Determination of total arsenic and hydrophilic arsenic species in seafood.
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ABSTRACT:
SUBMITTER: Luvonga C
PROVIDER: S-EPMC8174234 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Seafood is the main source of organic arsenic exposure (arsenobetaine, arsenosugars and arsenolipids) in the population. Arsenosugars and arsenolipids are metabolized to several species including dimethylarsinate (DMA).Evaluate the association of seafood intake with spot urine arsenic concentrations in the 2003-2006 National Health Nutrition and Examination Survey (NHANES).We studied 4276 participants ? 6 years. Total arsenic was measured using inductively coupled plasma dynamic reaction cell mass spectrometry (ICPMS). Urine DMA and arsenobetaine were measured by high-performance liquid chromatography coupled with ICPMS.Participants reporting seafood in the past 24-h had higher urine concentrations of total arsenic (median 24.5 vs. 7.3 ?g/L), DMA (6.0 vs. 3.5 ?g/L), arsenobetaine (10.2 vs. 0.9 ?g/L) and total arsenic minus arsenobetaine (11.0 vs. 5.5 ?g/L). Participants reporting seafood ? 2/wk vs. never during the past year had 2.3 (95% confidence interval 1.9, 2.7), 1.4 (1.2, 1.6), 6.0 (4.6, 7.8) and 1.7 (1.4, 2.0) times higher (p-trend <0.001) concentrations of total arsenic, DMA, arsenobetaine and total arsenic minus arsenobetaine, respectively. In participants without detectable arsenobetaine and in analyses adjusted for arsenobetaine, seafood consumption in the past year was not associated with total arsenic or DMA concentrations in urine.Seafood intake was a major determinant of increased urine concentrations of total arsenic, DMA, arsenobetaine and total arsenic minus arsenobetaine in the US population. Epidemiologic studies that use total arsenic, DMA, the sum of inorganic arsenic, methylarsonate and DMA, and total arsenic minus arsenobetaine as markers of inorganic arsenic exposure and/or metabolism need to address seafood intake.
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Project description:Arsenic (As) species analysis is important for the risk evaluation of seafood. Until now, there has been limited information on the change of As species during digestion. Here, the As species in different types of seafood before and after in vitro digestion were investigated. Although inorganic As was not detected in digested fish samples, As(V) contents in digested crabs and scallops were 17.12 ± 1.76 and 138.69 ± 7.53, respectively, which were approximately 2-3 times greater than those of the pre-digestion samples. In further experiments, arsenocholine, dimethylarsinate, arsenobetaine, and monomethylarsonate were all convertible to As(V) during in vitro digestions with different rates. The transformation demonstrates a complex process and could be affected by many factors, such as pH, time, and digestion juice composition, of which pH seemed to be particularly important. Free radicals were responsible for the oxidation in the transformation reactions. Unlike arsenobetaine, arsenocholine seemed to be able to directly transform to monomethylarsonate without the intermediate dimethylarsinate. This study reveals and validates the potential of other species (oAs or/and unknown species) to convert to iAs, identifies the main factors affecting this process, and proposes a reaction pathway. There is an important implication for promoting a more accurate risk assessment of arsenic in foodstuffs.
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Project description:Inorganic arsenic (i-As) has been related to wide-ranging health effects in children, leading to lifelong concerns. Proportionally, dietary i-As exposure dominates in regions with low arsenic drinking water. This study aims to investigate the relation between rice and seafood consumption and urinary arsenic species during childhood and to assess the proportion of urinary i-As metabolites. Urinary arsenic species concentration in 400 4-year-old children living in four geographical areas of Spain, in addition to repeated measures from 100 children at 7 years of age are included in this study. Rice and seafood products intake was collected from children's parents using a validated food frequency questionnaire (FFQ). At 4 years of age, children's urine i-As and monomethylarsonic acid (MMA) concentrations increased with rice product consumption (p-value = 0.010 and 0.018, respectively), and urinary arsenobetaine (AsB) with seafood consumption (p = 0.002). Four-year-old children had a higher consumption of both rice and seafood per body weight and a higher urinary %MMA (p-value = 0.001) and lower % dimethylarsinic acid (DMA) (p-value = 0.017). This study suggests increased dietary i-As exposure related to rice product consumption among children living in Spain, and the younger ones may be especially vulnerable to the health impacts of this exposure also considering that they might have a lower i-As methylation capacity than older children. In contrast, seafood consumption did not appear to influence the presence of potentially toxic arsenic species in this population of children.
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Project description:A dietary supplement, kelp contains a significant amount of arsenic that is mostly arsenosugars. The determination of arsenosugars is difficult due to a lack of arsenosugar calibration standard, because arsenosugar compounds are not commercially available. This work reports the determination of arsenicals in a kelp extract with traceability to the International System of Units (SI). The hydrophilic fraction of arsenicals was reproducibly extracted from a candidate Standard Reference Material (SRM) 3232 Kelp Powder (Thallus Laminariae) in development at the National Institute of Standards and Technology (NIST). Arsenosugars and dimethylarsinic acid (DMA) were separated into fractions using analytical liquid chromatography (LC) cation and anion columns. The arsenic in the fractions was determined using instrumental neutron activation analysis (INAA). Cation exchange separation was used for INAA determination of arsenosugar 3-[5'-deoxy-5'-(dimethylarsinoyl)-?-ribofuranosyloxy]propylene glycol (As(328)) for the first time, while DMA, arsenosugars 3-[5'-deoxy-5'-(dimethylarsinoyl)-?-ribofuranosyloxy]-2-hydroxypropyl 2,3-dihydroxypropyl hydrogen phosphate (As(482)), and 3-[5'-deoxy-5'-(dimethylarsinoyl)-?-ribofuranosyloxy]-2-hydroxypropanesulfonic acid (As(392)) were determined following anion exchange separation. The contents of DMA, As(328), As(482), and As(392) were 0.41 mg kg-1 ± 0.09 mg kg-1, 1.10 mg kg-1 ± 0.25 mg kg-1, 5.23 mg kg-1 ± 0.46 mg kg-1, and 13.17 mg kg-1 ± 0.67 mg kg-1, respectively. Separately, components of arsenic species in the kelp extract including DMA, As(328), and inorganic arsenic were determined using LC-inductively coupled plasma mass spectrometry. Results of DMA and As(328) were 0.485 mg kg-1 ± 0.024 mg kg-1 and 1.14 mg kg-1 ± 0.03 mg kg-1, respectively, which were in good agreement with those determined by INAA in fractions of LC eluent. The most toxic species, AsIII and AsV were found to be < 0.07 mg kg-1 and 0.231 mg kg-1 ± 0.018 mg kg-1, respectively. Results were traceable to SI.
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Project description:Insight into the mechanisms for arsenic detoxification by Geobacter species is expected to improve the understanding of global cycling of arsenic in iron-rich subsurface sedimentary environments. Analysis of 14 different Geobacter genomes showed that all of these species have genes coding for an arsenic detoxification system (ars operon), and several have genes required for arsenic respiration (arr operon) and methylation (arsM). Genes encoding four arsenic repressor-like proteins were detected in the genome of G. sulfurreducens; however, only one (ArsR1) regulated transcription of the ars operon. Elimination of arsR1 from the G. sulfurreducens chromosome resulted in enhanced transcription of genes coding for the arsenic efflux pump (Acr3) and arsenate reductase (ArsC). When the gene coding for Acr3 was deleted, cells were not able to grow in the presence of either the oxidized or reduced form of arsenic, while arsC deletion mutants could grow in the presence of arsenite but not arsenate. These studies shed light on how Geobacter influences arsenic mobility in anoxic sediments and may help us develop methods to remediate arsenic contamination in the subsurface.This study examines arsenic transformation mechanisms utilized by Geobacter, a genus of iron-reducing bacteria that are predominant in many anoxic iron-rich subsurface environments. Geobacter species play a major role in microbially mediated arsenic release from metal hydroxides in the subsurface. This release raises arsenic concentrations in drinking water to levels that are high enough to cause major health problems. Therefore, information obtained from studies of Geobacter should shed light on arsenic cycling in iron-rich subsurface sedimentary environments, which may help reduce arsenic-associated illnesses. These studies should also help in the development of biosensors that can be used to detect arsenic contaminants in anoxic subsurface environments. We examined 14 different Geobacter genomes and found that all of these species possess genes coding for an arsenic detoxification system (ars operon), and some also have genes required for arsenic respiration (arr operon) and arsenic methylation (arsM).
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Project description:Robust and sensitive methods for monitoring inorganic and organic As species As(III), As(V), dimethylarsinate (DMA), and monomethylarsonate (MMA) in environmental water are necessary to understand the toxicity and redox processes of As in a specific environment. The method is sufficiently sensitive and selective to ensure accurate and precise quantitation of As(III), As(V), DMA, and MMA in surface water and groundwater samples with As species concentrations from tens of nanograms per liter to 50 µg/L without dilution of the sample. Mean recoveries of the four species spiked into reagent water, surface water and groundwater and measured periodically over three months ranged from 87.2 % to 108.7 % and relative standard deviation of replicates of all analytes ranged from 1.1 % to 9.0 %.•A PRP-X100 column and nitrate/phosphate mobile phase was used to separate As(III), As(V), DMA, and MMA in 0.45 µm filtered surface water and groundwater matrices.•Oxygen was used in the collision cell of the inductively coupled plasma-mass spectrometer with MS/MS mode to shift the measured As mass from 75 to 91.•The analytical performance of the method and figures of merit including detection limits, precision, accuracy, and interferences when applied to surface water and groundwater matrices were investigated.
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Project description:The sum of urinary inorganic arsenic (iAs) and methylated arsenic (monomethylarsonate and dimethylarsinate (DMA)) species is the main biomarker of iAs exposure. Assessing iAs exposure, however, is difficult in populations with moderate-to-high seafood intakes. In the present study, we used subsamples from the Multi-Ethnic Study of Atherosclerosis (2000-2002) (n = 310) and the 2003-2006 National Health and Nutrition Examination Survey (n = 1,175). We calibrated urinary concentrations of non-seafood-derived iAs, DMA, and methylarsonate, as well as the sum of inorganic and methylated arsenic species, in the Multi-Ethnic Study of Atherosclerosis and of DMA in the National Health and Nutrition Examination Survey by regressing their original concentrations by arsenobetaine and extracting model residuals. To confirm that calibrated biomarkers reflected iAs exposure but not seafood intake, we compared urinary arsenic concentrations by levels of seafood and rice intakes. Self-reported seafood intakes, estimated n-3 polyunsaturated fatty acid levels, and measured n-3 polyunsaturated fatty acid levels were positively associated with the original urinary arsenic biomarkers. Using the calibrated arsenic biomarkers, we found a marked attenuation of the associations with self-reported seafood intake and estimated or measured n-3 fatty acids, whereas associations with self-reported rice intake remained similar. Our residual-based method provides estimates of iAs exposure and metabolism for each participant that no longer reflect seafood intake and can facilitate research about low-to-moderate levels of iAs exposure in populations with high seafood intakes.
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Project description:Toxic elements (Cd, Pb, and As) accumulate into the environment by industrialization and natural phenomena and then pass to organisms. Analysis of toxic elements in food must be accurately carried out on a regular basis so as to avoid any adverse impact. Salted foods are difficult samples and accurate analysis of As is not easy due to salt interference. In this study, analysis of As was carried without influence of salts in three types of salted foods via an analytical method, which was validated using spiking recovery experiments and by analyzing certified reference materials. As a result, toxic elements were detected in all samples but none of these exceeded the World Health Organization recommended limits. Among the As species, arsenobetaine (AsB) was the most abundant, while inorganic As was below the detection limit in all samples. All the analyzed salted food samples appeared to be safe for consumption. In addition, the analysis of sea shrimp, freshwater shrimp, and seawater verified As bioaccumulation in these organisms from the environment.
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Project description:Low temperature treatments commonly applied to seafood products have been shown to influence their phospholipid (PL) profile through enzymatic hydrolysis. In the present study, the generation of lysophospholipids (LPL) resulting from this process was systematically investigated for selected, commercially relevant seafood products, namely oysters, clams, octopuses, and shrimps. These products were subjected to thermal treatments like refrigeration or freezing after being purchased as fresh, defrozen, or frozen products depending on the case. The coupling between hydrophilic interaction liquid chromatography (HILIC) and electrospray ionization with high resolution/accuracy Fourier transform mass spectrometry (ESI-FTMS) was exploited to evaluate the PL profile of the cited products, especially the incidence of LPL related to the two main PL classes of seafood products-phosphatidylcholines (PC) and phosphatidylethanolamines (PE)-in the lipid extracts. The lyso forms of PE (LPE) were found to be generally more sensitive than those of PC (LPC) to thermal treatments, usually exhibiting a significant increase upon prolonged refrigeration at 4 °C in all types of investigated products except European flat oysters. Moreover, the distinction between fresh and frozen or defrozen products could be achieved in the case of octopuses and shrimps, respectively.
| S-EPMC6225239 | biostudies-literature
Project description:The large disparity between arsenic concentrations in drinking water and urine remains unexplained. This study aims to evaluate predictors of urinary arsenic in a population exposed to low concentrations (≤50 μg/l) of arsenic in drinking water. Urine and drinking water samples were collected from a subsample (n=343) of a population enrolled in a bladder cancer case-control study in southeastern Michigan. Total arsenic in water and arsenic species in urine were determined using ICP-MS: arsenobetaine (AsB), arsenite (As[III]), arsenate (As[V]), methylarsenic acid (MMA[V]), and dimethylarsenic acid (DMA[V]). The sum of As[III], As[V], MMA[V], and DMA[V] was denoted as SumAs. Dietary information was obtained through a self-reported food intake questionnaire. Log(10)-transformed drinking water arsenic concentration at home was a significant (P<0.0001) predictor of SumAs (R(2)=0.18). Associations improved (R(2)=0.29, P<0.0001) when individuals with less than 1 μg/l of arsenic in drinking water were removed and further improved when analyses were applied to individuals who consumed amounts of home drinking water above the median volume (R(2)=0.40, P<0.0001). A separate analysis indicated that AsB and DMA[V] were significantly correlated with fish and shellfish consumption, which may suggest that seafood intake influences DMA[V] excretion. The Spearman correlation between arsenic concentration in toenails and SumAs was 0.36 and between arsenic concentration in toenails and arsenic concentration in water was 0.42. Results show that arsenic exposure from drinking water consumption is an important determinant of urinary arsenic concentrations, even in a population exposed to relatively low levels of arsenic in drinking water, and suggest that seafood intake may influence urinary DMA[V] concentrations.
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