Nhom 10 Bai Bao So 1
Nhom 10 Bai Bao So 1
Nhom 10 Bai Bao So 1
Measurement: Food
journal homepage: www.elsevier.com/locate/meafoo
A R T I C L E I N F O A B S T R A C T
Keywords: Food packaging technology is changing significantly from its conventional protective role to one that is more
Carotenoids interactive, and communication driven. The goal is to enhance the safety and quality of the food by regular
Colorimetric monitoring during the supply chain. Natural food colorants such as carotenoids are being increasingly explored
pH indicator
for its potential application in the smart packaging films as an alternative to the synthetic dyes. In addition to
Antioxidant
Shelf life
adding color, these carotenoids improve the nutritional content and are known to impart health promoting el-
sensors ements to the food. The fruits and vegetables serve to be a rich source of carotenoids. Incorporated carotenoids
act as sensor or indicator, allowing for the real-time monitoring of food quality parameters such as microbial
growth, physiological changes, freshness, and physicochemical attributes. This property of carotenoids have
drawn the attention of consumers, food industries and scientific community. In addition, carotenoids are known
for its antioxidant, anti-microbial property which are known to benefit food matrix in increasing its shelf life. The
inclusion of carotenoids has been shown to positively influence the mechanical, thermal and barrier properties of
packaging films. Given the significance of aforementioned background, the present review aims to compile the
recent studies and investigations made on the potential use of carotenoids in food packaging as smart indicator.
Further it also captures the sources and extraction methodologies presently available for the enhanced recovery
process. It also provides the future line of work for the commercial realization of carotenoids based smart
packaging. This review article is aimed at summarizing the existing current state of knowledge on the carot-
enoids application in smart packaging systems and does not claim to be systematic or complete.
* Corresponding author at: Department of Food Technology, Islamic University of Science and Technology, Kashmir, India.
E-mail address: [email protected] (A.H. Dar).
https://doi.org/10.1016/j.meafoo.2024.100190
Received 19 January 2024; Received in revised form 13 June 2024; Accepted 2 August 2024
Available online 6 August 2024
2772-2759/© 2024 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
S.K. N et al. Measurement: Food 15 (2024) 100190
pH detection change in the foods via colorimetric, chemical, or electrical have been done is establishing the feasibility in incorporating natural
signals have made a significant contribution in increasing the quality, colorant compounds like carotenoids [8–11], anthocyanin [12–16],
safety and traceability of the food. The pH detection by colorant based curcumin [17–21], chlorophyll [22,23], betalains [24–27] in the food
method is the simplest yet accurate technology with the advantage of matrix. Carotenoids are tetraterpene fat soluble pigment with attractive
being economical, easy to use, and a proven non-destructive intelligent yellow, orange, red and purple colors contributed by compounds like
packaging [4,5]. Synthetic dyes and colorants such as methyl red, β-carotene, bixin, norbixin, lutein, cryptoxanthin, zeaxanthin, lycopene
xylenol, bromothymol blue, cresol red, chlorophenol, brilliant blue, and its derivatives. They are abundantly available in photosynthetic
patent blue, quinolone yellow, allura red are commonly used for these bacteria, species of archaea, fungi, algae, fruits, vegetables and animals
applications owing to its cost effectiveness, intensity, stability and ease The structure-function relationship of carotenoids in color exhibiting
of availability. But the use of synthetic dyes in packaging system is being property is attributed to its polyene chain with the property of conju-
perceived as potential negative attribute by the consumer on account of gation. They can be viewed as potential candidate for smart packaging
its toxic and carcinogenic effects. It is crucial to pay attention to the pH responsive colorant molecule. As far as we are aware, very few
migratory effects of synthetic colors on the food matrix and the residues studies have provided a thorough summary of the potential
they leave behind. However, by figuring out and setting the acceptable carotenoids-based pigments for the production of active and intelligent
daily intake (ADI) amounts, the Food and Drug Administration (FDA) food packaging materials, despite the fact that numerous papers on
and the European Food Safety Authority (EFSA) approved the use of carotenoid-based active and intelligent packaging have been published
synthetic dyes in a number of food products [6,7]. On the other end [28–31]. The present review aims at comprehensive understanding of
fruits, vegetables, marine species, microorganisms, algae are bestowed the source, biosynthesis and extraction of carotenoids followed by
with abundant bioactive compounds which can act as a source of natural various techniques currently used for fabricating food packaging poly-
colorant in the food packaging. In addition to its color inducing property mer. The molecular basis of understanding on the modifications in
these bioactive molecules by virtue of its chemical structure possess physicochemical, functional, and mechanical qualities of the carotenoid
antimicrobial, antioxidant properties which are of potential significance incorporated films is being discussed, and the future line of study for its
in strengthening the shelf life of food. Many scientific investigations expansion and commercial acceptance is being provided. The review
2
Table 1
Chemical structure of carotenoids and its sources.
Carotenoids Structure Sources
S.K. N et al.
α carotene Apricot, cantaloup, sweet potato, pumpkin, carrots, Spinach etc
β Carotene Carrot, sweet potato, acerola, mango, pumpkin rosehip fruits, palm, Dunaliella salina Sporidiobolus salmonicolor
Lycopene Gac fruit arils, tomato and tomato products, bitter melon seed arils, watermelon, papaya, guava
Fucoxanthin Seaweeds
S.K. N et al. Measurement: Food 15 (2024) 100190
does not claim to be exhaustive rather it aims at highlighting the key deterioration, thus generating a colorimetric change due to the acid -
findings and summarizing the knowledge on the carotenoids usage in base variations in the vicinity of the food environment. They are the
smart packaging applications. commonly used parameter in evaluating freshness of foods. A qualitative
or quantitative change in the vicinity of food is converted to a signal
2. Smart packaging which can be detected by the consumer [37]. Moreover, the use of pH
responsive indicators can be seen as non-destructive method of food
The concept of smart packaging is predicated on the application of quality analysis. Basically 3 methods can be employed for the pH
proactive and perceptive technologies that monitor and document responsive pigments preparation [38]. a) physical adsorption methods-
observable alterations in the product and surroundings. By the use of Immobilization by ion exchange, b) Covalent binding methods c)
indicators, the state of the product is tracked, traced, and made known to Entrapment based method. Sensitivity, reversibility, stability of the
stakeholders. It also gives the manufacturer, retailer, or consumer the pigment depends on the type of pigment, polymer support and the
chance to monitor and manage the environment both inside and outside method of preparation.
the package at any given time with regard to the productʼs status. Asia
Pacific is anticipated to grow at the faster rate for the forecast period of 3. Natural colorants
2025, with the highest compound annual growth rate (CAGR) for the
design, development and application of smart packaging. Smart pack- Color is one of the important visual attributes of the food playing an
aging can be grouped into active and intelligent packaging systems important role in the acceptance or rejection of food by the consumers.
Fig. (1). Active packaging refers to the incorporation of active compo- Colors are often added to the foods and beverages to enhance the
nents or ingredients in the packaging material which serves to enhance aesthetic quality. It has a direct influence on the appearance and
the shelf life of food by the use of emitters, absorbers, regulators etc. perception of the food quality [39]. Colorants can come in the form of
while the Intelligent packaging has more to do with regular monitoring pigments and dyes based on the solubility. Dyes are completely soluble
of food and provide real time information on the quality and safety while pigments are only dispersible and not completely soluble. Both are
aspect of the food. Food is a natural chemical which keeps on generating known to selectively absorb certain wavelength of light through the
varied biochemical metabolites right from its harvest, processing and chromophore molecule. The emitted color is dependent on the structure
continues to the end of supply chain. There is a need to monitor these of the molecule and its conjugation (organic pigments) and electron
changes which can be converted to a form that can be sensed by the transfer (inorganic pigments) mechanisms. Pigments can be divided on
instrument or sensor or visually detected by the consumers. The various the basis of a) chemical structure of molecule b) origin, and c) method of
metabolites generated in the immediate vicinity of the food product can application [40]. On the basis of chromophore structure, natural col-
be seen as an opportunity for the early detection of food spoilage that orants can be divided as a) chromophore with conjugated system - ca-
can prevent the food contamination related illness and its possible rotenoids, anthocyanins and betalains, b) chromophore with metal
outbreaks [32]. Various responses from the food and its surrounding coordinated porphyrins - chlorophyll, myoglobins etc. [41]. Depending
microenvironment can be harnessed in the form of signals and response. on the end product use and the techno-functional quality of the colorant
Gas concentrations (O2 and CO2), temperature, pH changes, metabolic molecule, different colorants are employed in food applications.
responses from the foods are some of the major biochemical process
which has received attention by the researchers for the deployment of 4. Carotenoids
smart indicators and sensors [33].
Carotenoids known for the attractive and diverse colors of red, yel-
2.1. Sensors and indicators low, orange, purple are seen to be widely distributed in nature. They are
the class of colorants widely being used in the food, pharma and
The sensing materials basically differs with the method of collecting cosmetic sectors. The derivatives of carotenoids like β carotene is viewed
the response from food matrix, transformation of collected response and as precursor to vitamin A. The carotenoids are well recognized for its
visualization/detection techniques. Detecting reactions in the food antioxidant property which can scavenge and neutralize the singlet
matrix and transforming them into a format that can be electronically radicals and peroxyl radicals [42,43]. Close to around 600 carotenoids
processed and present in the form of signal is the primary function of has been identified to occur naturally of which 50 are found to be
sensors. The sensor complex essentially consists of receiver (which is the included in the human diet by consumption of fruits and vegetables
sampling area for the metabolite of interest), transducer (converts the [44]. The various sources of carotenoids are listed in Table 1. Caroten-
signal change to output), processing (which converts the signal into an oids can be defined with hydrocarbons containing 40 carbon atoms and
electric readable format) and display unit [34]. The output received is two terminal rings [45]. They are commonly referred as tetraterpenoids
mainly quantitative in nature enabling the consumers for decision containing isoprenoids of 8 units each. They are hydrophobic com-
making regarding the quality. Barcodes and RFID (radio frequency pounds which are insoluble in water and are soluble in solvents like
identification tags) are the commonly available data carriers for the food acetone, alcohol, chloroform and are sensitive to heat, light and oxygen
packaging mainly providing insights towards the product traceability, [46]. They are generally seen to be esterified with fatty acids or com-
theft prevention and counterfeiting problems [35]. Mostly these data plexed with sugars and proteins [47]. The chemical structure, stericity of
carriers are placed on the tertiary component of packaging (such as the linear chain, unsaturation property plays a significant role in the
pallets, containers) as compared to former two which gets associated bioavailability and stability during the processing. They can be classified
with the primary or secondary packaging. The primary function of in- as - a) Carotenes with linear chain of hydrocarbons which are non-polar
dicator is to provide qualitative and semi-quantitative information and can be cyclized at one or both the ends such as a α carotene, β
about the food to the consumers that can occur merely by reaction with carotene, γ carotene, lycopene, phytoene and phytofluene; b) Carotenes
the substrate or presence/absence of the substrate or by measuring the containing polar oxygen molecule in the form of hydroxy, carbonyl,
concentration of the substrate etc. [36]. Time-Temperature indicators, aldehyde, carboxylic, epoxide, and furanoxide groups leading to xan-
Freshness indicators and Gas indicators are the categories under the thophylls lutein, zeaxanthin, violoxanthin, canthaxanthin, astaxanthin
Indicators. Of particular importance is the pH sensitive based dye in- etc. The carotenoids differ with respect to occurrence and the physical
dicators that are cost effective and does not require any sophisticated form in which they occur in the food matrices like reticulotubular,
analysis or instrumentation to decode. They rely on the interaction of crystalloid, membrane shrouded and globules with fibrillar extension
pigments embedded in the packaging matrix with the metabolites thus giving additional stability to the molecule.
emanating from the food on account of microbial and enzymatic
4
S.K. N et al. Measurement: Food 15 (2024) 100190
4.1. Chemical structure by successive transfer of isopentyl residues) by dimethyl allyl dis-
phosphate isomerase [49,50]. The formation of dimethylallyl pyro-
Carotenoids are isoprene containing tetraterpenoids with the prop- phosphate is the major step for the further carotenoid biosynthesis
erty of conjugation. Most carotenoids contain eight isoprene units of 40 which can get formed from mevalonate pathway or non-mevanolate
carbon chain. Higher group of carotenoids are known to occur in nature pathway. Phytoene which is a colorless, C40 carbon skeleton carot-
with 45–50 carbon chains. The main structure includes polyene chain enoid gets formed from dimethylallyl pyrophosphate through head to
with nine conjugated double bonds and the end group is seen at both the head condensation of two molecules of geranylgeranyl diphosphate.
ends of polyene chain [48]. Intensity of the colors from the carotenoid Phytoene gets progressively desaturated to form lycopene via phyto-
molecule corresponds to the absorption spectra in the range of 400–500 fluene, ζ-carotene, and neurosporene by phytoene desaturase. The
nm mainly attributed to the higher energy of the electronic transition occurrence of lycopene cyclases leads to the production of hydrocarbon
from ground state to S2 state. Termination by the hydrocarbon ring is derivatives of carotenoids with cyclic terminal end groups such as
seen in one or both the ends of the chain. The succession of carotene to α-carotene and β-carotene. Several enzymes carotene hydroxylases,
different forms and molecules can occur in any of the 3 ways a) by ketolases, and epoxidase leads to the production of xanthophyll. The
change in the hydrogenation level, b) by addition of oxygen to derive the xanthophyll contain oxygen functional group which can be in the form
xanthophyll molecules c) cyclisation at one or both the ends of the chain of alcohol (-OH) (lutein), ketone (=O) (canthaxanthin), alcohol and
to produce the different end groups. Carotenoids often exists as cis and ketone (astaxanthin) or as esters of alcohol (fucoxanthin). The biosyn-
trans isomers with significant difference in the solubility and absorb- thesis also leads to the apocarotenoids which gets oxidatively cleavage
ability. While the former isomer is relatively unstable with the loss in by carotenoid cleavage dioxygenases (CCD). The major apocarotenoids
color and pro-vitamin activity the latter is relatively stable. include bixin isolated from annatto seeds.
The biosynthesis of carotenoids is a complex yet highly regulated Fruits and natural commodities which are rich source of carotenoids
process catalyzed by stereo-specific enzymes and are known to follow are in general with a high moisture and water activity contents, there-
specific pathway. The biosynthesis of carotenoids starts from the gen- fore to extract the carotenoids from hydrophilic rich substrate several
eration of precursor acetyl CoA [49]. Two molecules of acetyl CoA reacts methods of cell destruction methods are used mostly in the lines of
to give acetoacetyl CoA and β‑hydroxy β-methyl glutaryl CoA (HMG dehydration. The extraction of carotenoids possess challenge owing to
CoA) gets formed by the action of HMG CoA synthase. Mevalonic acid is its solubility and sensitivity towards the external conditions and the
formed by the reduction reaction of ester group in HMG CoA by HMG process involved therefore the following points to `be considered for the
CoA reductase (which is a rate limiting enzyme) and NADPH. It gets extraction procedure [51]. The carotenoids prior to extraction needs
converted into mevanolate 5-phosphate with the addition of 2 molecules certain pre-treatment to enhance the extraction efficiency such as
of ATP by mevanolate kinase and latter to mevanolate 5-diphosphate by physical (cooking, drying, osmotic shock, freeze–thaw, cryogenic
phosphomevanolate kinase. Decarboxylation of mevanolate diphos- grinding), chemical usage (acid, base, surfactants) and biological (by
phate leads to isopentyl diphosphate (IPP) (which produces isoprene means of germination). Carotenoids by virtue of its sensitivity towards
chains) by mevanolate diphosphate decarboxylase and latter gets iso- light and heat leading to instability to the active compound, careful
merized into dimethylallyl diphosphate (DMAPP) (which is an acceptor consideration need to be taken to prevent exposure from external
5
S.K. N et al. Measurement: Food 15 (2024) 100190
surrounding. Carotenoids are chromatic compounds present in plants, like ethanol, acetone, methanol, propane, methylene chloride or ethyl
algae, and certain microbes. The extraction of carotenoids can be acetate leads to higher recovery rate of polar carotenoids by increasing
accomplished using diverse techniques, which are contingent upon the the solubility.
nature of the source material and the desired level of purity for the
recovered compounds. The various methods of extraction of carotenoid 4.3.3. Ultrasound-assisted extraction (UAE)
is shown in Fig. (2). Each method employed for extraction comes with The method utilizes the acoustic cavitation principle to rupture plant
associated advantage and disadvantage. The novel green extraction cells, facilitating the liberation of carotenoids. This technique improves
technologies are increasingly used in present scenario for enhancing the the extraction process by augmenting mass transfer, decreasing extrac-
recovery rate of carotenoids and reduced use of solvents and chemical tion time, and necessitating lower temperatures. The exposure of plant
residues. matrix to high intensity ultrasound leads to generation of free radicals
thus leading to degradation of carotenoids and reduction in antioxidant
4.3.1. Solvent extraction property. Tsiaka et al. [53] optimized the factors for higher extraction
Solvent extraction is the traditional and most widely used technique rate of xanthophyll (23.4 mg carotenoid/100 g dry sample) from
for the extraction of bioactive compounds. The process entails utilizing lyophilized Aristeus antennatus shrimp powder using acetone as solvent
non polar solvents such as hexane, petroleum ether, tetrahydrofuran for medium (10 ml/g) for 5 min at 600 W and 10:1 mL g− 1 (sample: solvent
extracting lipophilic carotenoids while polar solvents like acetone, ratio). While in the studies of Singh et al. (2015) found the power of
ethanol, and ethyl acetate are used for hydrophilic carotenoids. Some 27.82 % (from total power 500 W), solvent: sample ratio of 67.38
reports also suggested the combination of solvents for better extraction ml/mg, with a pulse length of 19.7 s for 13.48 min gave a higher yield of
of carotenoids from the plant matrix. The solvent solubilizes the carot- zeaxanthin and β-carotene from Chlorella saccharophila.
enoids, which are subsequently isolated from the solid residue using
filtration or centrifugation. But the process requires more time thus the 4.3.4. Microwave-assisted extraction (MAE)
plant matrix is exposed more to a high boiling solvents leading to The use of microwave radiation to facilitate the extraction process by
thermal degradation and possible chance of cis-trans isomerization heating both the solvent and the plant material. Utilizing this technique
reactions. can expedite the extraction procedure and enhance the carotenoid
output. But the microwave energy is known to induce thermal degra-
4.3.2. Supercritical fluid extraction (SFE) dation of sensitive carotenoid. Hence in the studies of Hiranvarachat &
The technique involves the use of supercritical fluids, such as carbon Devahastin [54] followed intermittent exposure of carrot waste to mi-
dioxide, as solvents under carefully controlled temperature and pressure crowave radiation to enhance the yield of β-carotene and carotenoids.
conditions. Supercritical fluids have characteristics that resemble both The split off was designated as intermittency ratio (α). Lower microwave
gases and liquids, rendering them highly effective for extracting carot- power of 180 W with solvent volume of 75 ml or higher microwave
enoids without any residual solvents. The higher rates of diffusion co- power of 300 W with solvent volume of 150 ml including the exposure to
efficient coupled with lower viscosity of SC–CO2 liquid enhances the microwave at a lower intermittency ratio (α = 1/4) lead to higher
rate of penetration into the pores of complex matrices, thus increasing extraction rate of β-carotene and total carotenoids respectively. Further
extraction efficiencies. The spent CO2 can be recycled thus proposing to enhance the recovery yield certain pretreatments to reduce the barrier
the concept of circularity. The highest extraction yield of total carot- effect of external cell matrix is being done. It includes subjecting to
enoids from microalgae Dunaliella salina was obtained at the operating blanching, pretreatment with acids leading to solubilization of pectin
temperature of 60 ◦ C and 400 bar pressure [52]. The use of co-solvents layer and assist in easy penetration of microwave energy.
6
S.K. N et al. Measurement: Food 15 (2024) 100190
7
S.K. N et al. Measurement: Food 15 (2024) 100190
effects against gram positive and gram negative bacteria. Analysis of zone, where air is removed from the mixture under high temperature
antibacterial activity by zone of inhibition showed that fucoxanthin and screw action; and finally the equalization zone, where the mixture of
extract had a negative impact on Streptococcus agalactiae, Staphylococcus molten viscous fluid is extruded from the machine head.
epidermidis, and Staphylococcus aureus [69]. β carotene exert a pro-
nounced antibacterial effect towards gram positive bacteria [70]. 6.3. Electrospinning
Various studies reported the antimicrobial effect occurring due to the
accumulation of toxic compounds that has a negative impact on ATP The electrospinning technique is recognized for production of poly-
hydrolysis and phosphorylation process ultimately leading to death of mers with diameters ranging from nanometers to micrometers. Here the
microbe. molten state of polymer film acts as electrode and as soon as it gets in
contact with high energy electric field, it further extends to the ground
5.3. Photoprotective property electrode forming fiber [72]. The stretching and whipping motion
created by the electric field leads to the deposition of ultrafine fibers. It is
Carotenoids due to its chemical structure and location tends to derive possible to tailor the characteristics of the electrospun fibers by adjust-
the property of photo protection against increased light and photo- ing processing parameters such as polymer concentration, solution vis-
oxidative damage. It can effectively reduce and quench the singlet cosity, applied voltage, and collector geometry. Electrospinning can be
radicals and reactive oxygen species and reduce the light penetration to the choice of option for the thermally sensitive bioactive molecules
the inner components. This particular use of carotenoids has an which need to be incorporated in the packaging matrix as it can even-
important role in packaging of fatty foods to reduce the light induced tually go for electrospun fiber encapsulation. Bruni et al. [73]. devel-
oxidation effects leading to off flavors generation and negatively oped the encapsulated electrospun fiber by creating and electrospinning
affecting the organoleptic property of the foods. the emulsion of soy protein isolate and polyvinyl alcohol (PVA) with the
soybean oil as carrier agent for β carotene, then it was electrospinned in
6. Techniques of preparation of carotenoid incorporated films (PHB92/ PHV8) film. Results revealed that encapsulation was efficient
in sustained release of bioactive compound to the food matrix. The
Incorporation method of pigments in the packaging material is electrospinning technology can enable the gradual and stable release of
important as it directly impacts the end usage of the polymer. Since the encapsulated bioactive compounds thus protecting the food matrix
polymer serves as the foundation for the addition of pigments, a strong during its shelf life.
synergy between the dosed pigments and polymer is required to main-
tain the desired benefits. Additionally, the pigments chosen must be 6.4. Graft polymerization
compatible with the food in order to preserve its texture and organo-
leptic qualities while it is being packed. Carotenoids are interesting Graft polymerization serves as a useful method for introducing or
molecule used in the recent food packaging system for the development modifying the functional groups in the monomers. It precisely refers to
of smart packaging materials. There are several types of preparation and the technique of reinforcing monomers into polymer matrix via covalent
fabrication of pigment based films, each coming with its own merits and bonding to enhance the wettability, biocompatibility and mechanical
demerit elements, However, the chosen approach must be cost-effective properties. There are several ways of introducing modifications in the
on a commercial level while still providing the desired outcome. The polymer few among them are synthetic, radiation, photochemical graft,
major fabrication methods for pigment incorporation of films includes enzymatic graft, and plasma-actuated grafting strategies. Inkjet printing
solution casting, melt extrusion, mold compression, electro-spinning, is a cost effective and non-contact method of fabricating the film with
photo grafting, inkjet printing and spraying [5]. enhanced sensitivity for detecting the metabolites and can occur via
thermal method or piezoelectric method.
6.1. Solution casting
6.5. Coating deposition method
Solution casting also known by flow drying is one of the versatile and
commonly used method for film preparation. The method follows by The method starts with continuous layer deposition of the polymer
dissolving the polymer in suitable solvent (aqueous or non-aqueous) and with the incorporation of functional molecules leading to the develop-
with the addition of various reinforcement materials like nanoparticles ment of thin film. The coatings provide better protection against envi-
and bioactive compounds to form a homogenous film solution. Then the ronmental factors such as moisture, corrosion, abrasion and the precise
solution goes for evaporation drying under controlled conditions leading alteration of material properties like thickness, composition, structure
to the formation of thin film [71]. Drying temperatures usually range and porosity. There are several methods of depositing coatings- spray
from 20 ◦ C to 60 ◦ C. Solution casting typically results in uniform film coating, dip coating, spin coating, electroplating, physical vapor depo-
thickness and homogeneous distribution of additives and added addi- sition, chemical vapor deposition.
tives and fillers. Careful consideration on the study of compatibility of
the added pigment with the solvent ensures developing the intended 7. Characterization of carotenoid incorporated films
film with bioactive properties.
7.1. Light barrier property
6.2. Melt extrusion
Carotenoids by virtue of its chromogenic molecule possess color
The process starts with forcing the polymer solution through the emitting property ranging from orange, red and yellow. They also act as
extruder subjected to the force of shear, temperature and pressure photo protectors, antioxidants, color attractants, hormone precursors in
leading to the development of polymer [5]. The process allows for photosynthetic and non-photosynthetic plants [74]. The coloring prop-
continuous processing resulting in higher production rate and efficiency. erty of carotenoids is due to nine conjugated double bonds in the
The minimum waste generation and ease of scalability has made the polyene chain, which tends to receive the light. This resonant structure
process very versatile in nature. But the process requires protecting the gets amplified by the presence of existing terminal groups on both sides
bioactive compounds from extreme heat and temperature conditions as of the polyene chain. Terminal groups on the sides of polyene chain
the direct exposure to extrusion condition lead to loss of activity. The modifies the wavelength at which the pigment absorbs light. Greater the
three main components of the extrusion process are: the feeding zone, number of double bonds in the terminal group, higher is the absorbance
where the polymer is mixed evenly under pressure followed by kneading of red color wavelength [74]. The lycopene having higher double bonds
8
S.K. N et al. Measurement: Food 15 (2024) 100190
exhibit red color and the β carotene shows the orange color [75]. Cis significant increase in the oxidation of smart biodegradable films
type of isomer has less color intensity due to the hypsochromic shift in developed from polylactic acid (PLA) and polyhydroxybutryate (PHB).
the wavelength of maximum absorption hence trans isomer is preferred With the addition of natural colorants like β carotene, lutein and cur-
for the colorimetric applications. Carotenoids can be used as freshness cumin a strong antioxidant property in the film gets developed. The
indicators thus increasing the food safety properties by virtue of its color change in color was so prominent in the carotenoids added films
change at altered pH conditions. Generally, pH-responsive colorimetric revealing the sensitivity of the dyes towards weathering and UV ageing
indicators are placed at the headspace or sides of the packaging material >100 h at an elevated temperature of above 60 ◦ C. Medina-Jaramillo
to monitor the metabolites generated (acidic or alkaline) [76,77]. The et al. [87] prepared and evaluated the cassava starch based biodegrad-
generated color stability depends on the unsaturation and stability of able films with the addition of basil leaf extract and green tea extract by
C=C double bonds. The color changing property of carotenoid on ac- casting method. They found a significant color change when the extract
count of scavenging the free radicals can be harnessed for food appli- incorporated films were subjected to pH change in acid and alkaline
cations. Carotenoids are relatively stable, and their color indicating especially more prominent change was seen in the basil leaf extract
property remains unchanged under low acid and neutral conditions in (carotenoid source). Mattish green color was changed to white in acidic
the pH scale of 2–7. However, their stability clearly gets decreased under condition and bright yellow in alkaline condition indicating its effec-
alkaline conditions. This is dependent on the source, method of extrac- tiveness for the colorimetric detection. Colín-Chávez et al. [88] prepared
tion, molecular structure, steric pattern, isomerization, solubility the bilayer coextruded films of HDPE with marigold extract as source of
pattern and functional groups present in the carotenoids which has the astaxanthin/carotenoids with the TiO2 and studied its effect on the
property to respond to the particular metabolites. It is also affected by soybean oil packaging. The co-extrusion strategy was adopted with ca-
the storage temperatures as the natural colors are sensitive to higher rotenoids in the inner packaging matrix protected by TiO2 on the outer
temperatures the response for the pH sensing reactions can be altered layer. TiO2 coextruded films reduced the degradation rate of films due to
drastically. It is reported that carotenoids are sensitive enough and get its UV absorbing capacity. Crystallinity, molecular weight of the used
degraded in presence of heat, light, oxygen, acids, transition metals, or polymers along with the polarity and solubility of the carotenoids plays
interactions with radical species [7,78]. an important role in establishing the diffusion pattern and partition
Asdagh and Pirsa [79] investigated the use of β carotene as a source coefficient of carotenoids to the soybean. Temperature dependent
of antioxidant as a functional packaging material for the butter. There release of carotenoid to the soybean oil was observed which signifies the
was significant change in color of the film of butter from golden orange oxidative stability of the prepared films to the soybean oil. The degra-
to yellow due to the radical scavenging activity of β carotene (dependent dation and release profile of carotenoids is known to get initiated with
on the double bonds) owing to slow and stable release of the carotenoids the generation of excited singlet state in response to light simulation and
from film to food matrix. It has thus improving the oxidative stability of thereby the double bonds in the carotenoid molecule elongate and the
butter. The proximate composition of food such as proteins, fats and oils, neighboring carbon atoms get a partial radical character, which makes
vitamins, and pigments, can break down and produce end products them susceptible to be attacked by a variety of reactants like triplet
when are exposed to UV and visible light during the supply chain, which oxygen molecule leading to its degradation. Hari et al. [89] developed
lowers the food’s quality. Free radicals and reactive oxygen species chitosan-gelatin based active packaging with the incorporation of β
(ROS) are produced as a result of these processes within the food chain. carotene loaded starch nanocrystals and shown that there is a significant
Reactive oxygen species (ROS) have a detrimental effect on food qual- rise in the radical scavenging activity of the β carotene loaded films from
ities, changing its color, flavor, and nutritional profile in addition to 7.81 % to 91.53 ± 0.3 % due to the antioxidant property of β carotene.
producing rancidity. These light-induced effects are most noticeable in
foods rich in fat and protein. Because of their deeper color and ability to 7.2. Mechanical properties
absorb light, carotenoids can also act as a vehicle for the additional
advantage of lowering UV visible light. On the other hand, they can Mechanical properties of the packaging film depend on the nature of
lessen the potential harm that chemicals may cause as well as the risk of polymer, its processing methods and crystalline pattern. They are
their migration to food components. UV barrier property of the colorants important by which the strength and durability of the packaging mate-
incorporated films is determined by light transmittance value or opacity rial gets established during the supply chain. Tensile strength (Ts) and
values. Colorants can increase the compatibility with the polymer elongation at break (Eb) are being evaluated at the lab conditions for the
structure thus affecting the crystalline structure and leading to light mechanical performance of packaging material. Tensile strength (Ts)
reflection [31,80]. Natural colors due to its chemical structure and measures the packaging material ability to perform under the applied
phenolic compounds are able to absorb the light in the wide range of stress prior becoming deformed while the elongation at break (Eb) sig-
wavelight [81,82]. Lino et al. [83] studied on the development of poly ℇ nifies the extent of stretchability which quantifies the ductility. In
caprolactone nanocapsules entrapped β carotene in methylcellulose addition, the type and dose of plasticizer has a role in determining the
films and observed an increase in the opacity values of the films which extent of stretchability. The mechanical property of film depends on the
correspondingly increasing the UV barrier property of the films. Lower complex interplay in the intermolecular forces within the polymer ma-
transmission property of the films in the UV visible region can reduce the trix and the added carotenoids. The addition of carotenoids are known to
effect of light induced lipid oxidation thus giving a better UV visible increase the elongation at break (Eb) and reduce the tensile strength (Ts)
barrier property [84,85]. The UV barrier properties of carotenoid values thereby reducing the Young’s modulus. Stoll et al. [90] developed
incorporated films depends on the proportion of UV-absorbing chro- the polylactic acid film (PLA) with incorporation of bioactive com-
mophores (aromatic amino acids, phenylalanine and disulfide bonds). It pounds lycopene, β carotene and bixin extracted from tomato, carrots
also depends on the phenolic acids and flavonoid profile in the carot- and annatto and evaluated its mechanical properties. Increased con-
enoid. Pirsa and Asadi [79] experimented on the development of centration of extracts in the films increased the lubrication property of
PLA/TiO2/lycopene composite films for the shelf life extension of the film thus increasing the elongation at break (Eb) values, the highest
margarine and found a linear relationship between the change in the being observed with the lycopene and highest increase in the tensile
color of the lyc/TiO2 nanoparticles dosed PLA films with the time and strength was provided by bixin incorporated films 29.9 ± 1.2 MPa. The
temperature. The stability of the margarine coated with active films also carotenoids property of reducing the intermolecular friction between
depends on the storage conditions as there was higher oxidative color the monomers would be a possible reason for increase in strain hard-
change in the refrigerated sample compared to the freezer stored con- ening. The flexibility of the astaxanthin incorporated CMC-gelatin
dition. This establishes the fact that the oxidative damage depends on composite film increased due to increase in the spatial volume be-
the temperature of storage. Latos-Brozio and Masek [86] observed a tween the polymer chain and astaxanthin [31]. The concentration of
9
S.K. N et al. Measurement: Food 15 (2024) 100190
added carotenoids ae known to play a role in reducing the Ts by exhibited a temperature dependent degradation predominantly higher
increasing the crystallization and behaving as plasticizer. Reports by the at 25 and 50 ◦ C as compared with 4 ◦ C. Thermal degradation depends on
scientific investigations revealed an elevation in the tensile strength on the functional groups and the stability associated with the bonding
addition of carotenoids in the polymer matrix thus giving a stable and characteristics [10]. The thermal stability of the carotenoids can be
strong film property due to the establishment of hydrogen bonding and increased by nanoencapsulation technique. The increase in thermal
increasing the interfacial adhesion properties with the polymer. stability is known to confer oxidative stability to the sunflower oil and
fried peanuts as reported in the studies of Asdagh and Pirsa [79];
7.3. Film thickness and water solubility Juan-Polo et al.[95].
Thickness and Water solubility serves as important physical prop- 7.5. Microstructure properties
erties of the films that derive a direct association with the barrier
properties of the films. Greater the thickness of the films better is its Surface characterization studies are characterized by Scanning
resistance to the external disturbances and external shock, vibration and electron microscope (SEM) and Atomic force microscopy (AFM). It re-
gives a higher barrier property. Both the test parameters depend on the veals the surface characteristic pattern and the homogeneity of the
compatibility between the colorants and packaging matrix. The added developed films. A smooth and homogenous matrix is produced by
carotenoids in the film generally shows an increase in the thickness certain colors due to molecular interactions, while certain colors form
values due to the increase in the interactions (hydrophilic/hydrophobic) aggregates and are visible as characteristic specks on the surface of the
with the packaging materials. Addition of β carotene significantly films due to non-compatibility and electrostatic repulsions among the
increased the thickness of films with a cumulative increase in the tensile charged residues. The compatibility between the added polymer and
strength due to the accumulation of β carotene droplets in the pectin color as well as the nature of association between them determines the
matrix thus strengthening the matrix [79]. Water solubility for the extent of homogenity. Addition of carotenoids to the polymer film
carotenoid incorporated films was generally on a reduced scale due to developed rough, cracky structure due to aggregate formation on ac-
the hydrophobic nature of the carotenoids on account of its lipophilic count of its poor compatibility, solubility and electrostatic repulsion
and hydrophobic nature. The solubility has a direct impact on the [96]. Stoll et al. [90] prepared the polylactic acid film (PLA) with the
gravimetric measurement of films. The higher the solubility, greater is incorporation of bioactive compounds lycopene, β carotene and bixin
its drying rate and a consequent rise in the weight loss of the films. extracts from tomato, carrots and annatto and studied for the surface
Development of hydrogen bonds and molecular interactions like elec- characteristic and found the occurrence of surface roughness that can act
trostatic repulsions leads to reduction of water solubility [89,91]. Water as barrier for the light to pass through. There was a drastic reduction in
solubility values were reduced from 88.6 % to 83.4 % and 83.9 % in the the transparency values for the extracts incorporated films. The results
β carotene incorporated films indicating the water repulsive effect of were similar in the studies of De Oliveira Filho et al. [29] where the
carotenoids [92]. Nevertheless, these properties are dependent on the incorporation of mangaba pulp as a source of carotenoids increased the
source of carotenoid and methods of extraction. Films with lycopene opacity of the films and lead to the increased thermal stability.
(extracted from tomato) was having higher water solubility as compared
with the carotenoid (extracted from the shrimp) [92]. 7.6. Barrier properties
7.4. Thermal properties The barrier property of the films plays an important role to in un-
derstanding the movement of air, moisture, and other gas components
Thermal properties of the films indicate the effectiveness of the through the film matrix. Permeability of the film is defined by its
polymer behavior at a higher temperature conditions. Added natural quantification of permeate (gas/water/oxygen) transmission through
colors due to its complex chemical structures are known to alter the resistant medium. This is described by diffusion models of Henrys and
thermal properties of the polymer. Differential scanning calorimetry Ficks law which relates the permeate value with the area and thickness
(DSC) and Thermogravimetric analysis (TGA) are often used to analyze of the films [97]. Water vapor and oxygen are the two major permeates
the thermal properties and stability of the film [93]. DSC studies the studied for the barrier property assessment. The determination of barrier
response of packaging material to the applied heat and assist to predict property becomes necessary to have an account for the shelf life of
the glass transition temperature (Tg), melting temperature (Tm) and products. The dry commodities like biscuits, cookies, dried vegetables,
crystallization temperature (Tc) which are directly dependent on the fried chips are susceptible to oxygen as the entry of oxygen may lead to
crystallinity matrix of the polymer. Higher melting point (Tm) and larger the development of rancidity and associated off-flavors. They are also
enthalpy energy (ΔHm) are generally noticed in the carotenoid incor- susceptible to moisture gain as it may lead to poor sensory attributes
porated films due to the molecular chain reorganization and complex (loss of crispiness in chips, loss of crunchiness in biscuits and cookies).
chemical structure which aims to reduce the mobility of the monomers Barrier properties to moisture and oxygen is evaluated by quantifying
but in few cases the added colorants led to reduction in thermal prop- the values of water vapor transmission rates (WVTR) and oxygen
erties due to weakening of molecular interactions while the TGA studies transmission rate (OTR). WVTR is generally depicted by water vapor
the relative changes in weight of the polymer as a function of time and permeability coefficients which measures the amount of water vapor
temperature. It reflects on the decomposition, oxidation reactions, permeated through unit area in unit time (g/m2 per day) while OTR is
physical transformations like sublimation, vaporization etc. which is expressed as the quantity of oxygen permeating through the unit area
dependent on the proportion of bound water and the functional groups and unit time and expressed by oxygen permeation coefficients. Addi-
provided by the colorants, monomers and additives added for the tion of colorants like carotenoids creates crosslinks with the existing
fabricating the films. Studies have shown that addition of carotenoids polymer and develop torturous pathway that reduces the diffusion of
increases the thermal stability due to its antioxidant nature. There is moisture and gases. Diffusibility of carotenoid molecule depends on the
considerable reduction in glass transition temperature (Tg) owing to attainment of activation energy (Ea) created by the polymer matrix. In
increased flexibility. There were reports of delayed thermal degradation the reported studies of Colín-Chávez et al. [88] the film blend containing
due to hydrogen bonding of carotenoid molecule with the polymer marigold extract took 53.66 kJ mol− 1 to undergo the complete diffusion.
matrix and formation of crystallites. Thermal stability of the norbixin The diffusion of carotenoids can be extended by the addition of nano-
was higher than lycopene and zeaxanthin as observed in the TGA studies materials or nanoencapsulation technique thereby prolonging the
of cellulose acetate films prepared with the extracts of tomato, gojiberry release. Additionally, by virtue of its insolubility and hydrophobic na-
and annatto. In the reported studies of Yuan et al. [94] astaxanthin ture carotenoid incorporated films generally lead to the reduction of
10
S.K. N et al. Measurement: Food 15 (2024) 100190
Table 3
Carotenoid application and properties of the films with various applications.
S. Type of carotenoid Polymer base Film forming method Food matrix Properties Reference
no
1 β-Carotene, lutein Polylactide and PHB Single screw extruder NA *Higher oxidation temperature (To) [102]
and curcumin observed due to antioxidant behavior of the
colorants
*Reduction in transparency of films.
*Reduction in tensile strength and
elongation at break as compared with
control.
2 β-carotene, lycopene, Polylactic acid Solution casting Sunflower oil *Enhanced UV–visible light barrier property [103]
and bixin *Lower peroxide value in bixin
incorporated films
3 Basil extract Cassava starch Solution casting NA *Increased sensitivity to color change in [87]
acid and alkaline condition coupled with
lower water vapor permeability as
compared with green tea extract
4 Oil palm extract as Cassava starch Solution casting Butter *Higher values for tensile strength at 0.03 % [98]
colorant source incorporation.
*Lower water vapor permeability
*Increase in total carotenoids of butter by
154.9 % after 45 days of storage
5 Mangaba pulp Alginate Solution casting NA *Reduced water solubility and water vapor [29]
permeability
*Higher thermal stability, tensile strength,
and elongation at break.
*Increased opacity of films
* Increased antioxidant property of the films
and improved barrier to UV–visible light
6 Mango pulp Cassava starch Solution casting Palm oil *Increased total carotenoid content of films [104]
of 44.22 μg/g.*Lower rate of oxidation in
the mango pulp fabricated film packed palm
oil.
7 β-carotene loaded Chitosan-gelatin starch Solution casting NA *Increased opacity of films.*Increase in the [89]
starch nanocrystals radical scavenging activity of β- carotene
loaded films to 91.53 %*Increased
crystallinity of films
8 Astaxanthin Carboxymethyl cellulose/ Solvent casting NA *Increased hydrophobicity and opacity of [31]
octenyl succinic anhydride/ films*Increased anti-radical capacity at 0.25
gelatin % concentration of astaxanthin.
9 β-carotene Shrimp muscle protein Solvent casting NA *Commercial β carotene reduced the water [92]
solubility values from 88.6 % to 83.4 %*
Increased oxygen barrier property with 5
fold reduction in oxygen permeability from
174.12 to 34.06 cm3 μm/m2/day
10 Astaxanthin from Chitosan Solvent casting NA *Tensile strength increased from 22.25 to [103]
shrimp waste 28.09 MPa with concomitant decrease in
the EB values from 35.35 % to 32.17 %
11 β- carotene LDPE/EVOH/PET Cast film extrusion Fried peanuts *Increased thermal stability due to increase [95]
in ΔH enthalpy (120.5 J/g)*Increased L*
and b* values*Higher oxygen induction
time with reduced oxygen absorbing
capacity of 1.7 ± 0.3 mL O2 per g of the
film.*Lowered rate of hexanal release
(marker of oxidation)
12 Lycopene and β- Sodium alginate Solvent casting Sunflower oil *Reduced water vapor [105]
carotene permeability*Increased thermal
stability*Reduced oxidative damage to the
sunflower oil
13 Tomato pulp PVA/gelatin Solvent casting Minced chicken meat *Reduced the rancidity of chicken meat in [106]
(lycopene) chilled condition up to 12 days* 2 log and 3
log reduction against Bacillus cereus and
Staphylococcus aureus respectively.
14 Bixin nanocapsules Cassava starch Solvent casting Sunflower oil * Higher thermal stability upto 270 ◦ C.* [107]
Increased water vapor permeability at 10 %
incorporation.* Increased UV barrier
property with reduced oxidative damage to
sunflower oil (12.6 mEq/kg)
15 Carotenoprotein Chitosan Solvent casting NA *Increase in hydrophobicity and opacity of [108]
extract from blue crab the films (reduction of 14 % in L*)
shell *Increased thickness (53.0 ± 0.67 µm) but a
reduction is seen the tensile strength and
elongation at break values.
16 Oily tomato extract Gelatin Solvent casting NA *Increased light barrier property to UV and [101]
(source of lycopene visible at 5 % incorporation of oily tomato
and β-carotene)
(continued on next page)
11
S.K. N et al. Measurement: Food 15 (2024) 100190
Table 3 (continued )
S. Type of carotenoid Polymer base Film forming method Food matrix Properties Reference
no
water transmission. Perazzo et al. [98] prepared the cassava starch [28]. López-Palestina et al. [101] prepared the gelatin based films
based film with the incorporation of green tea extract and commercially containing oily tomato extract (as a source of lycopene and β carotene).
available oil palm extract containing (35 % α-Carotene and 65 % Reduction of water vapor permeability values was observed up to 64.49
β-Carotene) and showed a significant reduction in water vapor perme- % in 5 % incorporated oily tomato extract due to hydrophobic nature of
ability (WVP) mainly attributed to the interactions of carotenoid com- the extract. In this way the carotenoids can enhance the barrier property
pounds to the hydrophobic region of the leached amylose and of the films. The polymer matrix, method of film forming and the
amylopectin molecules via vander walls force thus limiting the water compatibility with the polymer base are the factors to be considered
available for starch binding [99]. The developed films were evaluated by during the formulation. The list of different sources of carotenoids with
butter packaging and observed for 45 days at accelerated oxidation their potential application and significant results has been compiled in
conditions with LDPE coated butter as the control, and found that Table 3.
carotenoid extract incorporated film had significant impact in reducing
the peroxide values which inturn suggest the oxidative protection role. 8. Future outlook and considerations
The level of 0.5 % incorporation of carotenoids (β carotene and lyco-
pene) in the development of sodium alginate films lead to significant Despite the fact that a lot of research has been done on the use of
reduction of water vapor permeability values [100]. The crystallinity of natural colorants in food packaging systems, there is still a gap regarding
selected packaging material has a role in reducing the diffusibility of scale-up and future applications of carotenoids in potential food pack-
carotenoids. Among the carotenoid sources (β carotene, lycopene and aging applications. The gap can be of considerable economics involved
bixin) used in the development of polylactic acid films as a protective in sourcing, extracting and utilizing the carotenoids for film develop-
packaging material for sunflower oil. It was found that non-polar nature ment and can be the loss of compatibility between the added colorants
of β carotene and lycopene had a significant reduction in oxygen and base polymer matrix. Reported studies have presented considerable
transmission rates (OTR) as compared with bixin incorporated films variation in the carotenoid concentration, film development techniques
12
S.K. N et al. Measurement: Food 15 (2024) 100190
which has made pigment-incorporated film technology not competent Declaration of competing interest
and stable enough to gain traction in the marketplace. Film and carot-
enoid compatibility needs to be synergized by intervening additives like The authors declare that they have no known competing financial
hydrophilic and hydrophobic plasticizers, nano materials, composite interests or personal relationships that could have appeared to influence
films preparation [110]. It’s necessary to develop standard techniques the work reported in this paper.
that can accurately produce the required outcomes for detecting and
identifying the metabolite created by chromogenic molecules. This can Disclosure
be accomplished by integrating image processing equipment that are
able to precisely and immediately respond to the metabolite created at The authors are not aware of any affiliations, memberships, funding,
ppm and ppb levels. or financial holdings that might be perceived as affecting the objectivity
The stability of the added carotenoids can be enhanced by following of this review.
encapsulation techniques or nanoparticle formation or electrospinning
technique to deliver carotenoids in a stable and sustained manner. Non- References
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