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Abstract; About This Article; Background: Rice can be a major source of inorganic arsenic (As i) for many sub-populations. Rice products are also used as ingredients.
Citation: Jackson BP, Taylor VF, Karagas MR, Punshon T, Cottingham KL. 2012. Arsenic, Organic Foods, and Brown Rice Syrup. Environ Health Perspect 120:623–626; http://dx.doi.org/10.1289/ehp.1104619 Address correspondence to B. Jackson, Trace Element Analysis Core, Dartmouth College, Hanover, NH, 03755 USA. Telephone: (603) 646-1272. Fax: (603) 646-3922. E-mail: [email protected] We thank L. Webb for assistance with market-basket research and J. Chen for assistance in the laboratory. This work was supported by grants P20 ES018175 and P42 ES007373 from the National Institute of Environmental Health Sciences (NIEHS) and RD-83459901-0 from the U.S. Environmental Protection Agency (EPA). The NIEHS and U.S. EPA were not involved in the design and conduct of the study or collection, management, analysis, and interpretation of the data. The contents of this manuscript are solely the responsibility of the authors and do not necessarily represent the official views of the NIEHS or U.S. EPA. Further, the U.S. EPA does not endorse the purchase of any commercial products or services mentioned in the publication. The authors declare they have no actual or potential competing financial interests. Received: 13 October 2011 Accepted: 13 February 2012 Advance Publication: 16 February 2012 Final Publication: 1 May 2012 Arsenic (As) is an established carcinogen based on studies of populations consuming contaminated drinking water (Smith et al. 2002). Recently, attention has focused on As exposure from food, in particular fruit juices (Rock 2012) and rice (Stone 2008). Rice may contain As in total concentrations up to 100–400 ng/g, including both inorganic As (Asi) and the organic species dimethyl-arsenate (DMA) (Williams et al. 2005), with much lower concentrations (relative to DMA) of mono-methyl-arsenate (MMA) also occasionally detected. Total As (Astotal) in rice and relative proportions of DMA and Asi differ both geographically (Meharg et al. 2009) and as a function of genetic and environmental controls (Norton et al. 2009). As-i is more toxic than DMA or MMA (Le et al. 2000), and food regulatory limits, where they exist, are based on Asi. Infants fed rice cereal at least once daily may exceed the daily As exposure limit of 0.17 µg/kg body weight per day based on drinking water standards (Meharg et al. 2008b). Rice products such as cereals and crackers (Sun et al. 2009) and rice drinks (Meharg et al. 2008a) are potentially significant dietary sources of As. Infants and young children are especially vulnerable because their dietary As exposure per kilogram of body weight is 2–3 times higher than that of adults [European Food Safety Authority (EFSA) 2009 ]. DMA is a metabolite of Asi. Although considered less toxic than Asi, its toxicological potential has not been studied extensively. The presence of DMA in rice is likely due to natural soil microbial processes; however, DMA was used as a pesticide before being banned by the U.S. Environmental Protection Agency (EPA) in 2009 (U.S. EPA 2009). Organic food consumers may therefore object to its presence in organic foods even in the absence of direct evidence of human health effects of DMA. In the United States, organic brown rice syrup (OBRS) is used as a sweetener as a healthier alternative to high-fructose corn syrup in products aimed at the “organic foods” market. Added sugar is often the main ingredient in infant and toddler formula, and the addition of sucrose to a main-brand organic formula was the feature of a popular press article in relation to possible childhood obesity (Moskin 2008). Many products—including some baby milk formulas, cereal bars, and high-energy performance products for athletes—list OBRS as the major ingredient. Brown rice is usually higher in both Astotal and Asi than white rice because Asi is localized to the aleurone layer, which is removed when rice is polished, whereas DMA passes into the grain (Carey et al. 2011; Sun et al. 2008). Ranges of As concentration in rice products, including OBRS, are similar to As concentrations in brown rice (Signes-Pastor et al. 2009). We posit that consumers of organic food products are generally attempting to make educated eating choices and that this consumer group would be particularly interested to know if, and to what extent, OBRS introduces Asi, DMA, and MMA into these products. We therefore measured Astotal and As speciation in three commercially available brown rice syrups, 15 infant formulas without OBRS, 2 toddler formulas with OBRS, 29 cereal bars (13 with OBRS), and three flavors of a high-energy performance product. We purchased three commercial OBRSs from local or online stores. For one syrup, two bottles of the same product (from different lots) were tested. Fifteen infant formulas and two toddler formulas (initially purchased as part of a parallel study on As content of formulas and infant foods), as well as 29 cereal bars and three energy shot blocks were all purchased from local stores in the Hanover, New Hampshire, area. Sample preparation. All samples were analyzed for Astotal, and selected samples were extracted for As species. For formulas, Astotal was determined after closed vessel micro-wave digestion (MARSXpress; CEM Corp., Matthews, NC) with Optima HNO3. Approximately 0.25 g formula was digested in 2 mL 50% HNO3 (nitric acid). The samples were heated at 180°C for 10 min, allowed to cool, and then diluted to 10–25 mL with deionized water. Cereal bars and energy blocks were homogenized using a ceramic knife and were not dried before digestion. A sub-sample was digested in 2–3 mL Optima HNO3 and heated at 95°C for 30 min. The digested sample was diluted with deionized water to 25–50 mL. This digested sample was diluted a further 10× before analysis to reduce the acid concentration in the sample to < 5%. All digestions and dilutions were recorded gravimetrically. Samples were extracted for As speciation using 1% HNO3 and open-vessel heating in a micro-wave digestion unit following a heating profile of 55°C for 5 min, 75°C for 5 min, and 95°C for 20 min (Foster et al. 2007; Huang et al. 2010). An aliquot of the extracted sample was then centrifuged at 13,300 rpm for 30 min; an aliquot of that supernatant was further spin filtered at 10 kDa. Astotal and As speciation. Astotal was determined by inductively coupled plasma mass spectrometry (ICP-MS; model 7700x; Agilent, Santa Clara, CA) using helium as a collision gas at a flow rate of 4.5 mL/min. Samples were analyzed by either external calibration or the method of standard additions. As speciation of the 1% HNO3 extracts was determined by ion chromatography coupled to ICP-MS using a Hamilton PRP X100 anion exchange column (Hamilton Company, Reno, NV) and a 20 mM ammonium phosphate eluant at pH 8. Formulas were evaluated in triplicate, and 5% duplicate and duplicate spikes were performed for the cereal bars and energy blocks. We used NIST Standard Reference Material (SRM) 1568a rice flour (National Institute of Standards and Technology, Gaithersburg, MD) as a quality control material for both Astotal measurements and As speciation. Although As species are not certified for SRM 1568a, reproducible consensus values have been demon-strated in many studies (Meharg and Raab 2009; Raab et al. 2009; Williams et al. 2005). We determined Astotal in SRM 1568a to be 279 ± 31 ng/g (mean ± 1 SD; n = 6); the certified value is 290 ± 30 ng/g. For As speciation (n = 5), we determined DMA to be 186 ± 21 ng/g, MMA to be 9.4 ± 3.7 ng/g, and Asi to be 101 ± 15 ng/g, which are in the range reported by other studies. Data analyses. Given our calculated values for As speciation in the formulas, we estimated As concentrations (micrograms per liter) of reconstituted formulas assuming that one scoop of powdered formula weighs 8.75 g and that one scoop of formula is added to 60 mL As-free water to make 2 fluid ounces of formula. We then estimated daily intake of As species for a baby weighing 6 kg and 9 kg, assuming consumption of six 4-ounce bottles of milk formula each day, and compared this with “safe” levels estimated for consumption of drinking water containing Asi at the U.S. EPA and World Health Organization (WHO) maximum contaminant limit of 10 µg/L (Meharg et al. 2008b). Results and Discussion Rice syrups. Astotal concentrations in three rice syrups (and from two lots of one of the syrups) ranged from 80 to 400 ng/g (Table 1). Asi was 80–90% of Astotal for two of the three syrups; for the third syrup, only 50% of Astotal was Asi. However, because this syrup was much higher in Astotal, it also had the highest Asi concentration of the syrups. All syrups had detectable MMA, ranging from 3 to 4% of Astotal, but the major organic As species for each syrup was DMA. Our results are similar to those of Signes-Pastor et al. (2009) who reported dry weight Astotal concentrations of 80, 100, 120, and 330 ng/g in four rice syrups, with 71% Asi and 85% extraction efficiency in the highest As syrup. Moreover, given these authors’ estimate of 15% moisture content for the syrups, we estimate that the actual contribution to As concentration in food products that include OBRS as the dried product—such as toddler formulas—would be approximately 1.15 times the concentration listed in Table 1.
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Arsenic, Organic Foods, and Brown Rice Syrup