Dietary Sources of Methylated Arsenic Species in Urine of the United States Population, NHANES 2003–2010

PLOS ONE, Dec 2019

Background Arsenic is an ubiquitous element linked to carcinogenicity, neurotoxicity, as well as adverse respiratory, gastrointestinal, hepatic, and dermal health effects. Objective Identify dietary sources of speciated arsenic: monomethylarsonic acid (MMA), and dimethylarsinic acid (DMA). Methods Age-stratified, sample-weighted regression of NHANES (National Health and Nutrition Examination Survey) 2003–2010 data (∼8,300 participants ≥6 years old) characterized the association between urinary arsenic species and the additional mass consumed of USDA-standardized food groups (24-hour dietary recall data), controlling for potential confounders. Results For all arsenic species, the rank-order of age strata for median urinary molar concentration was children 6–11 years > adults 20–84 years > adolescents 12–19 years, and for all age strata, the rank-order was DMA > MMA. Median urinary molar concentrations of methylated arsenic species ranged from 0.56 to 3.52 µmol/mol creatinine. Statistically significant increases in urinary arsenic species were associated with increased consumption of: fish (DMA); fruits (DMA, MMA); grain products (DMA, MMA); legumes, nuts, seeds (DMA); meat, poultry (DMA); rice (DMA, MMA); rice cakes/crackers (DMA, MMA); and sugars, sweets, beverages (MMA). And, for adults, rice beverage/milk (DMA, MMA). In addition, based on US (United States) median and 90th percentile consumption rates of each food group, exposure from the following food groups was highlighted: fish; fruits; grain products; legumes, nuts, seeds; meat, poultry; and sugars, sweets, beverages. Conclusions In a nationally representative sample of the US civilian, noninstitutionalized population, fish (adults), rice (children), and rice cakes/crackers (adolescents) had the largest associations with urinary DMA. For MMA, rice beverage/milk (adults) and rice cakes/crackers (children, adolescents) had the largest associations.

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Dietary Sources of Methylated Arsenic Species in Urine of the United States Population, NHANES 2003–2010

NHANES 2003-2010. PLoS ONE 9(9): e108098. doi:10.1371/journal.pone.0108098 Dietary Sources of Methylated Arsenic Species in Urine of the United States Population, NHANES 2003-2010 B. Rey deCastro 0 Kathleen L. Caldwell 0 Robert L. Jones 0 Benjamin C. Blount 0 Yi Pan 0 Cynthia Ward 0 Mary E. Mortensen 0 David O. Carpenter, Institute for Health & the Environment, United States of America 0 Centers for Disease Control and Prevention, National Center for Environmental Health, Division of Laboratory Sciences , Atlanta, Georgia , United States of America Background: Arsenic is an ubiquitous element linked to carcinogenicity, neurotoxicity, as well as adverse respiratory, gastrointestinal, hepatic, and dermal health effects. Objective: Identify dietary sources of speciated arsenic: monomethylarsonic acid (MMA), and dimethylarsinic acid (DMA). Methods: Age-stratified, sample-weighted regression of NHANES (National Health and Nutrition Examination Survey) 20032010 data (,8,300 participants $6 years old) characterized the association between urinary arsenic species and the additional mass consumed of USDA-standardized food groups (24-hour dietary recall data), controlling for potential confounders. Results: For all arsenic species, the rank-order of age strata for median urinary molar concentration was children 6-11 years . adults 20-84 years . adolescents 12-19 years, and for all age strata, the rank-order was DMA . MMA. Median urinary molar concentrations of methylated arsenic species ranged from 0.56 to 3.52 mmol/mol creatinine. Statistically significant increases in urinary arsenic species were associated with increased consumption of: fish (DMA); fruits (DMA, MMA); grain products (DMA, MMA); legumes, nuts, seeds (DMA); meat, poultry (DMA); rice (DMA, MMA); rice cakes/crackers (DMA, MMA); and sugars, sweets, beverages (MMA). And, for adults, rice beverage/milk (DMA, MMA). In addition, based on US (United States) median and 90th percentile consumption rates of each food group, exposure from the following food groups was highlighted: fish; fruits; grain products; legumes, nuts, seeds; meat, poultry; and sugars, sweets, beverages. Conclusions: In a nationally representative sample of the US civilian, noninstitutionalized population, fish (adults), rice (children), and rice cakes/crackers (adolescents) had the largest associations with urinary DMA. For MMA, rice beverage/milk (adults) and rice cakes/crackers (children, adolescents) had the largest associations. - Data Availability: The authors confirm that all data underlying the findings are fully available without restriction. All National Health and Nutrition Examination Survey Data files are available at http://www.cdc.gov/nchs/nhanes.htm. Funding: The authors have no funding or support to report. Competing Interests: The authors have declared that no competing interests exist. Arsenic is an ubiquitous metalloid element present in the environment as inorganic species with different oxidation states, or as part of organic compounds. Inorganic arsenic species of greatest environmental health concern have oxidation states of +3 (As(III) or arsenite) or +5 (As(V) or arsenate), and are classified as human carcinogens [1,2]. People with chronic exposure to high levels of inorganic arsenic species in drinking water have manifested neurotoxicity, skin lesions, gastrointestinal and liver dysfunction, and cardiovascular disease [36]. In the United States, regulations limit arsenic in public water systems and in bottled water to 10 mg/L [7,8]. The methylated arsenic species dimethylarsinic acid (DMA) and monomethylarsonic acid (MMA) have both been detected in soils, fresh and marine waters, and fish and shellfish. Human metabolic biotransformation of inorganic arsenic involves reduction from As(V) to As(III), followed by oxidative methylation to monomethyarsinic acid (MMA) and dimethylarsinic acid (DMA) [5,9]. Since most arsenic species absorbed from the gastrointestinal tract is excreted in urine within 13 days [10 15], urinary arsenic is well-suited as an exposure biomarker to correlate with NHANES 24-hour dietary recall data. Although inorganic species have been a focus of concern because of their carcinogenicity [16], certain methylated arsenic species may be carcinogenic [17,18]. Indeed, there is greater awareness that methylation of inorganic arsenic species may also affect susceptibility to arsenic-induced disease and may vary among individuals depending on genetic polymorphism, dose, age, selenium intake, as well as folate and homocysteine status [5,17,1927]. Exposure to DMA [28] and MMA [2935] have produced tumors in animal studies, resulting in concerns about human carcinogenicity. Several studies have examined selected US (United States) foods for total and inorganic arsenic species content [3640], or have examined the relationship between consumption of selected foods and total urinary arsenic [36,39] and speciated arsenic [4143]. Using US FDAs (Food (...truncated)


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B. Rey deCastro, Kathleen L. Caldwell, Robert L. Jones, Benjamin C. Blount, Yi Pan, Cynthia Ward, Mary E. Mortensen. Dietary Sources of Methylated Arsenic Species in Urine of the United States Population, NHANES 2003–2010, PLOS ONE, 2014, 9, DOI: 10.1371/journal.pone.0108098