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Public Health

journal homepage: www.elsevier.com/puhe

Original Research

Evaluation of Cd, Cr, Cu, Ni, and Pb in selected


cosmetic products from Jordanian, Sudanese, and
Syrian markets

A.M. Massadeh*, M.Y. El-khateeb, S.M. Ibrahim


Jordan University of Science and Technology, Jordan

article info abstract

Article history: Objectives: There is no sufficient data that evaluate heavy metal content in cosmetic
Received 3 January 2017 products in Jordan as well as Sudan and Syria. This study aims to assess metal levels which
Received in revised form include Cadmium (Cd), Chromium (Cr), Copper (Cu), Nickel (Ni), and Lead (Pb) in cosmetic
3 March 2017 products. These elements have draft limits because they are identified as potential im-
Accepted 29 March 2017 purities and are known to be toxic. This study aims to provide information to the popu-
lation that may be beneficial to public health.
Study design: Samples were collected from different brands obtained from markets in Jor-
Keywords: dan, Sudan, and Syria. Some of the selected cosmetic products were eyeliner, eye pencil,
Analysis mascara, lipstick, powder, face cream, body cream, sun block, Vaseline, and the traditional
Cosmetics eye cosmetic (kohl). The heavy metal content in these samples were determined by atomic
Heavy metals absorption spectrometry (AAS). Based on analysis of variance analysis, a significant dif-
AAS ference in heavy metal levels was found for samples obtained from Jordanian and Suda-
nese markets.
Methods: The acid digestion method used in this study was based on procedures recom-
mended by Nnorom et al. with some modifications as follows. (i) A weight of 2.0 g of
cosmetic sample was dissolved in a mixture of 6 mL of high quality concentrated 69% nitric
acid (HNO3; Merck, Darmstadt, Germany) and 4 mL of concentrated 37% hydrochloric acid
(Scharlau, Spain) in a porcelain crucible and heated on a hotplate to near dryness. (ii) An
aliquot of 15 mL HNO3 (1.00 M) was added to the digested sample and filtered through a
Whatman No. 40 filter paper. (iii) The digested sample was transferred quantitatively into a
25 mL volumetric flask and then diluted with deionized water. (iv) Each digested sample
was evaporated at 70  C to about 1 mL and transferred into a polyethylene flask and diluted
with 25 mL deionized water. (v) Blank was treated in the same procedure.
Results: In Jordan the concentration ranges of heavy metals in the collected samples were:
Cd (0.03e0.10 mg/g), Cr (0.0e1.00 mg/g), Cu (0.60e7.40 mg/g), Ni (0.50e3.60 mg/g), and Pb (0.30e
15.4 mg/g). Whereas, in Sudanese market the concentration ranges were: Cd (0.01e0.15 mg/g),
Cr (0.00e27.9 mg/g), Cu (0.60e10.10 mg/g), Ni (0.00e5.70 mg/g), and Pb (0.02e3.80 mg/g). Also, the
concentration ranges of heavy metals in Syrian market were: Cd (0.04e0.056 mg/g), Cr (0.24e
0.83 mg/g), Cu (0.61e1.27 mg/g), Ni (0.73e1.41 mg/g), and Pb (4.85e27.70 mg/g). Results re-
vealed that kohl samples have the highest concentration of most of the studied metals,
particularly Pb.

* Corresponding author.
E-mail address: massadeh@just.edu.jo (A.M. Massadeh).
http://dx.doi.org/10.1016/j.puhe.2017.03.015
0033-3506/© 2017 The Royal Society for Public Health. Published by Elsevier Ltd. All rights reserved.
p u b l i c h e a l t h 1 4 9 ( 2 0 1 7 ) 1 3 0 e1 3 7 131

Conclusions: Based on the results obtained, it is likely to conclude the following: (i) It is not
possible to completely eliminate the presence of heavy metals from cosmetic products
after manufacturing. However, the quality of the products can be improved by careful
selection of raw materials, taking in consideration heavy metal levels. (ii) Heavy metal
concentration in lipstick differs with different manufacturers' colors and shade. Statisti-
cally significant associations between Pb level and the cosmetic type were found. (iii) Heavy
metals levels including Cd, Cr, Cu, Ni, and Pb may impose risk in daily use and repeated
application as well as in ingestion through the mouth even at concentration below the
allowed limits. (iv) It is the manufacturers' responsibility to ensure that the finished
cosmetic product contains the lowest levels possible of heavy metals. So it does not exceed
the limits set by health authorities.
© 2017 The Royal Society for Public Health. Published by Elsevier Ltd. All rights reserved.

after exposure to cosmetics containing heavy metal


Introduction impurities.14,15
Dermal exposure is expected to be the most significant
Cosmetics are substances used as personal care products to route because most of the cosmetic products are directly
enhance or protect the appearance or mask the odor of the applied to the skin.
human body. The demand for cosmetic products has Cosmetics and their ingredients have to be safe under the
increased recently, resulting in massive production by the conditions of normal use and must be thoroughly evaluated
cosmetic industry. Different products are marketed under the prior to marketing. Safety assessment should be performed on
name of cosmetics, such as creams, beauty soaps, talcum and finished products taking into consideration the toxicological
facial powder, lotions, shampoos, hair products such as hair profile of the ingredients, their chemical structure, and their
colors, baby products, bath oils, personal hygiene products, potential to produce local and systemic effects. In humans the
perfumes, lipsticks, skin care products, makeup products, concentration of heavy metals in cosmetic raw materials and
shaving creams, body lotions, fingernail polish and polish finished products has been strictly monitored and controlled
removal.1e5 In addition, the use of herbal medicinal prepara- by health authorities such as United States Food and Drug
tions is common in most developing countries due to poverty Administration (US FDA).16 Guidelines on safety assessment
and disillusionment with conventional medical care.6,7 of cosmetic ingredients have been published by the EU Sci-
On the other hand, there has been growing consumer entific Committee on Consumer Safety.17,18 The Notes of
concern that cosmetics may contain harmful levels of toxic Guidance include the toxicological test procedures reported in
substances such as heavy metals. Heavy metals are naturally Commission Regulation (EC) No. 440/2008. They enclose the
occurring in the environment and can make their way in trace basic toxicity testing procedures needed to evaluate different
quantities into raw materials.8,9 human health related toxicological endpoints and are inter-
The focus is on heavy metals with known significant nationally accepted as being the result of long term scientific
toxicological properties such as Lead (Pb), Arsenic (As), Cad- agreement. The Commission Regulation (EC) No. 440/2008
mium (Cd) and Mercury (Hg). Also, the essential elements includes Reduction and Refinement and Replacement
such as Copper (Cu) and Zinc (Zn) at high levels may cause methods. Given the fact that Regulation (EC) No. 1223/2009
adverse effects to human health. imposes the use of validated replacement methods not only
Heavy metals that build up in the body over time are known for finished cosmetic products but also for their ingredients,
to cause various health problems, such as: neurological and much attention is given to the use of validated replacement
developmental disorders, reproductive disorders, cardiovas- methods in the safety evaluation of cosmetic substances and
cular diseases, skeletal, blood, immune system, gastrointes- finished cosmetic products.
tinal disorders and renal problems, headaches, lung, skin and Since ancient times, kohl has been used as eye cosmetic
soft tissue disorders, and brittle hair and hair loss as well as especially in the Middle East, Far East, and Northern Africa.19
cancer. Some are identified as dysfunction hormone dis- Studies showed that kohl contains toxic metals, such as Pb
ruptors while others are respiratory toxins. Heavy metals have and have revealed that the Pb levels in the blood were
been implicated in cosmetics commonly used by women.10,11 significantly higher in individuals who used kohl compared to
Cd found in body and hair creams are absorbed into the those who did not.20,21
body through dermal contact then stored in the kidneys and A study in Nigeria reported that facial makeup creams have
liver, although it can be found in almost all adult tissues.9,12 Chromium (Cr), Fe, and Zn at much higher levels compared to
The essential metals such as Cu, Zn, Nickel (Ni), and Iron non-essential metals such as Pb, Cd, and Ni. These creams are
(Fe) can produce toxic effects when the metals intake is in relatively safe to use. Comparative amounts of Pb were found
high concentrations.13 in eyeliners and eye pencils.22 Similar studies of traditional
Oral exposure can occur with cosmetics used in and eye makeup products in Nigeria have reported very high levels
around the mouth as well as through hand-to-mouth contact of trace metals in locally produced eye makeup and eye
132 p u b l i c h e a l t h 1 4 9 ( 2 0 1 7 ) 1 3 0 e1 3 7

shadow samples.23e25 In Jordan, as well as in Sudan and Syria, i) A weight of 2.0 g of cosmetic sample was dissolved in a
such studies are lacking. mixture of 6 mL HNO3 and 4 mL HCl in a porcelain
crucible and heated on a hotplate to near dryness.
ii) An aliquot of 15 mL HNO3 (1.00 M) was added to the
Methods digested sample and filtered through a Whatman No. 40
filter paper.
Chemicals and reagents iii) The digested sample was transferred quantitatively into a
25 mL volumetric flask and diluted with deionized water.
All chemicals used in this study were analytical grade. Nitric iv) Each digested sample was evaporated at 70 C to about
acid (HNO3; 69% Merck, Darmstadt, Germany) and concen- 1 mL and transferred into a polyethylene flask and
trated hydrochloric acid (37% HCl; Scharlau, Spain) were used diluted with 25 mL deionized water.
as stock solutions. Deionized water was used in all v) Blank was treated in the same procedure.
experiments.
Calibration curves (concentration [mg/L] vs absorbance)
Collection of cosmetic samples were constructed by diluting standard solutions of Cd, Cr, Cu,
Ni, Pb, and Zn (1000 mg/L, Merck, Germany) to different con-
Different types of cosmetic brands and samples were collected centrations and recording their absorbance values by FAAS.
from Jordanian, Sudanese, and Syrian markets. The main Linear calibration curves were obtained for Cd 0.5e5 ppb
source of these samples was purchased from different cosmetic (r2 ¼ 0.9998), Cr: (r2 ¼ 0.9982), Cu: (r2 ¼ 0.9991), Ni: (r2 ¼ 1.000),
stores in these countries. These samples include: eyeliner, eye Pb: (r2 ¼ 0.9996), and Zn: (r2 ¼ 0.9996).
pencil, mascara, lipstick, powder, face cream, body cream, sun
block, Vaseline, and the traditional eye cosmetic (kohl). Validation and quality assurance of results

Instrumentation During the analysis of samples, quality control (QC) was used to
evaluate the accuracy of the method used in this study. In this
Precise determination of heavy metal levels in cosmetic QC method, different known standard concentrations of each
products is quite important because there is a narrow margin tested element were analyzed after analysis of 10 cosmetic
of safety between adequate amount and over consumption. samples. Results indicated that there was good agreement be-
Thus, analysis of Cd, Cr, Cu, Ni, and Pb was carried out by tween these standard concentrations for each element and its
using flame atomic absorption spectrometry (FAAS) and measured value. For example, the standard concentration used
graphite FAAS model (SOLAAR M5, UK) with a computer sys- for Pb was 5 mg/L, and the measured value was 4.93 ± 0.05 mg/L.
tem. The analysis was carried out at the proper wavelength for
each metal (Cd: 228.8 nm; Cr: 357.9 nm; Cu: 324.8 nm; Ni:
232.0 nm; Pb: 283.3 nm). Results

Sample preparation using acid digestion procedure In this study, the concentration of selected heavy metals (Cd,
Cr, Cu, Ni, Pb) in cosmetic samples obtained from Jordanian,
The acid digestion method used in this study was based on Sudanese, and Syrian markets were determined by atomic
procedures recommended by Nnorom et al.22 and Demirel absorption spectroscopy. The results obtained are shown in
et al.8 with some modifications as follows: Figs. 1e6. Fig. 1, shows metal concentrations (mg/g) in different

18
17
16
15
14
13
12
11
Metal Conc. ( g/g)

10
9 Cd Cr Cu Ni Pb
8
7
6
5
4
3
2
1
0
Eye line Mascara Lipstick Eye pencil Powder Face Cream Body Cream

Cosmetic Brands

Fig. 1 e Heavy metal concentrations (mg/g) in different brands from Jordanian market. Cd ¼ Cadmium; Cr ¼ Chromium; Cu ¼
Copper; Ni ¼ Nickel; Pb ¼ Lead.
p u b l i c h e a l t h 1 4 9 ( 2 0 1 7 ) 1 3 0 e1 3 7 133

35

30

25

Metal Conc. (μg/g)


20
Cd Cr Cu Ni Pb

15

10

0
Eye line Mascara Lipstick Eye pencil Powder Face Cream Body Cream

Cosmetic Brands

Fig. 2 e Heavy metal concentrations (mg/g) in different brands from Sudanese market. Cd ¼ Cadmium; Cr ¼ Chromium; Cu ¼
Copper; Ni ¼ Nickel; Pb ¼ Lead.

35
cream, and sun block, and the lowest concentrations of Cd
30 were found in all examined samples.
For kohl samples collected from Jordanian, Sudanese, and
Cd
25 Syrian markets (Fig. 4), the results for Cd levels were as fol-
Cr
lows: Sudan (8.43 mg/g) > Syria (0.89 mg/g) > Jordan (0.68 mg/g);
Metal Conc. (μg/g)

Cu
20 Ni for Cr: Sudan (0.96 mg/g) > Jordan (0.23 mg/g) > Syria (0.19 mg/g);
Pb for Ni: Sudan (1.14 mg/g) > Jordan (0.89 mg/g) > Syria (0.41 mg/g).
15 Figs. 4 and 5 showed the kohl content of Cu and Pb, respec-
tively. The highest concentrations of Cu (Fig. 5) were found in
10 kohl samples collected from Sudanese market (128.9 mg/g).
The order of Pb levels in kohl samples (Fig. 6) was as follows:
5 Syria (391 mg/g) > Sudan (352.3 mg/g) > Jordan (328.5 mg/g).
These results are consistent with the results found for sam-
0 ples in United Arab Emirates market. Depending on the
Body Cream Mascara Sun Block Vaseline samples' origin, samples obtained from Sudan have higher
Cosmetic Brands metal concentration than those obtained from Jordan or Syria.

Fig. 3 e Heavy metal concentrations (mg/g) in different Statistical analysis


brands from Syrian market. Cd ¼ Cadmium; Cr ¼
Chromium; Cu ¼ Copper; Ni ¼ Nickel; Pb ¼ Lead. Analysis of variance was used to analyze the results obtained.
Results of statistical analysis for Cd, Cr, Cu, Ni, and Pb for all
cosmetic samples collected from Jordanian and Sudanese
markets indicated that there was a significant difference be-
brands from the Jordanian market. The highest concentration tween metal concentrations in Sudan and Jordan. Fcal (F-
was found for Pb in face cream, powder, and body cream calculated) values for Cd (1.56), Cr (2.41), Cu (1.11), Ni (0.623),
samples, respectively. Lipstick and eyeliner samples were and Pb (1.26) were <Fcrit (F-critical) (4.17). P-values for Cd
found to contain the highest level of Cu; whereas, the lowest (0.221), Cr (0.132), Cu (0.301), Ni (0.437), and Pb (0.271) > P (0.05).
concentrations of Cd and Cr were found in all examined Correlations of concentrations of heavy metals in cosmetic
cosmetic samples. Fig. 2 shows metal concentrations (mg/g) in samples collected from Sudanese markets showed that there
different brands from Sudanese market. For Cr, the highest was a negative correlation between Cr vs Cd and Cu; Cu vs Cr;
levels were found in mascara, lipstick, and powder samples. Ni vs Cd; Pb vs Cr; and Ni vs Pb. Whereas a positive correlation
Moreover, lipstick and eye pencil samples contained the was found between Cr vs Ni; Cr vs Cd and Pb; Ni vs Cr; Pb vs Cd
highest levels of Cu, whereas mascara and body cream con- and Cu.
tained high Ni levels. Fig. 3 shows the element levels in For cosmetic samples collected from Jordanian market, the
different brands of cosmetics collected from Syrian market. results indicated that there were negative correlations be-
The highest concentrations of Pb were found in Vaseline, body tween Cd vs Cr and Ni; Cr vs Cd, Cu, and Pb; Cu vs Cr and Ni; Ni
134 p u b l i c h e a l t h 1 4 9 ( 2 0 1 7 ) 1 3 0 e1 3 7

10

7
Metal Conc. (μg/kg) Kohl (J)
6
Kohl (S)
5 Kohl (SY)

0
Cd Cr Ni

Element

Fig. 4 e Concentrations of Cadmium (Cd), Chromium (Cr) and Nickel (Ni) (mg/g) in kohl samples from Jordanian (J), Sudanese
(S), and Syrian (SY) markets.

160

140

120

100
Copper (μg/g)

80

60

40

20

0
Kohl (J) Kohl (S) Kohl (SY)

Cosmetic Brands

Fig. 5 e Concentrations of Copper (Cu) (mg/g) in kohl samples from Jordanian (J), Sudanese (S), and Syrian (SY) markets.

vs Cd; Cu and Pb; Pb vs Cr and Ni. Whereas a positive corre-


450
lations was found between Cd vs Cu and Pb; Cr vs Ni; Cr vs Cd
400
Lead Concentration (μg/g)

and Pb; Ni vs Cr; Pb vs Cd; Cu and Pb.


350 The levels of Cd, Cr, Cu, and Ni were generally low in all
300 samples and there were no significant differences between
250
their levels in Jordan and Sudan, whereas Pb had the highest
concentration in all samples with significant difference.
200

150

100
Discussion
50
Cosmetic products contain organic and inorganic components;
0 for example, lipstick may contain pigments, oils, waxes, and
Kohl (J) Kohl (S) Kohl (SY)
Pb; lip pot may contain castor oil, organic coconut oil, sun-
Kohl Samples bleached beeswax, castor wax, and organic essential oil of
sweet orange, mica, iron oxides, and titanium oxide; eye
Fig. 6 e Concentrations of Lead (Pb) (mg/g) in kohl samples
shadow may contain silica, mica, iron oxide; mascara may
from Jordanian (J), Sudanese (S), and Syrian (SY) markets.
p u b l i c h e a l t h 1 4 9 ( 2 0 1 7 ) 1 3 0 e1 3 7 135

contain mineral origin wax (ozokerite, paraffin), pigments (iron Chromium (Cr),Copper (Cu), Manganese (Mn), Nickel (Ni) and
oxide, ultramarine), and filmifying polymers; kohl may contain Titanium (Ti).33 In addition, the levels of Pb, Cd, As, Sb, Ni, Cr,
lead sulphide (PbS), Aluminum (Al), Antimony (Sb), Carbon (C), and Hg in 14 brands of lipsticks were assessed in Saudi mar-
iron (Fe) and zinc (Zn) compounds, camphor, and menthol; kets.34 In Nigeria, the levels of Cd, Cr, Cu, and Zn were deter-
foundation may contain sericite, micronized zinc, mica, iron mined in personal care products, and the highest values of Cd
oxide, silica, and titanium dioxide. (0.553 ppm) and Cu (0.783) were observed in hair cream.12
The Campaign for Safe Cosmetics in USA raised another Our findings revealed that the tested heavy metals in
concern about the presence of Pb in lipsticks, and found that cosmetic samples in the Jordanian market were less than the
more than one half of the tested 33 brand names of red lipstick permissible limit for Cd (0.03e0.10 mg/g), Cr (0.0e1.00 mg/g), Cu
(61%) contained detectable Pb in the range of 0.03e0.65 ppm.26 (0.60e7.4 mg/g), Ni (0.5e3.6 mg/g), and Pb (0.3e15.4 mg/g). These
A study of the Pb content in similar samples in Malaysia values are safe according to the Canadian guideline which
indicated a range of 10.23e23.05 mg/g.27 A study of Asian states that heavy metal impurity concentrations in cosmetic
remedies evaluated the levels of As, Pb, and Hg reported products are seen to be technically avoidable when they
values ranging from toxic to values exceeding public health exceed the following limits: Pb, 10 ppm; As, 3 ppm; Cd, 3 ppm;
guidelines.28 Hg, 1 ppm; Sb, 5 ppm.35 The United States Food and Drug
For example, Cd is used as color pigment in many cos- Administration (US FDA) limit for arsenic in certain colorants
metics industries.29 It is present in many cosmetic products, is <3 ppm.36 Our results were inconsistence with the German
but mostly present in lipsticks and facial powders. The car- Federal Government that conducted tests to determine back-
diovascular system is affected even at the low level of Cd. ground levels of heavy metal content in cosmetic products. It
Diabetes and hypertension are also associated with its was determined that heavy metal levels in cosmetic products
exposure.30 above the values listed below are considered technically
Some cosmetic products are applied via spray, presenting the avoidable; Pb: 20 ppm; As: 5 ppm; Cd: 5 ppm; Hg: 1 ppm; Sb:
possibility of inhalation. Also sunscreens, due to their extensive 10 ppm.37 On the other hand, Pb levels in most of the cosmetic
skin contact, combined with direct exposure to UV radiation for samples from the Syrian market exceeded the limit set by the
prolonged periods, require a distinct type of safety evaluation.2 Germany Federal regulations.
Lipsticks also have a higher risk of direct oral ingestion, aggra- The significant difference between the level of heavy
vating the negative effects of their ingredients. metals in different types of cosmetics may be due to its dis-
In general, there are no definite limit values for heavy tribution and mobility in matrix. In other words the distribu-
metal content in cosmetic products, therefore it is difficult to tion and mobility for each element may differ from one
ascertain if the values obtained in this study are deemed low cosmetic sample to another. This variation may be due to the
or high. The results obtained from this study revealed that difference in the component of the matrix, coloring and other
kohl samples obtained from the three markets have the additives in the cosmetic preparation.
highest concentrations among all the investigated samples
tested. Kohl obtained from Sudan has higher concentration Conclusion
than sample obtained from Jordan or Syria. Our findings
revealed that Pb is the major element found in kohl samples, A substance added to a cosmetic as a component of a cosmetic
and these results are in good agreement with a study of kohl product and has no technical or functional effect in the finished
from United Arab Emirates market which showed that sam- cosmetic. For example, a preservative of a raw material when
ples manufactured in India contained PbS and lead carbonate added to the cosmetic as an ingredient, its concentration is
(PbCO3),31 while those manufactured in Pakistan have no Pb reduced to a level at which it is no longer effective. Based on the
content contained and are safer to use.31 Moreover, eye cos- results obtained, it is likely to conclude the following:
metics could be another source of exposure to heavy metals.
For example, various colors are used in manufacturing eye i) It is not possible to completely eliminate the presence
shadows and the US FDA has allowed the use of some natural of heavy metals from cosmetic products after
colors or inorganic pigments such as iron oxide, carmine, ti- manufacturing. However, the quality of the products
tanium oxide, and aluminum powder.16 can be improved by careful selection of raw materials,
In this study, the results showed that Cr has a higher taking in consideration heavy metal levels.
concentration compared to Ni and Cd in mascara, lipstick, and ii) Heavy metal concentration in lipstick differs with
eyeliner obtained from Sudan whereas samples obtained from different manufacturers' colors and shade. Statistically
Jordan revealed that the level of Cr was higher than that of significant associations between Pb level and the
non-essential metals such as Pb and Cd. The study also cosmetic type were found.
showed that Pb has high concentrations in face cream, iii) Heavy metals levels including Cd, Cr, Cu, Ni, and Pb may
lipstick, and powder samples in Jordan. impose risk in daily use and repeated application as well
Again these findings are in good agreement with other as in ingestion through the mouth even at a concen-
studies which reported that heavy metals were found in in- tration below the allowed limits.
gredients that naturally contain heavy metals or are iv) It is the manufacturers' responsibility to ensure that the
contaminated with them during production or from con- finished cosmetic product contains the lowest levels
tainers.32 Other researchers reported that lipsticks contain not possible of heavy metals. So it does not exceed the
only Pb, but also Aluminum (Al), Cadmium (Cd), Cobalt (Co), limits set by health authorities.
136 p u b l i c h e a l t h 1 4 9 ( 2 0 1 7 ) 1 3 0 e1 3 7

Recommendations Competing interests

Extensive use of such products should be avoided until it is None declared.


adequately addressed. Therefore, efforts must be made to
inform the users and the general public especially pregnant
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