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Aluminium content in milk

powders by inductively‐coupled
argon plasma‐optical emission
spectrometry
a a a
B. C. Bloodworth , Chua Teck Hock & Tan Oon Boon
a
Institute of Science and Forensic Medicine , Outram Road,
Singapore
Published online: 10 Jan 2009.

To cite this article: B. C. Bloodworth , Chua Teck Hock & Tan Oon Boon (1991) Aluminium
content in milk powders by inductively‐coupled argon plasma‐optical emission spectrometry,
Food Additives & Contaminants, 8:6, 749-754, DOI: 10.1080/02652039109374033

To link to this article: http://dx.doi.org/10.1080/02652039109374033

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 FOOD ADDITIVES AND CONTAMINANTS, 1991, VOL. 8, NO. 6, 7 4 9 - 7 5 4

Aluminium content in milk powders by inductively-coupled argon

plasma-optical emission spectrometry

B. C. BLOODWORTH, CHUA TECK HOCK and TAN OON BOON

Institute of Science and Forensic Medicine, Outram Road, Singapore

(Received 7 November 1990; revised 12 July 1991; accepted 5 August 1991)

Forty-four brands of milk powders and simulated milk powders were analysed for
aluminium content using Inductively Coupled Plasma Spectroscopy (ICP-OES) technique.
The samples covered the full range of infant food items available in Singapore—full-cream
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milk formula, infant formula, fortified infant formula and milk-free soy protein formula.
ICP-OES technique was employed for the analysis. Most samples analysed were
found to contain less than 1 mg aluminium per kg powder. The highest aluminium content
found was 15.0 mg aluminium per kg powder in a milk-free soy protein formula.
The study found that ICP-OES is a convenient and accurate technique for trace metal
analysis. However, considerable care needs to be exercised in the selection of emission lines
of the metal under analysis to avoid error caused by emission from other metal present
in the sample.

Keywords: aluminium, milk powder, ICP-OES

Introduction
The past few years have seen an upsurge in aluminium and health. This is
because of the possible link between aluminium and Alzheimer's disease (Candy et
al. 1986). The idea that aluminium might be toxic did not become widely current
until 1976 when dialysis dementia was recognized as a new illness among dialysis
patients. Some workers in USA showed that dialysis patients had accumulation of
aluminium in their brains (Alfrey et al. 1976). Similar patients suffering from
Alzheimer's disease have elevated concentration of aluminium in some neurones
(Crapper etal. 1976). Alzheimer's disease and dialysis dementia have some
common behavioural and neurological symptoms and hence it was suspected that
aluminium may be a cause of Alzheimer's disease (Sherlock 1988).
Because of the possible health risk arising from the human exposure to
aluminium, there is a need for information about sources of exposure of man to
aluminium. Aluminium is the third most abundant element in the lithosphere and
its presence is ubiquitous. Iiuman exposure to aluminium can come from a variety
of sources such as w?ter, toothpaste, antacid, food, aluminium wares and infant
formulae. It has been estimated that in Britain between 5 and 10 mg are ingested
each day (MAFF 1985). Studies have also shown that bottle-fed infants may be
exposed to a much greater intake of aluminium than breast-fed infants (Freundlich
et al. 1985). This could be of concern since infants will tend to a have a higher
permeability of the blood-brain barrier to aluminium, a higher uptake of
aluminium via the still developing gastrointestinal tract and poorer excretion of
aluminium through the immature kidney (Findlow et al. 1987).
0265-203X/91 $3.00 © 1991 Taylor & Francis Ltd.
 750 B. C. Bloodworth, et. al.

The presence of aluminium in infant formulae has therefore attracted interest

in recent years. Levels of between 0-02 to 0*57 mg/kg have been reported for cows'
milk-based formulae and 0-42 to 2*35 mg/kg for soya-based formulae (Hewitt et
al. 1987, Koo et al., 1988).
This paper focuses on the use of Inductively-Coupled Argon Plasma-Optical
Emission Spectrometer (ICP-OES) as a reliable and convenient method for the
quantitation of aluminium in milk powder products. Altogether 44 brands of
various varieties of milk powder products available in Singapore were analysed, of
which 29 were infant formulae.

Materials and methods

Apparatus
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All glassware and silica dishes were washed with detergent (phosphate-free)
and followed by overnight soaking in nitric acid (20% v/v). These were then rinsed
thoroughly with deionized (Al-free) water and subsequently rinsed with acetone
(Merck AR Grade) and dried.

Inductively-Coupled Argon Plasma-Optical Emission Spectrometer (ICP-OES)

The ICP-OES used for the study was the Perkin Elmer Model Plasma 40
sequential multi-element analyser (40 MHz).

Reagents
(Only AR grade chemicals were used throughout the study.)
(a) Magnesium nitrate solution (29% w/v)—50 g of MgNO3.6H2O (Merck AR
Grade) were dissolved in 50 ml of deionized (Al-free) water.
(b) Dilute nitric acid solution (7% w/v)—100 ml concentrated HNO3 (BDH
Aristar—69-0-70-5% w/v) was diluted to 1 1 using deionized (Al-free) water.
(c) Aluminium standard solution—standard solutions were made up by
diluting BDH aluminium nitrate standard solution (1 -00 mg Al per ml) for atomic
absorption spectroscopy with nitric acid (7%) accordingly with deionized (Al-free)
water.

Sample acquisition
The samples of milk powders and infant formulae were purchased at retail
outlets in Singapore during 1989. All samples tested were of different commercial
brands.

Sample preparation
About 25 g of sample was weighed out accurately and this was mixed with
magnesium nitrate (3 ml; 29% w/v) and water (20 ml). The slurry was dried over
a water bath. This was then charred carefully over a Bunsen flame and subsequently
placed in the muffle furnace at 500°C till it turned to greyish ash (4-5 h). The ash
was digested in nitric acid (10 ml; 7% w/v). The solution was transferred to a 25 ml
graduated flask and the volume was brought up to 25 ml with nitric acid (7% w/v).
Samples were prepared in duplicate. Reagent blanks were included in each batch of
sample preparation to check for possible contamination from extraneous sources.
Standards were included in each batch to act as control. Each batch contained
 Aluminium content in milk powders 751

two reagent blanks, two standards of different aluminium concentration and five
samples.

ICP-OES analysis
The final sample solution was analysed directly using Perkin Elmer Model
Plasma 40 set as follows: emission wavelength (for aluminium) at 308-215 nm;
wavelength window at 0-1 nm; aspirate flow rate at 1 ml/min; nebulizer argon flow
rate at 0*8 1/min. Samples were analysed in duplicate. Two ICP-OES runs were
made on each replicate. Samples were quantified by reference to a calibration graph
obtained for standard solutions of aluminium (0-2-10 mg/1) in nitric acid.
Background corrections were applied to all sample results. Two reagent blanks and
two standards were included in each batch of five samples (in duplicate).
Although standard solutions of aluminium content as low as 50 ftg/1 could be
measured accurately using ICP-OES, in practice, the amount of aluminium in milk
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powder that could be quantified accurately was higher. This was reflected from the
recovery study of spiked samples.The samples used for this study were cows' milk-
based powder samples which were found to contain no detectable amount of
aluminium. These were spiked with different amounts of aluminium to provide a
series of milk powder samples containing 0-2-20 mg of aluminium per kg milk
powder. For each spiked aluminium concentration five samples were analysed. The
results of the analysis are tabulated in table 1. Recoveries from samples containing
aluminium less than 0-5mg/kg were below 90% with precision of recoveries
±9-11%. This level of recovery and precision was considered inadequate for
accurate quantification purpose. Thus, it is recommended that for analysis of milk
powder containing aluminium less than 0-5 mg/kg, an alternative technique such as
atomic absorption spectrometry should be used.

Results
The levels of aluminium found in the 44 brands of milk powder and infant
formula are shown in tables 2 and 3. The amount of aluminium found on a dry
mass basis, and the calculated concentrations of aluminium in the liquid feeds are
both presented. The amounts of aluminium in the liquid feeds were calculated
based on the manufacturers' feed preparation instructions. The calculated
aluminium values did not include the contribution from aluminium already present
in the water.
In the case of cows' milk-based infant formulae and cows' milk-based milk
powders, the ranges of aluminium levels found were 0—2-4 mg/kg with a mean*
value of 0-74 mg/kg, and 0-5-5 mg/kg with a mean* value of 1-1 mg/kg
respectively. The calculated amounts of aluminium in the prepared feed were found
to range from 0 to 0-37 mg/1 for cows' milk-based infant formulae from 0 to
0-70 mg/1 for cows' milk-based milk powders. With the soybean-based infant
formulae, a much higher aluminium level was found ranging from 2-8 to
15-0 mg/kg with a mean value of 6-1 mg/kg. The corresponding calculated amount
of aluminium levels in the liquid feeds ranged from 0-47 to 2-50 mg/1.
The levels of aluminium found in the infant formulae and milk powders are
similar to those reported by Baxter (Baxter et al. 1990), and are generally higher

*The arithmetic mean of the aluminium contents of the relevant samples analysed.
 752 B. C. Bloodworth, et. al.

Table 1. Recovery of aluminium from milk powder.

Al added Test portion Mean rec.

(ng per 10 g) n (g) ±SD(%)

2 5 25 76-2 ± 9-0
3 5 25 77-1 ± 9-1
4 5 25 86-0± 11-0
5 5 25 97-0 ± 4-0
10 5 25 98-1 ± 3-2
20 5 25 98-1 ± 4-1

Table 2. Aluminium in infant formulae.

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Sample Concentration in Concentration3 in

powder prepared feed (calc.)
(mg/kg) (mg/1)

(I) Cows' milk-based infant formulae

Sample 1 2-4 0-37
Sample 2 0-6 0-09
Sample 3 0-7 0-11
Sample 4 0-6 0-09
Sample 5 0-8 0-12
Sample 6 0 0
Sample 7 0-9 0-14
Sample 8 0-7 0-11
Sample 9 2-1 0-33
Sample 10 1-1 0-17
Sample 11 0-4 0-06
Sample 12 0-5 0-07
Sample 13 0-6 0-09
Sample 14 0-7 0-11
Sample 15 0-7 0-11
Sample 16 0-7 0-11
Sample 17 0-5 0-07
Sample 18 0-7 0-11
Sample 19 1-2 0-18
Sample 20 0-5 0-07
Sample 21 0 0
Sample 22 0-3 0-04
Sample 23 0-7 0-11
Sample 24 0-6 0-09
Sample 25 0-6 0-09
(II) Soybean-based infant formulae
Sample 1 2-8 0-47
Sample 2 3-5 0-59
Sample 3 15-0 2-50
Sample 4 3-5 0-59
a
The prepared feeds were made up according to the
manufacturers' instruction; the corresponding aluminium content
was calculated based on the amount of powder used. The amount
of aluminium contributed from water was excluded in the
calculation.
 Aluminium content in milk powders 753

Table 3. Aluminium in cows' milk-based milk powders.

Sample Concentration in Concentration' in

powder prepared feed (calc.)
(mg/kg) (mg/1)

Sample 1 0-9 0-11

Sample 2 0-5 0-06
Sample 3 0 0
Sample 4 5-5 0-70
Sample 5 1-5 0-20
Sample 6 0-6 0-08
Sample 7 0-7 0-09
Sample 8 0-8 0-10
Sample 9 0-7 0-09
Sample 10 0-5 0-06
Sample 11 0-9 0-11
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Sample 12 0-6 0-08

Sample 13 0-7 0'09
Sample 14 1-7 0-22
Sample 15 0-9 0-11

a
The prepared feeds were made up according to the
manufacturers' instruction; the corresponding aluminium content
was calculated based on the amount of powder used. The amount
of aluminium contributed from water was excluded in the
calculation.

but nevertheless in the same order as those reported by Hewitt (1987), and Koo et
al. (1988).

Discussion
In recent years, there has been a growing use of inductively-coupled plasma
technique for the analysis of trace elements in food samples. Amongst the
advantages are large linear dynamic range and relative freedom from matrix effects.
However, due to the intrinsic complexity of food items, the often unavoidable
presence of other elements apart from the element of interest may give rise to
interfering emission lines. Great care must be exercised to avoid misinterpretation
of the experimental results. In our experiment, the usual emission lines for
aluminium analysis 396-152 nm and 309*271 nm could not be used. The former
emission line was discarded due to the natural presence of a large amount of
calcium in the milk powders that would give rise to emission in this region masking
any aluminium lines present. The latter line was found to be unsuitable because of
the presence of an unknown large peak at 309-306 nm which interfered with the
detection and quantitation of aluminium. Aluminium up to 5 mg/kg in fortified
milk powders was detectable but not quantifiable using the emission line
309*271 nm because of the interference. The emission line at 309 '306 nm was later
traced to be caused by the matrix modifier magnesium nitrate. Emission at
308-215nm was used throughout this experiment.
The levels of aluminium found in cows' milk reported in the literature are
generally low—0-03 mg/1 (Koo et al. 1988), and 0-09 mg/1 (Weintraub et al. 1986).
Our calculated results for the prepared feeds from both cows' milk-based infant
formulae, 0-0-37 mg/1 with a mean value of 0-11 mg/1 (table 2), and cows' milk
 754 B. C. Bloodworth, et. al.

powders, 0-0-70 mg/1 with a mean value of 0-14 mg/1 (table 3) are of the same
order of concentration as those of cows' milk reflecting that aluminium
contamination during the manufacturing of such products is generally insignificant.
The range of aluminium levels 0-47-2-50 mg/1 (table 2) found in soybean-
based prepared feed is significantly higher than those of cows' milk-based products.
The results are consistent with the findings of Baxter et al. (1990) who reported a
range of 0-64-1-34 mg/1. The presence of higher aluminium levels in the soybean-
based products could be partly due to aluminium present naturally in the plant
materials.

Conclusions
The aluminium levels of a wide range of cows' milk-based products were found
to be low and similar to those present in cows' milk, reflecting that aluminium
contamination during the manufacturing process of such products is not significant.
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The higher aluminium levels found in the soybean-based products could be partly
due to aluminium naturally present in the plant materials.
The high percentage recovery and the low percent standard deviation obtained
with samples containing >0-5 mg aluminium per kg of milk powder showed that
the above analytical method using ICP-OES is suitable for quantitative analysis of
aluminium contamination in milk powder products at the mg per kg level.

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