessed June 1, 2012. 77:1783–1789.
Suglia, S. F., Solnick, S. and Hemenway, D. (2013). Soft drink consumption Wang, Y., Yang, H. and Deng, A. (2011). A sensitive and selective direct
Downloaded by [Universidad Nacional Colombia] at 16:11 05 September 2017

is associated with behavior problems in 5-yer-olds. J. Pediatr. competitive enzyme-linked immunosorbent assay for fast detection of
163:1323–1328. Sudan I in food samples. J. Sci. Food Agric. 91:1836–1842.
Sun, H., Wang, F. and Ai, L. (2007). Determination of banned 10 azo-dyes Watson, D. H. (2001). Food Chemical Safety, Volume 2: Additives. Wood-
in hot chili products by gel permeation chromatography-liquid chro- head, Cambridge, UK.
matography-electrospray ionization-tandem mass spectrometry. J. Wu, L. P., Li, Y. F., Huang, C. Z. and Zhang, Q. (2006). Visual detection of
Chromatogr. A 1164:120–128. Sudan dyes based on the plasmon resonance light scattering signals of
Tao, Y., Chen, D., Chao, X., Yu, H., Yuanhu, P., Liu, Z., Huang, L., Wang, Y. silver nanoparticles. Anal Chem. 78:5570–5577.
and Yuan, Z. (2011). Simultaneous determination of malachite green, Wu, X., Zhang, G., Wu, Y., Hou, X. and Yuan, Z. (2007). Simulta-
gentian violet and their leuco-metabolites in shrimp and salmon by liq- neous determination of malachite green, gentian violet and their
uid chromatographyetandem mass spectrometry with accelerated solvent leuco-metabolites in aquatic products by high-performance liquid
extraction and auto solid-phase clean-up. Food Control 22:1246–1252. chromatography-linear ion trap mass spectrometry. J. Chromatogr.
Tarbin, J. A., Barnes, K. A., Bygrave, J. and Farrington, W. H. (1998). A 1172:121–126.
Screening and confirmation of triphenylmethane dyes and their leuco Xiao, F., Zhang, N., Gu, H., Qian, M., Bai, J., Zhang, W. and Jin, L.
metabolites in trout muscle using HPLC-vis and ESP-LC-MS. The Ana- (2011). A monoclonal antibody-based immunosensor for detection
lyst 123:2567–2571. of Sudan I using electrochemical impedance spectroscopy. Talanta
Tarbin, J. A., Chan, D., Stubbings, G. and Sharman, M. (2008). Multiresi- 84:204–211.
due determination of triarylmethane and phenothiazine dyes in fish tis- Xing, W., He, L., Yang, H., Sun, C., Li, D., Yang, X., Li, Y. and
sues by LC-MS/MS. Anal. Chim. Acta 625:188–194. Deng, A. (2009). Development of a sensitive and group-specific
Tateo, F. and Bononi, M. (2004). Fast determination of sudan I by HPLC/ polyclonal antibody-based enzyme-linked immunosorbent assay
APCI-MS in hot chilli, spices, and oven-baked foods. J. Agric. Food (ELISA) for detection of malachite green and leucomalachite
Chem. 52:655–658. green in water and fish samples. J. Sci. Food Agric. 89:2165–
The Prevention of Food Adulteration Rules. (1955). Rules 26–28. Available 2173.
from <http://www.gujhealth.gov.in/images/pdf/legis/prevention-of- Xing, Y., Meng, M., Xue, H., Zhang, T., Yin, Y. and Xi, R. (2012). Develop-
food-adulteration-rules-1955.pdf>. Accessed May 1, 2013. ment of a polyclonal antibody-based enzyme-linked immunosorbent
Times of India. (2012). Kitchen tricks to expose food adulteration. Avail- assay (ELISA) for detection of Sunset Yellow FCF in food samples.
able from <http://articles.timesofindia.indiatimes.com/2012-05-30/ Talanta 99:125–131.
diet/30658656_1_food-adulteration-common-adulterants-metanil-yel Xinyi, C., Xiaogang, C., Zweigenbaum, J. A., Yanyan, F., Wei, Y. and Yun,
low>. Accessed September 6, 2013. L. (2009). Discovering sudan IV in Salty Eggs with LC–TOF-MS. Chro-
Tripathi, M., Khanna, S. and Das, M. (2007). Surveillance on use of syn- matographia 71:139–142.
thetic colours in eatables vis a vis Prevention of Food Adulteration Act Xu, H., Heinze, T. M., Chen, S., Cerniglia, C. E. and Chen, H. (2007).
of India. Food Control 18:211–219. Anaerobic metabolism of 1-amino-2-naphthol-based azo dyes (sudan
Turnipseed, S. B., Roybal, J. E., Rupp, H. S., Hurlbut, J. A. and Long, A. R. dyes) by human intestinal microflora. Appl. Environ. Microbiol.
(1995). Particle beam liquid chromatography-mass spectrometry of tri- 73:7759–7762.
phenylmethane dyes: Application to confirmation of malachite green Xu, J., Zhang, Y., Yi, J., Meng, M., Wan, Y., Feng, C., Wang, S., Lu, X. and
in incurred catfish tissue. J. Chromatogr. B 670:55–62. Xi, R. (2010a). Preparation of anti-sudan red monoclonal antibody and
Uematsu, Y., Ogimoto, M., Kabashima, J., Suzuki, K. and Kouichi, I. development of an indirect competitive enzyme-linked immunosorbent
(2007). Fast cleanup method for the analysis of sudan I-IV and para assay for detection of sudan red in chilli jam and chilli oil. The Analyst
red in various foods and paprika color (oleoresin) by high-performance 135:2566–2572.
liquid chromatography/diode array detection: Focus on removal of fat Xu, T., Wei, K. Y., Wang, J., Eremin, S. A., Liu, S. Z., Li, Q. X. and Li, J.
and oil as fatty acid methyl esters prepared by transesterification of (2010b). Development of an enzyme-linked immunosorbent assay spe-
acylglycerols. J. AOAC Int. 90:437–445. cific to sudan red I. Anal. Biochem. 405:41–49.
Valle, L., Diaz, C., Zanocco, A. and Richter, P. (2005). Determination of Xue, H., Xing, Y., Yin, Y., Zhang, T., Zhang, B., Zhang, Y., Song, P.,
the sum of malachite green and leucomalachite green in salmon muscle Tian, X., Xu, Y., Wang, P., Meng, M. and Xi, R. (2012). Applica-
by liquid chromatography–atmospheric pressure chemical ionisation- tion of an enzyme immunoassay for the quantitative determination
mass spectrometry. J. Chromatogr. A 1067:101–105. of azo dye (Orange II) in food products. Food Addit. Contam. Pt.
Varga, E., Glauner, T., Berthiller, F., Krska R., Schuhmacher, R. and A 29:1840–1848.
Sulyok, M. (2013). Development and validation of a (semi-)quantitative Yang, M., Fang, J., Kuo, T., Wang, D., Huang, Y., Liu, L., Chen, P. and
UHPLC-MS/MS method for the determination of 191 mycotoxins and Chang, T. (2007). Production of antibodies for selective detection of
other fungal metabolites in almonds, hazelnuts, peanuts and pistachios. malachite green and the related triphenylmethane dyes in fish and fish-
Anal. Bioanal. Chem. 15:5087–5104. pond water. J. Agric. Food Chem. 55:8851–8856.
548 M. OPLATOWSKA-STACHOWIAK AND C. T. ELLIOTT

Yoshioka, N. and Ichihashi, K. (2008). Determination of 40 synthetic food pepper by high-performance liquid chromatography with on-line elec-
colors in drinks and candies by high-performance liquid chromatogra- trogenerated BrO- -luminol chemiluminescence detection. J. Chroma-
phy using a short column with photodiode array detection. Talanta togr. A 1129:34–40.
74:1408–1413. Zhao, S., Yin, J., Zhang, J., Ding, X., Wu, Y. and Shao, B. (2012). Determi-
Yu, C., Liu, Q., Lan, L. and Hu, B. (2008). Comparison of dual solvent-stir nation of 23 dyes in chili powder and paste by high-performance liquid
bars microextraction and U-shaped hollow fiber–liquid phase microex- chromatography-electrospray ionization tandem mass spectrometry.
traction for the analysis of Sudan dyes in food samples by high-perfor- Food Anal. Method. 5:1018–1026.
mance liquid chromatography–ultraviolet/mass spectrometry. J. Zou, T., He, P., Yasen, A. and Li, Z. (2013). Determination of seven syn-
Chromatogr. A 1188:124–131. thetic dyes in animal feeds and meat by high performance liquid chro-
Zhang, Y., Zhang, Z. and Sun, Y. (2006). Development and optimization of matography with diode array and tandem mass detectors. Food Chem.
an analytical method for the determination of Sudan dyes in hot chilli 138:1742–1748.
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