Biological Trace Element Research (2019) 190:242–250

https://doi.org/10.1007/s12011-018-1538-0

Toxic Metals and Trace Elements in Artisanal Honeys

from the Canary Islands
Saray Díaz 1 & Soraya Paz 1 & Carmen Rubio 1 & Ángel J. Gutiérrez 1 & Dailos González-Weller 2 & Consuelo Revert 1 &
Antonio Bentabol 3 & Arturo Hardisson 1

Received: 11 July 2018 / Accepted: 27 September 2018 / Published online: 5 October 2018
# Springer Science+Business Media, LLC, part of Springer Nature 2018

Abstract
Honey is a natural product made by honey bees from the nectar of flowers or secretions produced by other living plant parts. The
metal content of the honeys is related to the levels of metals in the environment. Due to the importance of honey in the human diet
and the increase of environmental pollution, it is necessary to determine the content of metals in honey to evaluate the toxicological
risk derived from its consumption. The objective of this study was to determine the content of 20 metals (Al, B, Ba, Ca, Cd, Co, Cr,
Cu, Fe, K, Li, Mg, Mn, Mo, Na, Ni, Pb, Sr, V, and Zn) in different samples of artisanal honey from the Canary Islands (Spain) in
order to evaluate the dietary intake derived from the consumption of these honeys. A total of 161 samples of different types of
Canary honey were analyzed by ICP-OES (inductively coupled plasma–optical emission spectrometry). K (825 mg/kg) was the
macroelement found in highest concentration, while B (4.25 mg/kg) was the trace element with the highest mean concentration. Al
(3.33 mg/kg) was the most abundant toxic metal, followed by Pb (0.040 mg/kg) and Cd (0.002 mg/kg). A mean consumption of
25 g/day of honey mainly contributes to the recommended daily intake of Cu (1.34% adults) and K (0.67% adults). As regards the
toxic metals, the contribution percentage to the TDI (tolerable daily intake) of Pb at 2.92% for adults is noteworthy. However, the
consumption of honey does not imply a high intake of metals and, therefore, does pose a risk to the health of adult men and women.

Keywords Honey . Metals . Bioaccumulation . Contaminants . ICP-OES . Risk assessment

Introduction used [3]. Honeys can accumulate metals from nectar, which in
turn come from the plants that produce it [4, 5]. Studies have
Honey is a natural product produced by Apis mellifera bees shown a high correlation between the content of metals in
from the nectar of flowers or secretions from other plant parts. honey and their concentration of these in the environment,
The bees extract the nectar and, after combining it with other and thus, honey can be used as an indicator of environmental
specific substances, they store it in the cells of the hive for its pollution [6–8].
subsequent maturation [1, 2]. Due to its sweet taste, honey is widely used as a sweetener,
The composition and, therefore, the properties of honey even as a substitute for sugar. The honeys have common char-
depend on the botanical origin of the nectar and the secretion acteristics in terms of their major constituents making it nec-
essary to resort to their minority constituents to classify them
into different types and even to detect fraud in their declared
origin [3].
* Ángel J. Gutiérrez
[email protected]
The concentrations of metals vary in the different types of
honey, since they depend on the elemental composition of the
1
flowers and the botanical and geographical origin of the flow-
Department of Toxicology, Universidad de La Laguna, La Laguna,
er [9, 10]. Therefore, the content of metals or trace elements in
Tenerife, Canary Islands, Spain
2
the honeys can be used to distinguish the different geograph-
Health Inspection and Laboratory Service, Canary Health Service
ical origins of the honey [3, 11–13].
S/C de Tenerife, Tenerife, Canary Islands, Spain
3
The honey produced in the Canary Islands is monofloral
Casa de la Miel, Unidad de Valorización de Productos
and there is a wide variety of these honeys mainly due to the
Agroalimentarios, Área de Agricultura, Ganadería y Pesca,
Tenerife, Canary Islands, Spain diversity of the flora on the islands as well as to their
Toxic Metals and Trace Elements in Artisanal Honeys from the Canary Islands 243

microclimatic conditions. The particular conditions of each Sample Treatment

flower or plant increase the value of the honey.
Furthermore, honey is a source of metals such as the Five grams of each sample, previously homogenized, were
macroelements or major elements (Ca, K, Na, and Mg) needed weighed into porcelain capsules (Staalich, Germany) using a
by humans in large quantities, the trace elements (Mn, Fe, Cu, precision balance (Mettler Toledo, USA) and subjected to
Zn, Cr, Mo, and Co) which are necessary for the healthy drying at 70 °C for 24 h in an desiccation oven
development of physiological functions, the nonessential trace (Nabertherm, Germany). Acid digestion of the samples was
elements (Ni, Sr, V, Li, B, and Ba) that are naturally found in then carried out with 65% HNO3 (Sigma–Aldrich, Germany).
food and can be toxic in high concentrations [14, 15], and the After digestion, the samples were incinerated in a muffle fur-
toxic metals (Al, Cd and Pb) which are contaminating ele- nace (Nabertherm, Germany) at 450 °C for 24 h, with the
ments and toxic even at low concentrations [16–18]. temperature being increased by 50 °C/h. The white ashes ob-
However, the level of the abovementioned elements is lower tained were dissolved in 25 mL of 1.5% HNO3 [14, 21]. The
in comparison with the other compounds that can be found in solutions were transferred to sterile polypropylene containers
honeys [19, 20]. for subsequent analysis. Each sample was performed in
Bearing in mind the increase in environmental pollution triplicate.
and its influence on natural products such as honey as well
as on its nutritional contribution, it was decided to determine Method and Quality Control
the content of elements of nutritional interest and toxic metals
in order to evaluate the nutritional contribution and the toxic The analysis of the samples was performed by ICP-OES (in-
risk derived from the consumption of Canary honey. ductively coupled plasma atomic emission spectroscopy)
using a Thermo Scientific iCAP 6000 series spectrometer
(Waltham, USA) with the following instrumental conditions:
approximate RF power, 1.2 kW; gas flow (nebulizer flow,
Material and Methods auxiliary flow), 0.5 L/min; pump speed, 50 rpm; stabilization
time, 0 s [17, 18].
Samples The instrumental wavelengths for each metal (nm) were as
follows: Al (167.0), B (249.7), Ba (455.4), Ca (317.9), Cd
A total of 161 samples of traditional Canary honeys were (226.5), Co (228.6), Cr (267.7), Cu (327.3), Fe (259.9), K
analyzed. The samples were acquired in the BCasa de la (769.9), Li (670.8), Mg (279.1), Mn (257.6), Mo (202), Na
Miel^ (Tenerife, Spain). Table 1 shows the characteristics (589.6), Ni (231.6), Pb (220.3), Sr (407.7), V (310.2), and Zn
about the analyzed samples. (206.2).

Table 1 Characteristics of the analyzed honey samples

Botanical origin of honeys Local name Color Honey types No. of Origin Season Collection
samples year

Spartocytisus supranubius Teide broom Amber Unifloral 11 Tenerife North Spring–summer 2016
Echium spp Tajinaste White 10
Mentha pulegium Pennyroyal Amber 10 Summer
Castanea sativa Chestnut Dark 10
Bituminaria bituminosa Arabian pea Light amber 10 Spring
Honeydew Dark amber 10
Foeniculum vulgare Fennel Dark amber 10 Summer
Gran Canaria Island plants Light amber Multifloral 10 Gran Canaria South –
Achyranthes aspera Chaff-flower Light amber Unifloral 10 Tenerife North Summe–Autumn
Mesembryanthemum Ice plant or barrilla White 10 Spring–Summer
crystallinum
Lotus berthelotii Coral gem Light amber 10 Summer
Calendula officinalis Pot marigold White 10
Origanum vulgare Oregano Light amber 10 2014
Persea americana Avocado Dark 10 Spring 2015
Erucastrum canariense Relinchón Light amber 10 2016
Agave Amber 10 Summer 2014
244 Díaz et al.

The instrumental detection and quantification limits subjecting the reference materials to the same analytical pro-
(mg/L) were calculated according to the instrumental re- cedure as the samples. No significant differences were found
sponse of the equipment under conditions of reproducibil- (p < 0.05) between the certified concentration and the one
ity by means of the analysis of 15 targets [22]. The limits of found here.
detections (LODs) are as follows: Al (0.004), B (0.003),
Ba (0.001), Ca (0.58), Cd (0.0003), Co (0.0006), Cr
(0.003), Cu (0.004), Fe (0.002), K (0.565), Li (0.005), Calculations for the Intake Evaluation
Mg (0.583), Mn (0.002), Mo (0.0007), Na (1.097), Ni
(0.0007), Pb (0.0003), Sr (0.0007), V(0.001), and Zn The evaluation of the intake was based on the calculation of
(0.002).The limits of quantification (LOQs) are as follows: the estimated daily intake (EDI), and was calculated using
Al (0.012), B (0.012), Ba (0.005), Ca (1.955), Cd (0.001), the mean concentration of each metal found in the honeys
Co (0.002), Cr (0.008), Cu (0.012), Fe (0.009), K (1.884), and the mean consumption of the honeys, as shown below
Li (0.013), Mg (1.943), Mn (0.008), Mo (0.002), Na [24, 25]:
(3.655), Ni (0.003), Pb (0.001), Sr (0.003), V (0.005),
and Zn (0.007). EDI ðmg=dayÞ
The accuracy and precision of the method was verified by ¼ Mean honey consumption ðkg=day=personÞ
performing a quality control procedure based on the percent-
ages of recovery of certified reference materials (CRM) sim-  Metal concentration ðmg=kgÞ
ilar to the sample under study. These materials, chosen for
their high carbohydrate content such as honey [23], were typ- The estimated daily intake is a value that, in this case,
ical diet (SRM 1548a, NIST, USA), apple leaves (SRM 1515, represents the quantity of metal intake per day according to
NIST, USA), and wheat flour (SRM 1567a, NIST, USA). the daily consumption of honey. After calculating the EDI of
There were no available reference materials for lithium; for each metal, the percentage of contribution to the recommend-
that reason, the standard addition method was used. The stan- ed or maximum values established was calculated as follows:
dard addition method is based on the addition of a known Contribution percentage
concentration of Li to samples previously dehydrated.
Table 2 shows data from the recovery study obtained after ¼ ½EDI ðmg=dayÞ : Limit value 100

Table 2 Certified concentration

in mg/kg (mean ± SD, n = 3) of Material Metal Obtained concentration Certified concentration R (%)
the reference materials and (mg/kg) (mg/kg)
recovery study (%) of the
analyzed metals SRM 1515 apple leaves Al 286 ± 9 285.1 ± 26 99.7
B 27.0 ± 2.0 27.0 ± 1.5 99.9
Cr 0.30 ± 0.00 0.29 ± 0.03 97.8
Mo 0.09 ± 0.01 0.09 ± 0.02 99.4
Sr 25.0 ± 2.0 24.6 ± 4.0 98.3
SRM 1548a typical diet Ba 1.10 ± 0.10 1.13 ± 0.09 102.5
Ni 0.37 ± 0.02 0.38 ± 0.04 102.3
Pb 0.044 ± 0.000 0.044 ± 0.013 98.9
SRM 1567a wheat flour Ca 0.02 ± 0.00 0.02 ± 0.02 101.4
Cd 0.026 ± 0.002 0.026 ± 0.008 98.4
Co 0.006 ± 0.00 0.006 ± 0.002 102.4
Cu 2.1 ± 0.2 2.09 ± 0.4 99.7
Fe 14.1 ± 0.5 13.9 ± 0.3 98.9
K 0.133 ± 0.003 0.132 ± 0.02 99.3
Mg 0.04 ± 0.00 0.04 ± 0.03 102.6
Mn 9.4 ± 0.9 9.6 ± 1.5 102.4
Na 6.1 ± 0.8 6.1 ± 0.3 99.2
V 0.011 ± 0.00 0.011 ± 0.00 99.4
Zn 11.6 ± 0.4 11.9 ± 0.2 102.7
Standard addition method Li 0.20 ± 0.02 0.19 ± 0.03 95.0
Toxic Metals and Trace Elements in Artisanal Honeys from the Canary Islands 245

Statistical Analysis followed by Na > Ca > Mg is worth mentioning (Fig. 1a).

Some studies have reported that honeys from islands, as for
The statistical analysis was performed with the IBM Statistics example, the Canary Islands, tend to accumulate higher con-
SPSS 22.0 for Mac® program. This analysis determined the centrations of macroelements, mainly K and Na, because the
existence or not of significant differences (p < 0.05) between sea is a source of these alkaline metals that are in marine spray
the different types of honeys. Firstly, the normality of the data [3, 23, 34]. In terms of the trace elements (Fig. 1b), the mean
was verified by the Kolmogorov–Smirnov and Shapiro–Wilks concentrations of B (4.25 mg/kg) and Fe (1.95 mg/kg) are
tests. The data did not follow a normal distribution and were noteworthy, followed by the other trace elements Zn > Mn >
evaluated by a nonparametric study using the Kruskal–Wallis Li > Sr > Cu > V > Ba > Ni > Mo > Cr > Co. Finally, Al is the
test [26–28]. most notable toxic metal (Fig. 1c) with a mean concentration
of 3.33 mg/kg, followed by Pb and Cd.
The European Commission Regulation (EC) No 1881/
Results and Discussion 2006 of 19 December 2006 which set the maximum content
of certain contaminants in food products did not set any max-
Table 3 shows the mean concentrations (mg/kg) and standard imum limit of Cd in honeys [35]. However, there is a maxi-
deviations of the metals studied according to the type of hon- mum limit of Pb in honeys set on 0.10 mg/kg [36].
ey. K is the most noteworthy element found in all the honey Table 4 shows the mean concentrations of metals in honeys
types, with the highest mean concentration (1848 mg/kg) found by other authors. In the study of Fernández-Torres et al.
found in honeydew honeys. Several studies have concluded [39], in which samples of honeys from Spain were analyzed,
that K is one of the most abundant elements in honeys, so the Cu, Ca, K, and Zn concentrations were found to be similar to
results obtained in the present study are in agreement with this the mean concentrations in the present study. The samples
fact [29]. In addition, honeydew contains the highest mean analyzed by Fernández-Torres et al. [39] were produced in
levels of Na (311 mg/kg) and Mg (94.5 mg/kg). Spain.
The most noteworthy concentrations of the trace elements In another later study conducted by Frías et al. [38] in
were the B content (6.74 mg/kg) in the barrilla honey. which honey samples from the island of Tenerife were ana-
Avocado honeys, which is a dark honey, had the highest levels lyzed, Cd, Fe, Cu, and Zn concentrations were reported to be
of essential trace elements such as Zn (4.53 mg/kg), Fe higher than those found here, but the mean concentration of
(3.91 mg/kg), or Cu (1.31 mg/kg). Pb found by Frías et al. [38] is similar to the one obtained in
As regards the toxic metals, the mean level of Al the present study. It should be noted that the study of Frías
(8.13 mg/kg) and Cd (0.006 mg/kg) in the avocado honeys et al. [38] was conducted 10 years before the present study and
is worth mentioning. the environmental conditions would have changed.
The honey types containing the highest levels of metals are On the other hand, results obtained by Rashed and
avocado and honeydew honeys, which are dark honeys. Some Soltan [40] in samples of sesame honey from Egypt, show
authors conclude that dark honeys contain higher mineral con- markedly higher concentrations of Fe, Cu, Cd, and K than
tent than pale honeys [30, 31]. The dark color may indicate a those found here. Przybylowski and Wilczynska [6], who
higher mineral level. analyzed the content of metals in honeys from Poland,
The statistical analysis revealed significant differences found a mean level of Zn higher than that of the present
(p < 0.05) for the elements studied, as shown in Table 3. study, and very similar Cd and Pb levels to those found in
The most notable differences were those found in the con- the samples analyzed here.
tent of Ca, K, Mg, and Na in the chestnut, honeydew, avo- Soil composition, botanical origin, beekeeper practices,
cado (except for Ca), and fennel (only for Ca) honeys com- honey processing, and environmental pollution directly influ-
pared to the other honeys. In addition, there are statistical ence the metal content of honey [32], so countries like Egypt
differences in Cu, Fe, Zn, and Al levels among avocado or Turkey, with serious environmental pollution problems
honeys and the other honey types. These significant differ- [10], generally speaking, produce honeys with higher concen-
ences may be due to multiple factors such as botanical trations of toxic metals while the honey from other countries,
origin, season, and area. Even in the same honey types from such as Spain or Poland, have lower concentrations of toxic
the same botanical origin, it is possible to find differences metals. The Canary Islands, which are part of the Macaronesia
in the metal content because there are multiple factors that region, are islands without important industrialized areas; for
can influence in the metal levels as for example the collec- that reason, the levels of toxic metals (Cd, Al, Pb) should be
tion season [19, 32, 33]. For that reason, the metal content lower due to the low anthropogenic impact. However, volca-
of honeys could fluctuate widely. nic regions as the Canary Islands can accumulate higher metal
As regards the mean concentration of the macroelements concentrations in the soil and in the environment that could
without differentiating by type, the K content (825 mg/kg) influence the metal content of honeys [23].
Table 3
246

Concentration of each metal (mg/kg) and standard deviations (SD) of the Canary honeys

Teide broom Tajinaste Pennyroyal Chestnut Arabian pea Honeydew Fennel Gran Canaria

Ca 56.4 ± 2.3 54.0 ± 3.4 69.1 ± 5.0 145 ± 10.0* 49.0 ± 1.2 107 ± 9.4* 98.9 ± 6.7* 74.9 ± 4.0
K 360 ± 22.0 411 ± 15.0 365 ± 12.3 1833 ± 30.0* 407 ± 11.5 1848 ± 50.0* 588 ± 20.3 910 ± 14.3*
Mg 20.5 ± 2.1 16.7 ± 1.5 19.3 ± 4.4 91.2 ± 3.5* 17.5 ± 1.5 94.5 ± 6.8* 24.5 ± 2.3 36.3 ± 1.1
Na 84.6 ± 5.6 85.3 ± 10.1 104 ± 10.0 200 ± 5.6* 87.7 ± 2.3 311 ± 5.3* 147 ± 4.5 149 ± 9.2
B 1.84 ± 0.7* 2.80 ± 0.8 3.49 ± 0.6 4.88 ± 1.0 4.95 ± 0.5 6.36 ± 0.6 5.76 ± 1.0 3.37 ± 0.5
Ba 0.251 ± 0.02 0.216 ± 0.01 0.152 ± 0.01 0.470 ± 0.01 0.169 ± 0.04 0.203 ± 0.03 0.296 ± 0.02 0.534 ± 0.01
Co < LOD < LOD 0.001 ± 0.0 < LOD 0.004 ± 0.0 0.001 ± 0.0 0.008 ± 0.0 0.010 ± 0.0
Cr 0.011 ± 0.0 < LOD 0.013 ± 0.0 < LOD < LOD 0.006 ± 0.0 < LOD < LOD
Cu 0.913 ± 0.04 0.415 ± 0.01 0.593 ± 0.01 0.535 ± 0.01 0.250 ± 0.01 0.831 ± 0.01 0.450 ± 0.02 0.300 ± 0.0
Fe 1.39 ± 0.5 0.891 ± 0.03 1.36 ± 0.2 2.22 ± 0.2 0.703 ± 0.03 3.70 ± 0.8* 3.65 ± 0.4* 1.11 ± 0.3
Li 0.865 ± 0.6 0.704 ± 0.02 0.553 ± 0.01 0.954 ± 0.1 0.400 ± 0.05 0.898 ± 0.01 0.723 ± 0.03 0.894 ± 0.02
Mn 2.00 ± 0.2 0.834 ± 0.1 0.412 ± 0.0 1.84 ± 0.02 0.194 ± 0.07 1.84 ± 0.1 0.468 ± 0.05 0.518 ± 0.04
Mo 0.002 ± 0.0 < LOD 0.009 ± 0.0 0.008 ± 0.0 < LOD 0.073 ± 0.01 0.013 ± 0.04 < LOD
Ni 0.025 ± 0.0 0.016 ± 0.0 0.009 ± 0.0 0.033 ± 0.0 0.023 ± 0.0 0.061 ± 0.0 0.031 ± 0.0 0.071 ± 0.0
Sr 0.376 ± 0.02 0.441 ± 0.04 0.477 ± 0.01 1.09 ± 0.1 0.372 ± 0.01 0.673 ± 0.02 0.659 ± 0.01 1.49 ± 0.3
V 0.078 ± 0.0* 0.092 ± 0.01* 0.619 ± 0.03 0.450 ± 0.02 0.064 ± 0.0* 0.521 ± 0.06 0.878 ± 0.1 0.811 ± 0.01
Zn 0.99 ± 0.01 0.80 ± 0.1 0.97 ± 0.1 0.87 ± 0.03 0.68 ± 0.06 2.40 ± 0.15* 0.87 ± 0.06 0.66 ± 0.01
Al 1.57 ± 0.2 1.58 ± 0.4 0.923 ± 0.03 8.00 ± 1.1* 0.703 ± 0.05 4.67 ± 0.2 6.51 ± 0.7* 1.46 ± 0.7
Cd 0.000 ± 0.0 0.001 ± 0.0 0.002 ± 0.0 0.003 ± 0.0 < LOD 0.006 ± 0.0 0.003 ± 0.0 0.002 ± 0.0
Pb 0.019 ± 0.0 0.023 ± 0.0 0.035 ± 0.0 0.053 ± 0.0 0.057 ± 0.01 0.051 ± 0.0 0.049 ± 0.0 0.043 ± 0.0

Chaff-flower Barrilla Coral gem Pot marigold Oregano Avocado Relinchón Agave

Ca 54.6 ± 2.3 45.7 ± 1.1 33.7 ± 7.5 46.8 ± 1.7 78.7 ± 2.2 54.9 ± 1.7 29.1 ± 1.4 67.7 ± 2.6
K 407 ± 10.1 555 ± 9.6 161 ± 4.5 278 ± 2.3 299 ± 5.6 1490 ± 10.2* 201 ± 10.3 633 ± 21.0
Mg 16.7 ± 3.3 24.7 ± 1.4 5.4 ± 0.6 17.5 ± 1.7 18.4 ± 1.9 78.3 ± 1.8* 11.0 ± 1.1 25.8 ± 2.3
Na 99.4 ± 2.3 141 ± 1.2 69.4 ± 4.5 110 ± 7.3 105 ± 5.3 244 ± 5.6* 21.0 ± 3.2 102 ± 6.2
B 3.52 ± 0.6 6.74 ± 0.4 4.89 ± 1.0 4.81 ± 0.6 0.677 ± 0.01* 4.94 ± 0.5 3.97 ± 0.8 5.01 ± 1.0
Ba 0.183 ± 0.05 0.478 ± 0.01 0.203 ± 0.02 0.162 ± 0.02 0.310 ± 0.09 0.391 ± 0.01 0.171 ± 0.02 0.165 ± 0.02
Co < LOD < LOD < LOD 0.005 ± 0.0 0.019 ± 0.0 0.009 ± 0.0 0.005 ± 0.0 0.005 ± 0.0
Cr 0.024 ± 0.0 < LOD < LOD < LOD < LOD 0.016 ± 0.0 < LOD < LOD
Cu 0.450 ± 0.1 0.530 ± 0.1 0.334 ± 0.06 0.324 ± 0.01 0.257 ± 0.0 1.31 ± 0.03* 0.286 ± 0.03 0.342 ± 0.05
Fe 0.932 ± 0.3 1.13 ± 0.3 0.635 ± 0.01 0.634 ± 0.05 1.02 ± 0.4 3.91 ± 0.4* 1.04 ± 0.1 1.27 ± 0.2
Li 0.359 ± 0.05 0.880 ± 0.05 0.320 ± 0.02 0.286 ± 0.06 1.23 ± 0.3 2.11 ± 0.3 0.231 ± 0.05 0.468 ± 0.01
Mn 0.362 ± 0.01 4.42 ± 0.6* 0.105 ± 0.01 0.234 ± 0.05 0.229 ± 0.05 0.571 ± 0.01 0.134 ± 0.03 0.417 ± 0.01
Mo 0.010 ± 0.0 0.017 ± 0.0 0.012 ± 0.0 < LOD < LOD 0.059 ± 0.0 0.014 ± 0.0 < LOD
Ni 0.014 ± 0.0 0.026 ± 0.0 0.014 ± 0.0 0.029 ± 0.0 0.014 ± 0.0 0.079 ± 0.0 0.018 ± 0.0 0.148 ± 0.06
Sr 0.526 ± 0.1 0.668 ± 0.1 0.520 ± 0.01 0.429 ± 0.01 3.32 ± 0.4* 0.459 ± 0.02 0.148 ± 0.01 0.776 ± 0.04
V 0.797 ± 0.1 0.846 ± 0.05 0.794 ± 0.08 0.848 ± 0.06 0.877 ± 0.05 0.465 ± 0.06 0.268 ± 0.03 0.285 ± 0.01
Zn 0.74 ± 0.03 1.15 ± 0.2 0.72 ± 0.06 0.76 ± 0.04 0.44 ± 0.04 4.53 ± 0.7* 1.99 ± 0.1* 0.87 ± 0.02
Díaz et al.
 Table 3 (continued)

Chaff-flower Barrilla Coral gem Pot marigold Oregano Avocado Relinchón Agave

Al 1.42 ± 0.4 1.29 ± 0.1 0.480 ± 0.1 0.391 ± 0.02 1.50 ± 0.3 8.13 ± 0.3* 1.85 ± 0.03 1.24 ± 0.4
Cd 0.002 ± 0.0 < LOD < LOD 0.005 ± 0.0 < LOD 0.006 ± 0.0 0.005 ± 0.0 < LOD
Pb 0.026 ± 0.0 0.038 ± 0.01 0.041 ± 0.0 0.052 ± 0.0 0.052 ± 0.0 0.052 ± 0.0 0.037 ± 0.0 0.043 ± 0.0

*Significant differences (p < 0.05)

Toxic Metals and Trace Elements in Artisanal Honeys from the Canary Islands

(mg/kg) of the trace elements. c Mean content (mg/kg) of the toxic metals
247

Fig. 1 a Mean content (mg/kg) of the macroelements. b Mean content

248 Díaz et al.

Table 4 Metal concentration obtained by other authors for different honey types and geographical locations

Author Honey type/country Concentration (mg/kg)

Fe Cu Zn Pb Cd K Ca Na Mg Co Mn

Ru et al. [37] Different types – 46.18* 1329.5* 33.98* 1.34* – – – – – –

(n = 48)/China
Fríaset al. [38] Different types 3.37 1.28 2.83 37.33* 4.38* – – – – – –
(n = 140)/Tenerife
(Spain)
Fernández-Torres Different types – 0.531–2.117 1.332–7.825 – – 434.1–1935 42.59–341.0 – – – –
et al. [39] (n = 40)/Spain
Rashed&Soltan [40] Sesame honey/Egypt 202 1.70 – – 12.5 1500 – – – – –
Przybytowski & Different types – – 7.76 0.048 0.015 – – – – – –
Wilezynska [6] (n = 15)/Poland
Yilmaz&Yavuz [12] Different types 6.6 1.8 2.7 – – 296 51 118 33 1.0 1.0
(n = 30)/Turkey
The present study, Different types 1.95 0.59 1.91 0.04 0.002 825 78.8 146 40.2 0.003 0.91
2018 (n = 161)/Tenerife
(Spain)

*Expressed in μg/kg

Evaluation of Dietary Intake and Nutrition Societies and Dietetics [48]. Furthermore, this
daily consumption would provide a Pb contribution of 2.92%
Table 5 shows the estimated daily intakes (EDI) and the per- of the TDI (tolerable daily intake) set at 0.5 μg/kg bw/day by
centages of contribution to the guide values for each of the the Spanish Agency for Consumer Affairs, Food Safety and
metals studied. Suggesting a consumption of 25 g of honey Nutrition [46]; this contribution does not pose a risk to the
per day (approximately 3–4 teaspoons) provides a noteworthy health of adults. In general, the contribution of the macro
Cu contribution of 1.34% of its recommended daily intake set and trace elements analyzed is low and is less than 3% in all
at 1.1 mg/day by the Spanish Federation of Nutrition, Food cases. However, a higher consumption of the analyzed honeys

Table 5 Estimated daily intake values (mg/day) and contribution percentages (%) for the analyzed Canary honeys

Metal Parameter Value Reference EDI (μg/day) Contribution percentages (%)

Al TWI 1 mg/kg bw/week [41] 83.3 0.85

Cd 2.5 μg/kg bw/week [42] 0.05 0.20
Sr TDI 0.13 mg/kg bw/day [43] 16.3 0.18
Ba 200 μg/kg bw/day [44] 6.75 0.05
Ni 2.8 μg/kg bw/day [45] 1.00 0.52
Pb 0.5 μg/kg bw/day [46] 1.00 2.92
B UL 17–20 mg/day [47] 106 0.63
V 1.8 mg/day 8.75 0.49
Ca RDI 900–1000 mg/day [48] 1970 0.22
Cr 35 mg/day (men)–25 mg/day (women) 0.13 –
Cu 1.1 mg/day 14.8 1.34
Fe 9 mg/day (men)–18 mg/day (women) 48.8 0.54 (men)–0.27 (women)
K 3100 mg/day 20,625 0.67
Mg 350 mg/day (men)–300 mg/day (women) 1005 0.29 (men)–0.34 (women)
Mn 2.3 mg/day (men)–1.8 mg/day (women) 22.8 0.99 (men)–1.26 (women)
Mo 45 mg/day 0.50 –
Na 1500 mg/day 3650 0.24
Zn 9.5 mg/day (men)–7 mg/day (women) 47.8 0.50 (men)–0.68 (women)

Body weight (bw) of an adult set at 68.48 kg by the AECOSAN [49]

TWI, tolerable weekly intake; TDI, tolerable daily intake; UL, upper level intake; RDI, recommended daily intake
Toxic Metals and Trace Elements in Artisanal Honeys from the Canary Islands 249

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