Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se, and Zn contents in baby foods from the EU market: Comparison of assessed infant intakes with the present safety limits for minerals and trace elements

Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se, and Zn contents in baby foods from the EU market: Comparison of assessed infant intakes with the present safety limits for minerals and trace elements

Journal of Food Composition and Analysis 27 (2012) 120–127 Contents lists available at SciVerse ScienceDirect Journal of Food Composition and Analys...

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Journal of Food Composition and Analysis 27 (2012) 120–127

Contents lists available at SciVerse ScienceDirect

Journal of Food Composition and Analysis journal homepage: www.elsevier.com/locate/jfca

Original Research Article

Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se, and Zn contents in baby foods from the EU market: Comparison of assessed infant intakes with the present safety limits for minerals and trace elements Marchela Pandelova a,*, Walkiria Levy Lopez a, Bernhard Michalke a, Karl-Werner Schramm a,b a b

Helmholtz Zentrum Mu¨nchen, German Research Center for Environmental Health, Institute of Ecological Chemistry, Ingolsta¨dter Landstrasse 1, 85764 Neuherberg, Germany TUM, Wissenschaftszentrum Weihenstephan fu¨r Erna¨hrung und Landnutzung, Department fu¨r Biowissenschaften, Weihenstephaner Steig 23, 85350 Freising, Germany

A R T I C L E I N F O

A B S T R A C T

Article history: Received 17 October 2011 Received in revised form 9 March 2012 Accepted 25 April 2012

In this study calcium (Ca), cadmium (Cd), copper (Cu), iron (Fe), mercury (Hg), manganese (Mn), nickel (Ni), lead (Pb), selenium (Se), and zinc (Zn) were determined in most consumed baby foods in Europe including infant formulae and solid foods and beverages (SFB). Additionally, Cd and Zn contents were determined in baby foods from the ‘‘national baskets’’ of four selected countries (Italy, Spain, Slovakia, and Sweden). Overall, highest element levels were found in the soy-based infant formulae. Furthermore, the assessed daily/weekly intakes of the 0–9-month-old non-breast-fed infants were compared with the current safety limits of the 10 elements here analyzed. Assessment to Cd exposure to infants consuming commercial SFB was found to exceed the limit established by the European Food Safety Authority (EFSA) of a tolerable weekly intake (TWI) of 2.5 mg Cd/kg bw. Furthermore, mercury acquisition higher than the Joint FAO/WHO Expert Committee of Food Additives (JECFA) established provisional tolerable weekly intake (PTWI) of 4 mg Hg/kg bw was determined for infants fed specifically with ‘‘follow on’’ milk infant formula. In regard to the estimated infant intakes of the non-essential (Pb and Ni) and the essential (Ca, Cu, Fe, Mn, Se and Zn) elements the values were within the safety limits. ß 2012 Elsevier Inc. All rights reserved.

Keywords: Minerals Micronutrients Trace element Heavy metal contamination in food Recommended dietary allowance Food analysis Infant Infant formula Baby food Exposure Europe Food safety Food composition

1. Introduction During infancy, breast milk and infant formulae are the major source of nutrients for infants (Ikem et al., 2002). Although the World Health Organization (WHO) recommends breastfeeding as the best feeding choice (WHO, 2008), infant formulae are an alternative to breast-milk that often play an important role in the

Abbreviations: ATSDR, Agency for Toxic Substance and Disease Registry; bw, body weight; Ca, calcium; Cd, cadmium; Cu, copper; dw, dry weight; EFSA, European Food Safety Authority; EU, European Union; Fe, iron; fHAf, ‘‘follow-on’’ hypoallergenic-based infant formula; fMf, ‘‘follow-on’’ milk-based infant formula; fSf, ‘‘follow-on’’ soy-based infant formula; fw, fresh weight; HAf, hypoallergenic-based infant formula; HFCS, high fructose corn syrup; Hg, mercury; JECFA, Joint FAO/WHO Expert Committee of Food Additives; Mf, milk-based infant formula; Mn, manganese; Ni, nickel; Pb, lead; PTWI, provisional tolerable weekly intake; RDI, recommended daily intake; RF, radio frequency; SCF, Scientific Committee for Food; Se, selenium; Sf, soy-based infant formula; TDI, tolerable daily intake; TWI, tolerable weekly intake; UL, tolerable upper limit; WHO, World Health Organization; Zn, zinc. * Corresponding author. Tel.: +49 89 3187 2932; fax: +49 89 3187 3371. E-mail address: [email protected] (M. Pandelova). 0889-1575/$ – see front matter ß 2012 Elsevier Inc. All rights reserved. http://dx.doi.org/10.1016/j.jfca.2012.04.011

infant’s diet. According to statistics from 2007, few European women breastfeed their infants exclusively at 6 months of age, and only 33% of infants in the USA are exclusively breastfed up to 3 months of age (Cattaneo, 2004). An increasing number of mothers feed their babies with industrially processed formula milk or solids such as vegetables and meat or fish pure´e, so that in recent years the baby food market and the assortment of products offered have grown significantly. Since the first year of life is a sensitive period in the human development of the nervous, reproductive, digestive, respiratory and immune systems, the composition of baby foods and their consumption pattern are crucial. Despite the benefits of infant formulas as a major source of food for infants, the presence of contaminants, such as heavy metals, may pose health risks to children (Souad et al., 2006; Tripathi et al., 2001). Moreover, infants tend to be exposed to relatively higher levels of food chemicals, since they consume more food than adults relative to their body weight. Thus, a child can absorb as much as 50% of the lead present in food, whereas an adult takes up only 10% (CEC, 2003). There is evidence that vegetables are able to accumulate mercury, lead, cadmium, zinc, and copper in their edible and inedible parts at various concentration levels (Zheng

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et al., 2007). Mercury, and in particular methylmercury, poses a risk to public health; for example, it can affect the development of the infant brain and can cause neurological changes in adults (Jedrychowski et al., 2006). Negative effects on the behavior and intelligence of children are found at lower levels of lead exposure than those commonly associated with lead poisoning (Tripathi et al., 2001). Furthermore, recent studies show that cadmium and zinc can act as endocrine disruptors in fish, either in vivo or through a direct action on steroidogenic cells, as it has been demonstrated in vitro (Gagnon et al., 2007). Although, copper, zinc, manganese, iron, calcium, and selenium are essential micronutrients and have a variety of biochemical functions in living organisms, these elements can be toxic when taken in excess. For example, high manganese exposure in childhood can result in a neurotoxic syndrome affecting dopamine balance and behavior control (Ericson et al., 2007). Considering the recommended dietary allowance (RDA) values for zinc and iron, some authors have observed nutritional deficiencies for bottle-fed infants (Ikem et al., 2002). As a constituent of selenoproteins, selenium has structural and enzymatic roles, being best known as an antioxidant and catalyst for the production of active thyroid hormone (Rayman, 2000). It has been suggested that dietary calcium supplementation may be an effective prevention strategy to reduce the circulating levels of lead in the mother and the lead exposure in the developing fetus and nursing infant (Ettinger et al., 2007; Jiao et al., 2011). Therefore, the EU-funded research project CASCADE (chemicals as contaminants in the food chain; Network of Excellence, FP6 funded consortium, targeting health risks in food) decided to determined the levels of the 10 essential and non-essential elements such as: calcium (Ca), cadmium (Cd), copper (Cu), iron (Fe), mercury (Hg), manganese (Mn), nickel (Ni), lead (Pb), selenium (Se), and zinc (Zn) in the most-consumed baby foods in Europe. These elements were analyzed in weighted mixtures designed to represent an exclusive feeding based on commercial baby food at the different month-ages of an average European infant until reaching the age of 9 months. Additionally, the selected elements Cd and Zi were analyzed in four European national baskets designed until 5 months of age. Furthermore, the daily/ weekly intake of these elements in the age range 0–9 months for non-breast-fed infants was estimated and compared with recently established safety limits. 2. Materials and methods 2.1. Baby food items included in the study Market baskets of baby foods designed for consumption during the first 9 months of life by an ‘‘average’’ EU baby fed with infant formulae and weaned (at 5 months) with solid foods and beverages (SFB) were assessed and representatively pooled. These assessments were based on an infant whose diet consisted entirely of commercial baby foods, i.e. who was not breast fed at all. The 2007 market data made available by Food for Thought (www.fft.com) was used to identify the major brands of baby foods and their shares of the market in 22 EU countries considered to represent the entire EU. A total of 6 pooled samples of ‘‘starting’’ infant formulae of milk-based (Mf), soy-based (Sf), hypoallergenic-based (HAf) and ‘‘follow-on’’ infant formulae of milk-based (fMf), soy-based (fSf) and hypoallergenic-based (fHAf) and 5 pooled samples of solid foods and beverages designed for 5–9-month-old infants (SFB5, SFB6, SFB7, SFB8 and SFB9) were prepared separately for chemical target element analysis. Thus, 11 heterogenic samples were generated considering the different types of milk feeding (milk, soy-based and hypoallergenic) and the pattern of food consump-

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tion according to age in months of the non-breast-fed infant (solids and beverages). 2.1.1. ‘‘EU basket’’ To identify the holding companies and their main brands from which products would have to be sampled, the companies that constitute, altogether, over 80% of the market were selected (Piccinelli et al., 2010). Finally, 42 different infant formulae products were sampled from 6 different countries including France, Germany, Italy, Portugal, Sweden and UK. For the basket of SFB the same procedure was followed and 112 products were identified. Since it would have lead to very high costs of time and resources, a random sampling of brands, weighed on market share data, was performed in order to select only one brand within each typology of product. Consequently, 22 different SFB products were sampled from 5 different countries including Germany, Italy, France, Spain and UK. 2.1.2. ‘‘National basket’’ – Italy, Spain, Slovakia and Sweden In order to design the ‘‘national basket’’ of infant formulae in the 4 selected countries (Italy, Spain, Slovakia and Sweden) only one brand within basket was selected. This was the main brand producing infant formulae from the leading company with the highest market share in the country (Piccinelli et al., 2010). Finally, 24 national market baskets of infant formulae were designed including 24 different infant formulae products. For the national baskets of SFB, only the fifth month diet was considered due to lower number products included compared with the sixth, seventh, eighth and ninth months. A total of 4 national baskets of SFB5 were designed including 13 different solid food products (one brand within each typology product was considered). 2.2. Sample preparation The proportion of each infant formula product in the pooled EU basket sample was the same as its share of the European market, whereas the proportion of SFB item in the pooled sample was the same as its energy percentage in the infant diet. With regard to the national basket of infant formula, a single product was investigated and no sample preparation was performed. However, the proportion of each item in the pooled SFB5 sample was the same as its energy percentage in the infant diet. Further details have been reported in (Piccinelli et al., 2010). Sample lyophilization was performed for baby jar and beverage products using freeze drying equipment (Type BETA 1–16, Christ GmbH, Osterode, Germany) for about 36 h per sample. Consequently, in regard to the EU basket the fresh weight (fw) of 20 g SFB5, SFB6, SFB7, SFB8 and SFB9 resulted dry weight (dw) of 9.44, 8.55, 8.01, 8.59, 7.87 g, respectively. For the national baskets of Italy, Spain, Slovakia and Sweden the resulted dw of 20 g fw SFB5 was 9.72, 9.62, 10.66 and 9.86, respectively. The weighing procedures were performed in a purified glovebox under nitrogen atmosphere and the pooled samples were further homogenized in a rotoshaker (Type Reax 20/8, Heidolph GmbH) for 8 h. The samples were kept at room temperature and stored in brown glass jars protected from direct light. In order to prevent any contamination the opening and closing of the sample collector was performed under nitrogen atmosphere. For element determination, a 300 mg sample (related to solids) was exactly weighed into quartz vessels, and subsequently 8 mL of suprapure, subboiling distilled nitric acid (Merck, Darmstadt) was added. Digestion was performed in a Multiwave 3000 microwave digestion system (Anton Paar, Graz, Austria) at a power increase up to 750 W and remaining at 600 W for 30 min, followed by a 20-min cooling period. The resulting clear solution was filled up exactly to 30 mL with Milli-Q H2O (Millipore GmbH,

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Schwalbach, Germany) and was then ready for element determination. 2.3. Element determination Ten elements (Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se and Zn) were determined in EU basket samples, and only Cd and Zn were determined in the samples of the national basket from Italy, Slovakia, Spain and Sweden. The concentration levels of the SFB samples were converted per fw considering the lyophilization data. Since no freeze drying procedures were employed to the infant formula samples the results were given per fw powder. 2.3.1. ICP-AES An ICP-AES ICAP system (Thermo-Fischer Scientific GmbH, Dreieich, Germany) was used for Ca, Cu, Fe, Mn, Ni, Se and Zn determination in samples. Sample introduction was carried out using a peristaltic pump equipped with an ‘‘anti-pulse-head’’ (SPETEC, Erding, Germany), connected to a Meinhard nebulizer with a cyclon spray chamber. The measured spectral element lines were: Ca: 393.366 nm; Cu: 324.752 nm; Fe: 259.939; Mn: 257.61 nm; Ni: 231.604 nm; Se: 196.026 nm; and Zn: 213.857 nm. The radio frequency (RF) power was set to 1400 W, the plasma gas was 15 L argon (Ar)/min, whereas the nebulizer gas was 0.7 L Ar/min. Argonliqu was purchased from Air-Liquide, Gro¨benzell, Germany. An Ar vaporizer at the tank provided Ar gas. Quantification of element concentrations was done using 9 point calibration for each element in the range 0–2000 mg/L. Samples with concentrations above were appropriately diluted. 2.3.2. ICP-sf-MS An ELEMENT 1, Thermo-Finnigan (Bremen, Germany) ICP-sfMS instrument was employed for 208Pb, 202Hg and 112Cd determination in low resolution mode. Sample introduction was carried out using a peristaltic pump equipped with an anti-pulsehead (SPETEC), connected to a Meinhard nebulizer with a cyclon spray chamber. The RF power was set to 1200 W, the plasma gas was 15 L Ar/min, whereas the nebulizer gas was 0.9 L Ar/min. Argonliqu was purchased from Air-Liquide, Gro¨benzell, Germany.

An Ar vaporizer at the tank provided Ar gas. Quantification of element concentrations was done using 9 point calibration for each element in the range 0–10,000 ng/L. Samples with concentrations above were appropriately diluted. 2.3.3. Quality control for ICP-AES and ICP-sf-MS Ten sample measurements, three blank determinations and a control determination of a certified standard (CPI International) for all mentioned elements were performed. Dilutions of these certified standards were prepared at concentrations in the same range as previously determined sample concentration. Calculation of results was carried out on a computerized lab-data management system, relating the sample measurements to calibration curves, blank determinations, control standards and the weight of the digested sample. The limits of detection (LOD) related to infant formulae were 0.5 mg/kg fw for Cd, Pb and Hg; 0.1 mg/kg fw for Mn; 0.5 mg/kg fw for Cu, Fe, Ni, Se and Zn; and 0.005 g/kg fw for Ca. Furthermore, the LOD related to SFB were 0.2 mg/kg fw for Cd, Pb and Hg in SFB5–9; 0.05 and 0.04 mg/kg fw for Mn in SFB5 and SFB6–9; 0.2 mg/kg fw for Cu, Fe, Ni, Se and Zn in SFB5–9; and 0.002 g/kg fw for Ca in SFB5–9. 2.4. Reference values and safety limits for Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se and Zn in children Reference values and safety limits for children, adolescents and adults related to Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se and Zn were retrieved from the European Food Safety Authority (EFSA), the Scientific Committee for Food (SCF), Joint FAO/WHO Expert Committee on Food Additives (JECFA) and World Health Organization (Table 1). The safety limits were given in tolerable weekly intake (TWI), provisional tolerable weekly intake (PTWI), tolerable daily intake (TDI), tolerable upper limit (UL) and/or recommended daily intake (RDI). 2.5. Estimated daily baby foods consumed per body weight regarding EU babies in the first 9 months of life The mean daily intake of the 10 elements was calculated based on estimated average amount of infant formulae (ml/day) and solid

Table 1 Reference values and safety limits for Cd, Fe, Pb, Se, Hg, Cu, Ni, Zn, Ca, Mn in children. European Food Safety Authority (EFSA)

Scientific Committee for Food (SCF) (SCF, 2006)

Joint FAO/WHO Expert Committee on Food Additives (JECFA)

World Health Organization (WHO)

TWI

RDI

PTWI

TDI

UL

UL

Non-essential elements Cd 2.5 mg/kg bw (EFSA, 2011)

7 mg/kg bw (JECFA, 2003) 25 mg/kg bw (JECFA, 2002) 4 mg/kg bw (JECFA, 2010)

Pb Hg Ni

11 mg/kg bw (WHO, 2007)

Essential elements Se

60 mg/day for 1–3-year-old children (EFSA, 2009a)

Cu Fe

6 mg/day for 0.5–1-year-old children

Zn Ca

Mn

No TWI established for children and adolescents

For adults 2500 mg/day (EFSA, 2008) Adequate intake level of 1.2 mg/day for 1–3-year-old children (EFSA, 2009b)

500–800 mg/day for children up to 7 years old

60 mg/day for 1–3-year-old children 1 mg/day for 1–3-year-old children No UL established 7 mg/day for 1–3-year-old children No ULs for children and adolescents No UL established

M. Pandelova et al. / Journal of Food Composition and Analysis 27 (2012) 120–127 Table 2 Results of triplicate analysis of Cd, Fe, Pb, Se, Hg, Cu, Ni, Zn, Ca, Mn in hypoallergenic ‘‘follow-on formulae’’ (fHAf).

Ca (g/kg fw) Cd (mg/kg fw) Cu (mg/kg fw) Fe (mg/kg fw) Hg (mg/kg fw) Mn (mg/kg fw) Ni (mg/kg fw) Pb (mg/kg fw) Se (mg/kg fw) Zn (mg/kg fw)

fHAf (1)

fHAf (2)

fHAf (3)

4.2 4.5 3.5 59.5 25.6 809.0 270.0 10.8 645.0 39.2

4.1 3.5 3.5 58.1 11.8 856.0 83.7 7.5 299.0 41.4

4.3 3.6 3.2 59.7 5.7 1180.0 104.0 9.5 286.0 43.1

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pooled items (9 different hypoallergenic infant formulae) is given as an example. To achieve this quality control, fHAf was three times independently sampled and measured in their element content. The results of triplicate elemental analysis are shown in Table 2. Thus, the successful homogenization of the pooled samples was achieved such as it is indicated in this example. However, a deviation was observed for mercury, selenium and nickel. In the case of mercury this is related to the very low values present in the sample (closeness to the limit of detection), whereas nickel deviations are related to the limit of quantification of the methodology applied. 3.2. Concentration levels of Cd, Fe, Pb, Se, Hg, Cu, Ni, Zn, Ca, Mn in infant formulae and solid foods and beverages

foods and beverages (g/day) consumed by an ‘‘average EU baby’’ (Piccinelli et al., 2010). The values thus obtained were 25.2, 22.9, 21.0, 18.3, 12.8, 8.0, 4.6, 4.4 and 4.2 g (fw)/kg bw for infant formulae (powder) consumed by infants aged 0–1, 1–2, 2–3, 3–4, 4–5, 5–6, 6–7, 7–8 and 8–9 months, respectively; and 28.8, 54.7, 72.6, 70.2 and 71.9 g (fw)/kg bw for SFB consumed by infants aged 4–5, 5–6, 6–7, 7–8 and 8–9 months, respectively. In order to establish a meaningful comparison between the calculated dietary exposure and the safety limits established by international expert committees in some cases the values were additionally expressed in weekly units. 3. Results and discussion 3.1. Quality control of the pooled baby foods samples The quality control of the correct homogenization of each different type of sample was proven by elemental analysis of one sample. The sample of fHAf which contains the largest amount of

The concentration levels of Cd, Fe, Pb, Se, Hg, Cu, Ni, Zn, Ca and Mn in infant formulae and solid foods and beverages for infants until the age of 9 months based on the EU basket designed are shown in Table 3. In this table, the results of Cd and Zn in baby foods for infants until the age of 5 months based on the 4 national baskets designed (Italy, Slovakia, Spain and Sweden) are further presented. 3.3. Comparison between obtained and supplier labeled Zn values in infant formula Since each infant formula sample from the 4 national baskets was represented by one unique brand product the detected Zn amount was compared with the labeled value given from the product supplier (random selection). As a result, the obtained levels in the range of 31.7–55.8 mg/kg fw (Table 3) were found to be in agreement with the Zn values presented by supplier in the range of 32.9–47.7 mg/kg fw (data not shown). Cd values are not provided by any baby food supplier because it is a non-essential

Table 3 Concentration levels of Cd, Fe, Pb, Se, Hg, Cu, Ni, Zn, Ca, Mn in infant formulae and solid foods and beverages of designed ‘‘EU basket’’ and ‘‘national basket’’ (Italy, Slovakia, Spain, and Sweden). Element

Relative expanded uncertainty (%)

‘‘Starting’’ infant formulae Mf

EU basket Ca (g/kg fw) Cd (mg/kg fw) Cu (mg/kg fw) Fe (mg/kg fw) Hg (mg/kg fw) Mn (mg/kg fw) Ni (mg/kg fw) Pb (mg/kg fw) Se (mg/kg fw) Zn (mg/kg fw) National basket Cd (mg/kg fw) Zn (mg/kg fw) National basket Cd (mg/kg fw) Zn (mg/kg fw) National basket Cd (mg/kg fw) Zn (mg/kg fw) National basket Cd (mg/kg fw) Zn (mg/kg fw)

<3 <3 <5 <3 <10 <2 <7 <2 <12 <2 from Italy <3 <2 from Slovakia <3 <2 from Spain <3 <2 from Sweden <3 <2

Sf

HAf

‘‘Follow-on’’

SFB5

SFB6

SFB7

SFB8

SFB9

1.1 8.3 0.6 23.6 3 3 0.1 8.7 198.4 4.7

1.4 9.6 0.8 20.8 4.5 3.3 0.2 8.3 165.8 6

1.4 9.5 0.7 22.6 29.9 3.2 0.1 17.2 161.5 5.7

1.4 9.1 0.7 20.6 5.9 3.1 0.1 11 169.6 5.4

Infant formulae fMf

fSf

fHAf*

3.4 3.3 2.6 47.7 <0.5 0.5 <0.5 8.2 84.7 32.9

4.8 15.8 3.3 70.4 <0.5 3.3 <0.5 30.5 120 41.6

3.1 4.2 2.5 46.5 <0.5 0.8 <0.5 13.2 73.8 36

5.5 4.5 3.9 69.1 113 0.6 0.1 43.9 510 46.5

4.8 18.3 3.2 67.3 29.3 3.3 1.3 20.1 222 47.7

4.2 3.9 3.4 59.1 14.4 0.9 0.1 9.3 410 41

0.2 2.8 0.4 27 2.7 1.5 <0.2 7.9 81.7 2.9

5.8 31.7

18.2 45.1

3.7 37.7

5.2 37.6

17.2 47.8

7.1 36.1

10.3 6.6

5 37.9

3.7 38.6

14.6 55.2

1.9 55.2

3.7 38.6

2.6 51.3

7.2 7.1

5.6 37.7

10.6 49.9

2.2 39.8

5.7 49.6

10.6 49.9

7.5 55.8

10.1 6.2

3.9 52.3

12.8 52

9 41.5

3 36.2

12.8 52

9 41.5

21.8 16.5

Expanded uncertainty (EUc) was calculated twice the standard deviation. EUc-values for an element are below the given range for all results in a row. Mf: ‘‘starting’’ infant formulae of milk-based; Sf: ‘‘starting’’ infant formulae of soy-based; HAf: ‘‘starting’’ infant formulae of hypoallergenic-based; fMf: ‘‘follow on’’ infant formulae of milk-based; fSf: ‘‘follow on’’ infant formulae soy-based; fHAf: ‘‘follow on’’ infant formulae hypoallergenic-based; SFB5, SFB6, SFB7, SFB8, and SFB9: solid baby foods and beverages designed for 5, 6, 7, 8, and 9-month-old infants, respectively. * Mean value within triplicate analysis.

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element. It makes a direct comparison not possible. In the case of the European baskets, the obtained values correspond to pooled samples thus, a direct comparison with the labeled data provided by the single product suppliers is not possible. 3.4. Infant daily/weekly intake of Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se and Zn by consumption of commercial baby foods Based on the consumption data (see Section 2.5) and the concentration levels of the 10 elements here analyzed (Table 3), the daily/weekly intake of Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se and Zn of

infants fed with baby foods until 9 months of age from the EU basket and Cd and Zn intakes from the national baskets (Italy, Slovakia, Spain and Sweden) until 5 months of age was estimated (Table 4). The results shown in Table 4 were further compared with the current safety limits of these elements (Table 1). 3.4.1. Cadmium In regard to both types of baskets, a similar Cd intake of 0.5  0.4 mg/kg bw/week was assessed for infants consuming infant formulae (Table 4). However, greater Cd intake of 2.1  0.7 mg/kg bw infant was estimated when considering the consumption of ‘‘starting’’

Table 4 Calculated daily/weekly infant intake of Ca, Cd, Cu, Fe, Hg, Mn, Ni, Pb, Se and Zn through consumption of infant formula and solid foods and beverages (SFB) based on designed EU basket and national basket (Italy, Slovakia, Spain, and Sweden). Infant age (month)

EU basket Ca (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Cd (mg/kg bw/week) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Cu (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Fe (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Hg (mg/kg bw/week) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Mn (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Ni (mg/kg bw/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Pb (mg/kg bw/week) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Se (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Zn (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB National basket from Italy Cd (mg/kg bw/week) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB

0–1

1–2

2–3

3–4

4–5

5–6

6–7

7–8

8–9

331.2 459.8 297.6

382.9 531.7 344.1

414.0 574.8 372.0

403.6 560.4 362.7

493.1 428.1 376.5 37.8

332.4 288.6 253.8 450.2

199.4 173.2 152.3 769.4

199.4 173.2 152.3 782.0

199.4 173.2 152.3 831.9

0.6 2.8 0.7

0.5 2.5 0.7

0.5 2.3 0.6

0.4 2.0 0.5

0.4 1.6 0.4 0.6

0.3 1.0 0.2 3.2

0.1 0.6 0.1 4.9

0.1 0.6 0.1 4.7

0.1 0.5 0.1 4.6

0.2 0.3 0.2

0.3 0.4 0.3

0.3 0.4 0.3

0.3 0.4 0.3

0.3 0.3 0.3 0.1

0.2 0.2 0.2 0.2

0.1 0.1 0.1 0.5

0.1 0.1 0.1 0.4

0.1 0.1 0.1 0.4

4.6 6.8 4.5

5.3 7.8 5.2

5.7 8.4 5.6

5.6 8.2 5.4

6.1 6.0 5.3 5.4

4.1 4.0 3.5 9.6

2.5 2.4 2.1 11.8

2.5 2.4 2.1 12.9

2.5 2.4 2.1 12.4

<0.1 <0.1 <0.1

<0.1 <0.1 <0.1

<0.1 <0.1 <0.1

<0.1 <0.1 <0.1

10.2 2.6 1.3 0.5

6.4 1.6 0.8 1.1

3.6 0.9 0.5 2.3

3.5 0.9 0.4 14.7

3.4 0.9 0.4 3.0

0.0 0.3 0.1

0.0 0.4 0.1

0.1 0.4 0.1

0.1 0.4 0.1

0.0 0.3 0.1 0.3

0.0 0.2 0.1 1.2

0.0 0.1 0.0 1.9

0.0 0.1 0.0 1.8

0.0 0.1 0.0 1.9

<0.01 <0.01 <0.01

<0.01 <0.01 <0.01

<0.01 <0.01 <0.01

<0.01 <0.01 <0.01

0.00 0.02 0.00 <0.01

0.00 0.01 0.00 0.01

0.00 0.01 0.00 0.01

0.00 0.01 0.00 0.01

0.00 0.01 0.00 0.01

1.4 5.4 2.3

1.3 4.9 2.1

1.2 4.5 1.9

1.0 3.9 1.7

3.9 1.8 0.8 1.6

2.5 1.1 0.5 3.3

1.4 0.6 0.3 4.2

1.4 0.6 0.3 8.5

1.3 0.6 0.3 5.5

8.1 11.5 7.1

9.4 13.3 8.2

10.2 14.4 8.9

9.9 14.0 8.6

45.4 19.8 36.5 16.3

30.6 13.3 24.6 80.3

18.4 8.0 14.8 93.7

18.4 8.0 14.8 91.9

18.4 8.0 14.8 102.4

3.2 4.0 3.5

3.6 4.6 4.0

4.0 5.0 4.3

3.8 4.9 4.2

4.1 4.2 3.6 0.6

2.8 2.9 2.5 1.9

1.7 1.7 1.5 3.4

1.7 1.7 1.5 3.2

1.7 1.7 1.5 3.3

1.0 3.2 0.7

0.9 2.9 0.6

0.8 2.7 0.5

0.7 2.3 0.5

0.5 1.5 0.6 2.1

0.3 2.0 0.0

0.2 2.7 0.0

0.2 2.6 0.0

0.2 2.6 0.0

M. Pandelova et al. / Journal of Food Composition and Analysis 27 (2012) 120–127

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Table 4 (Continued ) Infant age (month) 0–1 Zn (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB National basket from Slovakia Cd (mg/kg bw/week) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Zn (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB National basket from Spain Cd (mg/kg bw/week) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Zn (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB National basket from Sweden Cd (mg/kg bw/week) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB Zn (mg/day) Milk infant formula Soy infant formula Hypoallergenic infant formula SFB

1–2

2–3

3–4

4–5

5–6

6–7

7–8

8–9

3.0 4.3 3.6

3.5 5.0 4.2

3.8 5.4 4.5

3.7 5.3 4.4

3.3 4.2 3.2 1.3

2.3 2.9 2.2

1.3 1.7 1.3

1.3 1.7 1.3

1.3 1.7 1.3

0.9 0.6 2.6

0.8 0.6 2.3

0.7 0.5 2.1

0.6 0.5 1.9

0.2 0.3 0.2 1.5

0.0 0.2 0.0

0.0 0.1 0.0

0.0 0.1 0.0

0.0 0.1 0.0

3.6 3.7 5.3

4.2 4.3 6.1

4.5 4.6 6.6

4.4 4.5 6.5

4.9 3.4 4.6 1.4

3.3 2.3 3.1

2.0 1.4 1.8

2.0 1.4 1.8

2.0 1.4 1.8

1.0 1.9 0.4

0.9 1.7 0.3

0.8 1.6 0.33

0.7 1.4 0.3

0.5 0.1 0.7 2.0

0.3 0.6 0.4

0.2 0.3 0.2

0.2 0.3 0.2

0.2 0.3 0.2

3.6 4.8 3.8

4.2 5.5 4.4

4.5 6.0 4.8

4.4 5.8 4.7

4.4 4.4 5.0 1.2

3.0 3.0 3.3

1.8 1.8 2.0

1.8 1.8 2.0

1.8 1.8 2.0

0.7 2.3 1.6

0.6 2.0 1.4

0.6 1.9 1.3

0.5 1.6 1.1

0.3 1.1 0.8 4.4

0.2 0.7 0.5

0.1 0.4 0.3

0.1 0.4 0.3

0.1 0.4 0.3

5.0 5.0 4.0

5.8 5.8 4.6

6.3 6.2 5.0

6.1 6.1 4.9

3.2 4.6 3.7 3.3

2.2 3.1 2.2

1.3 1.9 1.3

1.3 1.9 1.3

1.3 1.9 1.3

soy-based infant formulae. Overall, these values are lower than the reported Cd exposure of 3.6–4.9 mg/kg bw/week for 0–9 month Canadian infants fed with soy-based formula (Dabeka, 1989). Elevated Cd week exposure during the first 4 months considers only these infants, whose diet is based on soy products. For the period from the 5th to the 9th month of life, the main contribution to Cd exposure is found to be the SFB. A cumulative exposure of 4.7  0.7 mg/kg bw/week may occur for infants during the weaning period. Furthermore, a Swedish data have manifested that more than 80% of the dietary Cd intake comes from plant foods (Olsson et al., 2002), mainly cereals (especially whole grains), vegetables, root vegetables and potatoes. Cadmium absorption after dietary exposure in humans is relatively low (3–5%) but cadmium is efficiently retained in the kidney and liver in the human body, with a very long biological half-life ranging from 10 to 30 years (EFSA, 2009a). The developed approach also showed that feeding with foods from different country markets influences the amount of Cd intake. For example, a 4–5month-old Swedish infant fed with SFB from the local market may ingest up to 5.3 mg/kg bw/week or about twice more than an infant from Italy, Spain, or Slovakia. Accordingly, in many cases (Table 4) the safety limit established by EFSA for cadmium (TWI = 2.5 mg/kg bw/ week) is exceeded (EFSA, 2011). 3.4.2. Zinc Since there are no data indicating that children or adolescents are more susceptible to the adverse effects of Zn (SCF, 2003), the SCF had extrapolated the UL from adults to children (1–3 years old) and proposed 7 mg/day as a UL for zinc in this age class (SCF, 2006). Considering the EU basket, the estimated mean daily intake of Zn was 4.5  0.5 mg/day for the infants aged 0–9 months (Table 4).

Similar Zn intake of 4.4  0.7, 5.0  1.0, 4.9  0.8 and 5.7  1.0 mg/ day was assessed for 0–5-month-old infants fed with baby foods from the ‘‘national basket’’ of Italy, Slovakia, Spain and Sweden, respectively. 3.4.3. Iron Present data suggested 6.1  1.4 mg of Fe mean daily intake for infants aged 0–4 months who were fed exclusively with infant formulae, whereas the mean daily intake for infants aged 5–9 months during the weaning period was 13.7  1.5 mg iron (Table 4). For comparison, SCF established RDI for infants aged 0.5–1 years is 6 mg Fe (SCF, 2006). 3.4.4. Copper Nearly identical Cu mean intakes of 0.4  0.1 mg/day were estimated during the whole infant formula feeding and the weaning period for the EU average infant aged 0–9 months (Table 4). These values are within ULs of 1 mg Cu/day regarding 1–3-year-old children (SCF, 2006). However, a recent Fe, Cu and Zn survey manifested significantly higher concentrations in powdered infant formula than those concentrations found in human milk from Canary Island women (Saracoglu et al., 2007). Moreover, the Committee noted that additional copper intakes from drinking water may be appreciable and may need to be taken into account for the whole intake assessment. 3.4.5. Selenium Relatively low Se mean intake of 10.3  2.5 mg/day was estimated for the infants exclusively fed with infant formula during the first 4 months of life (Table 4). Another study on estimation of selenium infant intake that consider some commercial infant

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formulae from the Spanish market has indicated a value lower than 10 mg Se/day for infants in the first month of their life (NavarroBlasco and Alvarez-Galindo, 2005). However, the assessed cumulative mean Se intake of 98.0  23.0 mg/day for infants aged 5–9 months exceeded EFSA and SCF established UL of 60 mg/day for children at the age of 1–3 years (SCF, 2006; EFSA, 2009b). 3.4.6. Manganese Since there is no recommended Mn tolerable upper level, the ATSDR estimated adequate intake level of 0.003 and 0.6 mg/day for infants aged 0–6 and 7–12 months, respectively (EFSA, 2009c). The estimated here Mn mean intakes for the mentioned above infant periods (0–6 and 7–12 months) were 0.53  0.64 and 1.92  0.06 mg/day, respectively (Table 4). In agreement with our results, several other studies have found a newborn’s overexposure to Mn through ingestion of infant formula that may be associated with adverse neurotoxic effects (Ljung et al., 2011; Menezes-Filho et al., 2009). 3.4.7. Calcium Stepwise increase in Ca daily mean intake from 362.9  85.6 mg to 740.0  39.4 mg and to 1011  23.6 mg for infants aged 0–1, 5–6 and 8–9 months, respectively, is shown in Table 4. According to German data of non-breast-fed infants, the 90th percentile of Ca intake was from 700 to 900 mg/day (Alexy and Kersting, 1999). Since there were no sufficient data to define UL for infants, only the RDI of 500–800 mg Ca for children up to 7 years of age was considered (SCF, 2006). 3.4.8. Lead Mean Pb intakes of 2.6  1.6 and 5.8  2.1 mg/kg bw/week for infants during the formula-feeding (0–4 months old) and weaning period (5–9 months old), respectively, were suggested. Considering the weaning period, a progressive increase in Pb exposure was observed. The leading contribution of Pb exposure between 1.6 and 8.5 mg/kg bw/week for the non-breast-fed infants was determined in the SFB samples (Table 4). Indeed, the highest cumulative Pb exposure assessed was 9.8 mg/kg bw/week and concerned infants aged 7–8 months fed with fMf and SFB8. Overall, the estimated values do not exceed JECFA established PTWI of 25 mg/kg bw/week (JECFA, 2002). Several studies conducted in Germany (Schumann, 1990), Australia (Gulson et al., 2001) and Canada (Dabeka and McKenzie, 1987) manifested higher Pb level determined in cows’ milk-based infant formula than human milk. Therefore, the control of Pb in infant formulae seems to be essential. 3.4.9. Mercury Our results suggested Hg levels lower than the LOD in ‘‘starting’’ infant formulae (Table 3). However, elevated Hg levels in fSf and SFB8 samples and considerable Hg level of 113 mg/kg fw in fMf (Table 3) were found. Due to differences in the pattern of consumption during the weaning period the assessed Hg exposure was mainly contributed by the SFB. The worst-case scenario suggested a weekly exposure of 18.2 mg Hg/kg bw infants (7–8 months old) consuming fMf and fish-based commercial infant solid foods. However, the estimated Hg exposure for infants aged 8–9 months was reduced by three when considering the factor of body weight and the introduction of new food items in SFB9 of designed EU basket. Subsequently, the highest exposure via infant formula (10.2 mg/kg bw/week) was assessed during the first 4–5 months of life regarding infants who consume fMf. In this context, the estimated exposure exceed the established by JECFA PTWI of 4 mg Hg/kg bw (JECFA, 2010) regarding dietary exposure of inorganic mercury from foods others than fish and shellfish. Recently, the Institute for Agriculture and Trade Policy has reported detectable levels of Hg in high fructose corn syrup

(HFCS) (IATP, 2009). But, no presence of HFCS was labeled in here investigated infant formulae. 3.4.10. Nickel Dietary exposure of 0–0.02 mg/kg bw/day was assessed for nonbreast-fed infants aged 0–9 months consuming food from the EU market (Table 4). These values are well below the WHO TDI for nickel of 11 mg/kg bw (WHO, 2007). 4. Conclusions The results of generated EU basket and national basket samples suggest that the levels of all essential and non-essential elements in ‘‘starting’’ soy-based infant formulae are higher than the values obtained for the milk-based or hypoallergenic-based powder formulations. The same finding of higher metal abundance in soy-based powder brands was also manifested by other large surveys in USA and Canada (Ikem et al., 2002). Besides, elevated levels of the non-essential Hg and Pb were observed in designed fMf sample. Due to possible risks on human health from the consumption of foods other than fish and shellfish, the JECFA established a PTWI of 4 mg/kg bw that takes inorganic Hg into consideration (JECFA, 2010). Since 10.1 and 6.4 mg Hg/kg bw/week was found for infants aged 4–5 and 5–6 months who consume fMf the exposures could be harmful. The current study based on consumption of infant food based on a designed EU basket suggested Pb exposure for infants aged 0–9 months lower than the established PTWI of 25 mg Pb/kg bw. However, the assessed Cd exposure during the weaning period was found to exceed the TWI of 2.5 mg/kg bw (EFSA, 2011) and nearly attain the JECFA established PTWI of 7 mg/kg bw (JECFA, 2003). Finally, it should be pointed out that the infant baskets designed here concern only foods that may include the diet for infants aged 0–9 months and belong to one particular case within current feeding practices, where breast milk (mother’s milk) is the preferred food. Despite the strong endorsement of breastfeeding, the vast majority of infants receive infant formulae or solid foods during their first year, exclusively or in combination with breast milk. Consequently, additional survey work on element analysis and dietary infant intake by breast milk is necessary. To sum up, the current study provides a broad overview of the intake of essential minerals and non-essential trace elements in industrial baby foods, and can be useful for further studies in health risk assessments. Acknowledgements The authors would like to thank to Raffaela Piccinelli and Catherine Leclercq for their cooperation work and support in preparation of the manuscript. Thanks to all CASCADE partners who assisted in acquiring information and shopping for baby food products, namely Ingemar Pongratz, Lars-Arne Haldosen, Stefan Rehnmark, Nicolas Olea, Jean-Pierre Cravedi and Ju´lius Brtko. The study was financial supported by the European Union network CASCADE (FOOD-CT-2003-506319) within the framework of WP19 projects (bread project and baby food project). References Alexy, U., Kersting, M., 1999. Was Kinder essen und was essen sollten. Die DONALDStudie und die Erna¨hrungskonzepte des Forschungsinstituts fu¨r Kindererna¨hrung Dortmund (FKE) Hans Marseille Verlag GmbH, Mu¨nchen. Cattaneo, A., 2004. Protection, promotion and support of breastfeeding in Europe: a blueprint for action. EU Project Contract N. SPC 2002359. Retrieved June 18, 2004 from the European Commission home page http://ec.europa.eu/health/ ph_projects/2002/promotion/fp_promotion_2002_frep_18_en.pdf.

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