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Arsenic exposure can perturb gut microbiota and their metabolic functions. We exposed C57BL/6 mice to 1 ppm arsenic in drinking water and investigated whether arsenic exposure affects the homeostasis of bile acids, a group of key microbiome-regulated signaling molecules of microbiome-host interactions. We found that arsenic exposure differentially changed major unconjugated primary bile acids and consistently decreased secondary bile acids in the serum and liver. The relative abundance of Bacteroidetes and Firmicutes was associated with the bile acid level in serum. This study demonstrates that arsenic-induced gut microbiota dysbiosis may play a role in arsenic-perturbed bile acid homeostasis.

This study aims at making a comprehensive assessment of the impact of land use and the hydrogeological properties on groundwater quality. First, factor analysis (FA) is applied to reveal the main pollutant sources and hydrogeological processes controlling the groundwater quality. FA identifies the four most important factors. Factor 1 (seawater salinization) is characterized by a medium loading of land use type of aquaculture. It is recognized that the high scores for factor 1 in coastal areas are due to over-pumping from aquafarms. Focused land use management is required to prevent saline-water intrusion in coastal aquifers. Factor 3 (nitrate pollution) shows high correlations with the land use type of fruit farming and the gravel thickness in unsaturated layers. High scores for factor 3 are also found in the proximal area of the Chuoshui River Alluvial Fan and the northeastern mountain area in the Pingtung Plain. Fruit farmers should be educated to reduce the application of fertilizers and promote the organic fruit farming. The impacts of land use and the hydrogeological properties on both Factor 2 (arsenic enrichment) and Factor 4 (reductive dissolution of Fe 2+ and Mn 2+ ) are negligible. Second, cluster analysis (CA) is performed on computed scores of the four main factors to separates 123 monitoring wells into cluster 1 (low polluted zone), cluster 2 (nitrate polluted zone) and cluster 3 (hybrid polluted zone). The results obtained from CA provide practical applications such as reduce agrichemical use in the areas of cluster 2 and enforce intensive monitoring in the prioritizing areas of cluster 3. This study successively uses the FA and CA to extract the meaningful information present by geographical visualization of scores for 4 main factors and 3 distinct clusters zones. The results are essential for formulating sound groundwater resource and land use management policies to ensure groundwater sustainability., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Background: Arsenic-induced liver X receptor/retinoid X receptor (LXR/RXR) signaling inhibition is a potential mechanism underlying the cardiovascular effects caused by arsenic. The gut microbiota can influence arsenic toxic effects., Objective: We aimed to explore whether gut microbiota play a role in arsenic-induced LXR/RXR signaling inhibition and the subsequent lipid and cholesterol dysbiosis., Methods: Conventional and antibiotic-treated mice (AB-treated mice) were exposed to 0.25   ppm and 1   ppm arsenic for 2 wk. Hepatic mRNAs were extracted and sequenced. The expression levels of genes associated with LXR/RXR signaling were quantified by quantitative real-time polymerase chain reaction (qPCR), and serum and hepatic cholesterol levels were measured. Liquid chromatography-mass spectrometry (LC-MS)-based lipidomics were used to examine serum and hepatic lipids., Results: Pathway analysis indicated that arsenic exposure differentially influenced the hepatic signaling pathways in conventional and AB-treated mice. The expression of sterol regulatory element-binding protein 1 ( Srebp1c ), 3-hydroxy-3-methylglutaryl-CoA reductase ( Hmgcr ), and cytochrome P450 family 7 subfamily A member 1 ( Cyp7a1 ), as well as cholesterol efflux genes, including ATP binding cassette subfamily G member 5/8 ( Abcg5/8 ) and cluster of differentiation 36 ( Cd36 ), was lower in arsenic-exposed conventional mice but not in AB-treated mice. Similarly, under arsenic exposure, the hepatic expression of scavenger receptor class B member 1 ( Scarb1 ), which is involved in reverse cholesterol transport (RCT), was lower in conventional mice, but was higher in AB-treated animals compared with controls. Correspondingly, arsenic exposure exerted opposite effects on the serum cholesterol levels in conventional and AB-treated mice, i.e., higher serum cholesterol levels in conventional mice but lower levels in AB-treated mice than in respective controls. Serum lipid levels, especially triglyceride (TG) levels, were higher in conventional mice exposed to 1   ppm arsenic, while arsenic exposure did not significantly affect the serum lipids in AB-treated mice. Liver lipid patterns were also differentially perturbed in a microbiota-dependent manner., Conclusions: Our results suggest that in mice, the gut microbiota may be a critical factor regulating arsenic-induced LXR/RXR signaling perturbation, suggesting that modulation of the gut microbiota might be an intervention strategy to reduce the toxic effects of arsenic on lipid and cholesterol homeostasis. https://doi.org/10.1289/EHP4415.

Chronic arsenic exposure from drinking water is a global public health issue, which is associated with numerous human diseases and influences millions of people worldwide. The effects of arsenic exposure to the metabolic networks remain elusive. Here, we exposed female C57BL/6J mice to 1 ppm inorganic arsenic in drinking water for 3 months to investigate how arsenic exposure perturbs serum and fecal metabolic profiles. We found decreased levels of serum compounds with antioxidative activities in arsenic-treated mice, in accordance with elevated oxidative stress indicated by higher urinary 8-oxo-2'-deoxyguanosine (8-oxo-dG) levels. Moreover, the levels of multiple lysophosphatidylcholines (lysoPCs) were significantly increased in the sera of arsenic-exposed mice, including lysoPC (O-18:0), lysoPC (20:3), lysoPC (18:1), and lysoPC (22:6). Arsenic exposure perturbed the levels of several key polyunsaturated fatty acids (PUFAs) in the fecal samples in concert with alterations in related microbial pathways. Additionally, changes in the abundances of many functional metabolites, together with decreased levels of amino acids, were found in the fecal samples of arsenic-treated mice. By delineating the impact of arsenic exposure on the metabolic profiles, the findings may provide new biomarkers and mechanistic insights into arsenic-associated diseases.

The movement of high-arsenic (As)-concentration Beitou geothermal spring water up to 4600 μg/L from the upstream area may affect the downstream Guandu plain and Guandu wetland. The major As pathway is via the subsurface flow. The study assesses the fate and transport of As-enriched geothermal spring water in the Beitou-Guandu area. The groundwater head and flow field velocity are first simulated by using HYDROGEOCHEM-fluid flow model. The steady state flow field is well-calibrated with root mean square error 1.73 m and R 2  = 0.992. The spatial-temporal distributions of As in the Beitou-Guandu area are simulated by the HYDROGEOCHEM reactive transport model using the calibrated steady state flow field. The results show that high As concentration (250 μg/L) in groundwater of Guandu plain was caused by the movement of high As concentration from the Beitou geothermal spring water. In contrast, the low As concentration (5-50 μg/L) in Guandu wetland was mitigated by the tidal water dilution. The simulated As concentrations increase in the first 3 years, and then gradually decrease due to the adsorption of As on the iron oxide minerals ferrihydrite and iron sulfide minerals pyrite. Furthermore, the hydrogeochemical transport model is applied to assess the effect of bioaccumulation of As by the mangrove plants of Guandu wetland. The dominant mangrove plants, Kandelia obovata, can reduce about 5-30 μg/L As concentration in groundwater. It may be one of sinks of As in Guandu wetland. The inclusion of K. obovata can uptake the aqueous As and allow the simulated As concentration further close to the field measurement in the Guandu wetland. The study successfully models the reactive chemical transport of As by considering both geochemical reactions and biochemical uptakes in the Beitou-Guandu area. The result demonstrates that the complex biogeochemical transport can be quantified by the sophisticated HYDROGEOCHEM model. Moreover, the salient features of the biogeochemical reactions can be recovered and elucidated through a series of systematic simulation.

Quantitative metaproteomics is a relatively new research field that applies proteomics techniques to study microbial proteins of the microbiome and holds great potential in truly quantifying the functional proteins actually expressed by microbes in the biological environment, such as the gastrointestinal tract. The significant association between arsenic exposure and gut microbiome perturbations has been reported; however, metaproteomics has not yet been applied to study arsenic-induced proteome changes of the microbiome. Most importantly, to our knowledge, isobaric-labeling-based large-scale metaproteomics has not been reported using the advanced database-search approaches such as MetaPro-IQ and matched metagenome database-search strategies to provide high quantification accuracy and fewer missing quantification values. In the present study, a new experimental workflow coupled to isobaric labeling and MetaPro-IQ was demonstrated for the metaproteomics study of arsenic-induced gut microbiome perturbations. The advantages of this workflow were also discussed. For all 18 fecal samples analyzed, 7611 protein groups were quantified without any missing values. The consistent results of expression profiles were observed between 16S rRNA gene sequencing and metaproteomics. This isobaric-labeling-based workflow demonstrated the significant improvement of quantitative metaproteomics for gut microbiome study.

Arsenic contamination in drinking water has been a worldwide health concern for decades. In addition to being a well-recognized carcinogen, arsenic exposure has also been linked to diabetes, neurological effects, and cardiovascular diseases. Recently, increasing evidence has indicated that gut microbiome is an important risk factor in modulating the development of diseases. We aim to investigate the role of gut microbiome perturbation in arsenic-induced diseases by coupling a mass-spectrometry-based metabolomics approach and an animal model with altered gut microbiome induced by bacterial infection. Serum metabolic profiling has revealed that gut microbiome perturbation and arsenic exposure induced the dramatic changes of numerous metabolite pathways, including fatty acid metabolism, phospholipids, sphingolipids, cholesterols, and tryptophan metabolism, which were not or were less disrupted when the gut microbiome stayed normal. In summary, this study suggests that gut microbiome perturbation can exacerbate or cause metabolic disorders induced by arsenic exposure.

Arsenic (As) contamination in water or food is a global issue affecting hundreds of millions of people. Although As is classified as a group 1 carcinogen and is associated with multiple diseases, the individual susceptibility to As-related diseases is highly variable, such that a proportion of people exposed to As have higher risks of developing related disorders. Many factors have been found to be associated with As susceptibility. One of the main sources of the variability found in As susceptibility is the variation in the host genome, namely, polymorphisms of many genes involved in As transportation, biotransformation, oxidative stress response, and DNA repair affect the susceptibility of an individual to As toxicity and then influence the disease outcomes. In addition, lifestyles and many nutritional factors, such as folate, vitamin C, and fruit, have been found to be associated with individual susceptibility to As-related diseases. Recently, the interactions between As exposure and the gut microbiome have been of particular concern. As exposure has been shown to perturb gut microbiome composition, and the gut microbiota has been shown to also influence As metabolism, which raises the question of whether the highly diverse gut microbiota contributes to As susceptibility. Here, we review the literature and summarize the factors, such as host genetics and nutritional status, that influence As susceptibility, and we also present potential mechanisms of how the gut microbiome may influence As metabolism and its toxic effects on the host to induce variations in As susceptibility. Challenges and future directions are also discussed to emphasize the importance of characterizing the specific role of these factors in interindividual susceptibility to As-related diseases.

High concentrations of naturally occurring arsenic (As) are typically found in young alluvial and deltaic deposits, and high concentrations of ammonium (NH 4 + ) and nitrate (NO 3 - ) are often present in groundwater affected by anthropogenic activities. In this study, on the basis of physicochemical characteristics of groundwater and the nitrogen and oxygen isotope composition of NO 3 - , it was inferred that the main sources of NO 3 - in the proximal fan of the Choushui River alluvial fan are likely to be ammonium fertilizers, manure, and septic waste; that in the mid-fan and the distal fan, the possible sources are nitrate fertilizers and marine nitrate. In the proximal fan, the oxidative state obviously promotes microbial nitrification. Denitrification occurs from the upstream region to the downstream region of the Choushui River, and therefore, the decrease in NO 3 - concentration along streams connecting the Choushui River to the ocean appears plausible. High DO concentrations and relatively low values of δ 18 O NO3 in the deeper aquifer of the proximal fan may be attributed to unconfined granular nature and groundwater pumping by agricultural activities. In the mid-fan, NO 3 - assimilation is the dominant response to NO 3 - attenuation, and denitrification is insignificant; however, high concentrations of As, NH4 + and Fe and depletion of δ 15 N NO3 imply the occurrence of feammox process. By contrast, denitrification evidently occurs in the distal fan, through assimilation, mineralization, and dissimilatory NO 3 - reduction to NH 4 + , resulting in depletion of NO 3 - and increase in NH 4 + in groundwater. Feammox in the mid-fan and denitrification in the distal fan may be the main processes leading to the release of As from As-bearing Fe oxyhydroxides into groundwater., (Copyright © 2016 Elsevier B.V. All rights reserved.)

This study involved assessing and simulating the probable major pathways (surface and subsurface flow) and hydrogeochemical transport of arsenic (As) in the Beitou-Guandu area, Taiwan. A one-dimensional (1-D) generic, reactive, chemical transport model (PHREEQC) was adopted. The calibrated model showed that As transported to the downstream Guandu plain and Tan Shui river mouth accounted for 50.7 and approximately 100 % of the As in the subsurface flow pathway, respectively, suggesting that subsurface flow constituted a major As pathway. The highest As water concentration occurred near the Beitou geothermal valley because of the low pH and high redox potential in both the surface and subsurface pathways. However, As may be scavenged by aqueous Fe(II) in a reducing environment. The As concentrations in the downstream Guandu plain and Guandu wetland decreased as the simulated time increased, resulting in the adsorption of As on the surface of Fe oxydroxides and limiting the mobility of As in the surface flow pathway. The major retardation mechanism of As mobility in the subsurface flow pathway of the Guandu plain and Guandu wetland was governed by the adsorption reactions of iron-oxide and iron-sulfide minerals. The 1-D transport model was applied to predict the evolution of As in the subsurface flow pathway from 2013 to 2020. The results indicated that the As concentrations in all cells gradually increased. The geochemical redox reactions of As in the subsurface pathway subsequently led to the oxidization of As-bearing sulfides, causing As concentrations to rise substantially in the hillside area.

We propose a systematical approach to assessing arsenic concentration in a river through: important factor extraction by a nonlinear factor analysis; arsenic concentration estimation by the neuro-fuzzy network; and impact assessment of important factors on arsenic concentration by the membership degrees of the constructed neuro-fuzzy network. The arsenic-contaminated Huang Gang Creek in northern Taiwan is used as a study case. Results indicate that rainfall, nitrite nitrogen and temperature are important factors and the proposed estimation model (ANFIS(GT)) is superior to the two comparative models, in which 50% and 52% improvements in RMSE are made over ANFIS(CC) and ANFIS(all), respectively. Results reveal that arsenic concentration reaches the highest in an environment of lower temperature, higher nitrite nitrogen concentration and larger one-month antecedent rainfall; while it reaches the lowest in an environment of higher temperature, lower nitrite nitrogen concentration and smaller one-month antecedent rainfall. It is noted that these three selected factors are easy-to-collect. We demonstrate that the proposed methodology is a useful and effective methodology, which can be adapted to other similar settings to reliably model water quality based on parameters of interest and/or study areas of interest for universal usage. The proposed methodology gives a quick and reliable way to estimate arsenic concentration, which makes good contribution to water environment management., (Copyright © 2014 Elsevier B.V. All rights reserved.)

Groundwater is a major water resource in Southwestern Taiwan; hence, long-term monitoring of water quality is essential. The study aims to assess the hydrochemical characteristics of water in the arsenic-contaminated aquifers of Choushui River alluvial fan and Chianan Plain, Taiwan using multivariate statistical methods, namely, factor analysis (FA), cluster analysis (CA), and discriminant analysis (DA). Factor analysis is applied to reveal the processes controlling the hydrochemistry of groundwater. Cluster analysis is applied to spatially categorize the collected water samples based on the water quality. Discriminant analysis is then applied to elucidate key parameters associated with the occurrence of elevated As concentration (>10 μg L(-1)) in groundwater. Major water types are characterized as Na-Ca-Cl and Na-Mg-Cl in the Choushui River alluvial fan and Chianan Plain, respectively. Inorganic species of arsenic (As), particularly As(III), prevail in these two groundwater catchments, and their levels are higher in the Chianan Plain than in the Choushui River alluvial fan. Through FA, three factors, namely, the degree of salination, As reduction, and iron (Fe) reduction, are determined and denoted irrespective of some differences between the factorial compositions. Spatial distribution patterns of factors As reduction and Fe reduction imply that the redox zonation is delineated by As- and Fe-dominance zones separately. The results of CA demonstrate that three main groups can be properly explained by the factors extracted via FA. Three- (Fe(2+), Fe(3+), and NH (4) (+) ) and four-parameters (Fe(2+), Fe(3+), NH (4) (+) , and Ca(2+)) derived from discriminant analysis for Choushui River alluvial fan and Chianan Plain are elucidated as key parameters affecting the distribution of As-contained groundwater. The analytical results indicate that the reductive dissolution of Fe minerals is prerequisite for the mobilization of As, whereas the shift of redox condition from Fe- to As-reducing leads to the accumulation of dissolved As in this area.

High arsenic (As) concentration in groundwater potentially poses a serious threat to the health of local residents in southwestern Taiwan. Although the As release to groundwater is responsible for the reducing bacteria-mediated reductive dissolution of As-rich Fe hydroxides, the influences of FeRB and different organic substrates on As and Fe mobility and transformation were rarely discussed. An experiment that involved As-adsorbed synthetic amorphous Fe(III) hydroxide (HFO) and the inoculation of in situ Fe-reducing bacteria (FeRB) was performed to evaluate the contribution of FeRB to the As mobility and transformation. The batched experiment of As-free HFO showed that the reducing bacteria rapidly induced the reduction of amorphous Fe oxyhydroxide to Fe(II) by reductive dissolution of HFO and formation of Fe-citrate complexation. For aqueous As(V) reduction experiment, arsenate was effectively reduced to As(III) by the facultative anaerobic bacterium in the cultured FeRB. In the experiment of As-containing HFO reduction, the aqueous As(V) acts as an electron acceptor and reduced to As(III) after the reductive dissolution of Fe(III) on HFO. However, the increase in the As(III) concentrations with time for various organic substrates in the As-adsorbed HFO-reducing experiment differ from the rates of As(V) reduction with various organic substrates in the As(V)-reducing experiment. The decrease in sorption sites by coupled reductive dissolution of HFO and the competitive desorption of small molecular organic carbon is apparently the important factor of As mobility. For large molecular organic carbon (i.e., citrate), the significant contribution of citrate on As mobility is the complexation of iron citrate. A working hypothesis model of As biogeochemical cycling is proposed to illustrate the relevant processes in the groundwater aquitard of southwestern Taiwan.

Many regions of Latin America are widely reported for the occurrence of high arsenic (As) in groundwater and surface water due to a combination of geological processes and/or anthropogenic activities. In this paper, we review the available literature (both in English and Spanish languages) to delineate human As exposure pathways through the food chain. Numerous studies show that As accumulations in edible plants and crops are mainly associated with the presence of high As in soils and irrigation waters. However, factors such as As speciation, type and composition of soil, and plant species have a major control on the amount of As uptake. Areas of high As concentrations in surface water and groundwater show high As accumulations in plants, fish/shellfish, livestock meat, milk and cheese. Such elevated As concentrations in food may result in widespread health risks to local inhabitants, including health of indigenous populations and residents living close to mining industries. Some studies show that As can be transferred from the water to prepared meals, thereby magnifying the As content in the human diet. Arsenic speciation might also change during food preparation, especially during high temperature cooking, such as grilling and frying. Finally, the review of the available literature demonstrates the necessity of more rigorous studies in evaluating pathways of As exposure through the human food chain in Latin America., (Copyright © 2011 Elsevier B.V. All rights reserved.)

The global impact on public health of elevated arsenic (As) in water supplies is highlighted by an increasing number of countries worldwide reporting high As concentrations in drinking water. In Latin America, the problem of As contamination in water is known in 14 out of 20 countries: Argentina, Bolivia, Brazil, Chile, Colombia, Cuba, Ecuador, El Salvador, Guatemala, Honduras, Mexico, Nicaragua, Peru and Uruguay. Considering the 10 μg/L limit for As in drinking water established by international and several national agencies, the number of exposed people is estimated to be about 14 million. Health effects of As exposure were identified for the first time already in the 1910s in Bellville (Córdoba province, Argentina). Nevertheless, contamination of As in waters has been detected in 10 Latin American countries only within the last 10 to 15 years. Arsenic is mobilized predominantly from young volcanic rocks and their weathering products. In alluvial aquifers, which are water sources frequently used for water supply, desorption of As from metal oxyhydroxides at high pH (>8) is the predominant mobility control; redox conditions are moderate reducing to oxidizing and As(V) is the predominant species. In the Andes, the Middle American cordillera and the Transmexican Volcanic Belt, oxidation of sulfide minerals is the primary As mobilization process. Rivers that originate in the Andean mountains, transport As to more densely populated areas in the lowlands (e.g. Rímac river in Peru, Pilcomayo river in Bolivia/Argentina/Paraguay). In many parts of Latin America, As often occurs together with F and B; in the Chaco-Pampean plain As is found additionally with V, Mo and U whereas in areas with sulfide ore deposits As often occurs together with heavy metals. These co-occurrences and the anthropogenic activities in mining areas that enhance the mobilization of As and other pollutants make more dramatic the environmental problem., (Copyright © 2011 Elsevier B.V. All rights reserved.)

High levels of arsenic in groundwater and drinking water represent a major health problem worldwide. Drinking arsenic-contaminated groundwater is a likely cause of blackfoot disease (BFD) in Taiwan, but mechanisms controlling the mobilization of arsenic present at elevated concentrations within aquifers remain understudied. Microcosm experiments using sediments from arsenic contaminated shallow alluvial aquifers in the blackfoot disease endemic area showed simultaneous microbial reduction of Fe(III) and As(V). Significant soluble Fe(II) (0.23±0.03 mM) in pore waters and mobilization of As(III) (206.7±21.2 nM) occurred during the first week. Aqueous Fe(II) and As(III) respectively reached concentrations of 0.27±0.01 mM and 571.4±63.3 nM after 8 weeks. We also showed that the addition of acetate caused a further increase in aqueous Fe(II) but the dissolved arsenic did not increase. We further isolated an As(V)-reducing bacterium native to aquifer sediments which showed that the direct enzymatic reduction of As(V) to the potentially more-soluble As(III) in pore water is possible in this aquifer. Our results provide evidence that microorganisms can mediate the release of sedimentary arsenic to groundwater in this region and the capacity for arsenic release was not limited by the availability of electron donors in the sediments., (Copyright © 2011 Elsevier B.V. All rights reserved.)

Arsenic (As) contamination of groundwater, accompanied by critical salinization, occurs in the southwestern coastal area of Taiwan. Statistical analyses and geochemical calculations indicate that a possible source of aqueous arsenic is the reductive dissolution of As-bearing iron oxyhydroxides. There are few reports of the influence of sulfate-sulfide redox cycling on arsenic mobility in brackish groundwater. We evaluated the contribution of sulfate reduction and sulfide re-oxidation on As enrichment using δ(34)S([SO(4)]) and δ(18)O([SO(4)]) sulfur isotopic analyses of groundwater. Fifty-three groundwater samples were divided into groups of high-As content and salinized (Type A), low-As and non-salinized (Type B), and high-As and non-salinized (Type C) groundwaters, based on hydro-geochemical analysis. The relatively high enrichment of (34)S([SO(4)]) and (18)O([SO(4)]) present in Type A, caused by microbial-mediated reduction of sulfate, and high (18)O enrichment factor (ε([SO(4)-H(2)O])), suggests that sulfur disproportionation is an important process during the reductive dissolution of As-containing iron oxyhydroxides. Limited co-precipitation of ion-sulfide increased the rate of As liberation under anaerobic conditions. In contrast to this, Type B and Type C groundwater samples showed high δ(18)O([SO(4)]) and low δ(34)S([SO(4)]) values under mildly reducing conditions. Base on (18)O mass balance calculations, the oxide sources of sulfate are from infiltrated atmospheric O(2), caused by additional recharge of dissolved oxygen and sulfide re-oxidation. The anthropogenic influence of extensive pumping also promotes atmospheric oxygen entry into aquifers, altering redox conditions, and increasing the rate of As release into groundwater., (Copyright © 2011 Elsevier B.V. All rights reserved.)

This paper assesses health risks due to the ingestion of inorganic arsenic from fish and shellfish farmed in blackfoot disease areas by general public in Taiwan. The provisional tolerable weekly intake of arsenic set by FAO/WHO and the target cancer risk assessment model proposed by USEPA were integrated to evaluate the acceptable consumption rate. Five aquacultural species, tilapia (Oreochromis mossambicus), milkfish (Chanos chanos), mullet (Mugil cephalus), clam (Meretrix lusoria) and oyster (Crassostrea gigas) were included. Monte Carlo analysis was used to propagate the parameter uncertainty and to probabilistically assess the health risk associated with the daily intake of inorganic As from farmed fish and shellfish. The integrated risk-based analysis indicates that the associated 50th and 95th percentile health risk are 2.06×10(-5) and 8.77×10(-5), respectively. Moreover, the acceptable intakes of inorganic As are defined and illustrated by a two dimensional graphical model. According to the relationship between C(inorg) and IR(f) derived from this study, two risk-based curves are constructed. An acceptable risk zone is determined (risk ranging from 1×10(-5) to 6.07×10(-5)) which is recommended for acceptable consumption rates of fish and shellfish. To manage the health risk due to the ingestion of inorganic As from fish and shellfish in BFD areas, a risk-based management scheme is derived which provide a convenient way for general public to self-determine the acceptable seafood consumption rate., (Copyright © 2010 Elsevier B.V. All rights reserved.)

Redox couples approach and multivariate statistical techniques, including factor analysis, cluster analysis and discriminant analysis, were applied to evaluate and to interpret the complex groundwater quality in the blackfoot disease endemic area, Taiwan. Most groundwater samples were characterized as Na-Ca-HCO(3) with HCO(3)(-) as the dominant anion. Total arsenic (As) concentration, predominantly as As(3+), ranged from <1.0 to 562.7 μg/L. The patterns of measured reducing potential were consistent with those values calculated from As couple, revealing the in situ environment enhanced the accumulation of As concentration in the groundwater. Factor analysis proposed a four-factor model, comprising salination, reductive dissolution of Fe/Mn oxyhydroxides, As reduction and chemical potential factor, and explained 89.94% of total variance in groundwater. Furthermore, two factors, reductive dissolution of Fe/Mn oxyhydroxides and As reduction, suggested that the decoupled reductive processes accounted for high As concentration in this area. Cluster analysis was adopted to spatially categorize the sampled wells into three main clusters and characterized by the factor scores of the four-factor model. Two-parameter (pH and Eh) model derived from discriminant analysis can be used for preliminary assessment to determine whether the As concentration exceeds 10 μg/L with simple field measurements in this area., (Copyright © 2010 Elsevier B.V. All rights reserved.)

Aquacultural tilapia (Oreochromis mossambicus L.) and shrimp (Penaeus monodon L.) from groundwater-cultured ponds in southwestern Taiwan were analyzed to estimate arsenic (As) bioaccumulation and the potential health risk to human intake. Most of aquacultural ponds exhibited higher arsenic than maximum allowed concentrations (50 μg L(-1)) in pond water of Taiwan. Arsenic levels in tilapia in Budai, Yichu and Beimen were 0.92 ± 0.52 μg g(-1), 0.93 ± 0.19 μg g(-1) and 0.76 ± 0.03 μg g(-1), respectively and in shrimp was 0.36 ± 0.01 μg g(-1) in Beimen. Total arsenic in tilapia is highly correlated (R(2) = 0.80) with total arsenic concentration of pond water. Total arsenic in fish showed high correlation with that in bone (R(2) = 0.98), head (R(2) = 0.97) and tissue (R(2) = 0.96). Organic arsenic species (DMA) was found higher relative to inorganic species of As(III) and As(V). The average percent contribution of inorganic arsenic to total arsenic in fish samples was 12.5% and ranged between 11.7 to 14.2%. Bioaccumulation factors (BAFs) for total arsenic in fish ranged from 10.3 to 22.1, whereas BAF for inorganic arsenic ranged from 1.33 to 2.82. The mean human health cancer risk associated with the ingestion of inorganic arsenic in the fish was estimated at 2.36 × 10(-4) ± 0.99 × 10(-4), which is over 200 times greater than a de Minimus cancer risk of 1 × 10(-6). The mean human health hazard quotient associated with ingesting inorganic arsenic in the fish was 1.22 ± 0.52, indicating that expected human exposure exceeds the reference dose for non-cancer health effects by 22%. These results suggest that the inhabitants in this region are being subjected to moderately elevated arsenic exposure through the consumption of tilapia and shrimp raised in aquaculture ponds.

This study presented an integrated GIS-based approach for assessing potential carcinogenic risks via food-chain exposure of ingesting inorganic arsenic (As) in aquacultural tilapia, milkfish, mullet, and clam in the As-affected groundwater areas. To integrate spatial information, geographic information system (GIS) was adopted to combine polygon-shaped features of aquacultural species with cell-shaped features of As contamination in groundwater. Owing to sparse measured data, Monte Carlo simulation and sequential indicator simulation were used to characterize the uncertainty of assessed parameters. Target cancer risks (TRs) of ingesting As contents at fish ponds were spatially mapped to assess potential risks to human health. The analyzed results reveal that clam farmed at the western coastal ponds and milkfish farmed at the southwestern coastal ponds have high risks to human health, whereas tilapia cultivated mainly at the inland ponds only has high risks at the 95th percentile of TR. Mullet in general has low risks to human health. Moreover, to decrease risks, this study suggests reducing the use of As-affected groundwater at clam and milkfish ponds due to high bioconcentration factor (BCF) of clam and inorganic As accumulation ratio of milkfish. The integrated GIS-based approach can provide fishery administrators with an effective management strategy at specific fish ponds with high risks to human health.

Spatial distributions of groundwater quality are commonly heterogeneous, varying with depths and locations, which is important in assessing the health and ecological risks. Owing to time and cost constraints, it is not practical or economical to measure arsenic everywhere. A predictive model is necessary to estimate the distribution of a specific pollutant in groundwater. This study developed a logistic regression (LR) model to predict the residential well water quality in the Lanyang plain. Six hydrochemical parameters, pH, NO3- -N, NO2- -N, NH+ -N, Fe, and Mn, and a regional variable (binary type) were used to evaluate the probability of arsenic concentrations exceeding 10 microg/L in groundwater. The developed parsimonious LR model indicates that four parameters in the Lanyang plain aquifer, (pH, NH4+, Fe(aq), and a component to account for regional heterogeneity) can accurately predict probability of arsenic concentration > or =1 microg/Lin groundwater. These parameters provide an explanation for release of arsenic by reductive dissolution of As-rich FeOOH in NH4+ containing groundwater. A comparison of LR and indicator kriging (IK) show similar results in modeling the distributions of arsenic. LR can be applied to assess the probability of groundwater arsenic at sampled sites without arsenic concentration data apriori. However, arsenic sampling is still needed and required in arsenic-assessment stages in other areas, and the need for long-term monitoring and maintenance is not precluded.

We developed an inductance-based valvometry technique as a detection system to measure the valve daily activity in freshwater clam Corbicula fluminea in response to waterborne arsenic. Our findings reveal that C. fluminea experiences a valve opening in the absence of arsenic predominantly in the morning hours (03:00-08:00) with a mean daily opening/closing period of 21.32 (95% CI: 20.58-22.05) h. Amplification of daily activity occurred in the presence of arsenic. Behavioral toxicity assays revealed arsenic detection thresholds of 0.60 (95% CI: 0.53-0.66) mg l(-1) and 0.35 (95% CI: 0.30-0.40) mg l(-1) for response times of 60 and 300 min, respectively. The proposed valve daily activity model was linked with response time-specific Hill dose-response functions to predict valve opening/closing behavior in response to arsenic. The predictive capabilities were verified satisfactory with the measurements. Our results implicate a biomonitoring system by valve daily activity in C. fluminea to identify safe water uses in areas with elevated arsenic.

Arsenic is a potent human carcinogen of skin, lung, and urinary bladder. Freshwater clam Corbicula fluminea is a commercially important native species in Taiwan. C. fluminea is also a suitable biomonitoring test organism. Little is known, however, about the actual effects of arsenic on C. fluminea. The objectives of this study were to provide information on the acute toxicity and bioaccumulation kinetics of arsenic in C. fluminea. We carried out a 14-day exposure experiment to obtain bioaccumulation parameters. Uptake was very rapid when C. fluminea was first exposed and then slightly decayed during the uptake phase of the experiment and an uptake rate constant of 1.718 +/- 6.70 (mean +/- SE) mL g(-1) d(-1) was estimated. The elimination of arsenic from C. fluminea obeyed first-order depuration kinetics (r(2) = 0.85, p < 0.05) with a calculated half-life of 6.80 days. The derived bioaccumulation factor of 16.84 suggests that arsenic has a high potential for bioaccumulation in C. fluminea. This had important implications for dietary exposure of arsenic to humans who eat contaminated clams, because the soft tissue usually constitutes the majority of tissue consumed. The 96-h LC50 value was estimated to be 20.74 (95% CI: 11.74-30.79) mg L(-1) obtained from a 7-day acute toxicity bioassay. We also kinetically linked an acute toxicity model and a Hill sigmoid model to reconstruct an internal effect concentration based dose-response profile to assess the effect of soft tissue arsenic burden on the C. fluminea mortality. This result could be used to support the establishment of an ecological risk assessment to prevent possible ecosystem and human health consequences., (2008 Wiley Periodicals, Inc.)

This study investigated total arsenic (As) and As species contents of oysters (Crassostrea gigas) in different production areas, seasons and sea locations on the southwestern coast of Taiwan. Analytical results indicate that contents of total As, arsenite, arsenate, dimethylarsinic acid, monomethylarsonic acid and arsenobetaine in oysters are 9.90+/-3.68, 0.091+/-0.104, 0.033+/-0.038, 0.529+/-0.284, 0.037+/-0.046 and 3.94+/-1.33 mg/g (dry wt), respectively. A ratio of inorganic As concentrations to total As concentrations is 1.26%. Total As contents of oysters cultured in the outer sea are statistically significantly lower than those of oysters cultured in the inner sea. The total As contents of oysters is the highest in Putai, where the blackfoot disease prevails. The low As contents in oysters is attributed to the low temperature in winter, which slows the metabolism of oysters. A maximum value is 33.37 microg/g (dry) in Putai in spring, because a considerable amount of aquacultural waste water with high As contents is discharged into adjacent drainage channels and rivers there during that season.

This work determined scopes of arsenic(As)-contaminated groundwater using risk-based indicator classification approaches in blackfoot disease hyperendemic areas of southern Taiwan. Indicator kriging was first used to establish a conditional cumulative distribution function at each cell. Three approaches--the p-quantile estimate, the E-type estimate and the minimization of the expected loss--were then adopted to delimit contaminated regions for a regulated standard of As concentrations in groundwater. According to a risk assessment model established in our previous research, the standard was set to 250 microg/l for aquacultural use, corresponding to the 77.1th percentile of observed concentrations. Misclassification risks and uncertainty were examined for the classification approaches. The analyzed results reveal that contaminated areas are the largest using the 0.771-quantile estimate, whereas they are the smallest using the minimization of the expected loss. Proportions of credible polluted areas with low risks to false positives maintain a constant, 12.9-13.2%, for the classification approaches. To reduce a great impact on human health, As-polluted groundwater should be strictly prohibited to cultivate fish in credible polluted zones and monitored persistently in polluted zones with high risks to false positives.

This study analyzed the potential health risk associated with the ingestion of arsenic-affected groundwater in the arseniasis-endemic Lanyang plain of northeastern Taiwan. Indicator kriging was used to estimate arsenic concentrations in groundwater. Target cancer risk (TR) and dose response functions were adopted to evaluate the potential health risk based on the estimated arsenic concentration distributions. The estimated arsenic concentrations in groundwater reveal that arsenic concentrations (>50 microg/L) in well water are high in six townships - JiaoSi, YiLan, JhungWei, WuJie, DonShan and LouDon. Highest arsenic concentrations (70.32 microg/L) are in the YiLan and the JhungWei townships. The estimated TR values at the arsenic-affected townships are ten times more than an acceptable standard (10(-6)). The largest TR values are 145.5 and 91.2 times higher than an acceptable standard for males and females, respectively. The estimated annual mortalities by arsenic-induced internal cancers occur in the YiLan township (ten cases), LouDon (five cases), WuJie (three cases), JhungWei (two cases) and DonShan (one case). The highest number of mortalities per year in the study area is 24. Residents of the six townships with high arsenic-affected groundwater should use tap water as drinking water and use groundwater only for other purpose. The well water in other townships in the Lanyang plain has no adverse effects on human health.

This study surveyed the total arsenic (As) and As species contents in clams (Meretrix lusoria) farmed in areas of hyperendemic blackfoot disease (BFD) in southwestern Taiwan. Total As and As species in sediment and pond water were also analyzed to examine the bioaccumulation of As in clams in their exposure environment. Moreover, potential carcinogenic risks associated with the ingestion of As in aquacultural clams were evaluated probabilistically. The average total As contents in medium-sized and small clams were 7.62 and 10.71 microg/g (dry wt), respectively. The content of the As species in this study was approximately 61% of the total As content. The other unquantified As species are possibly arsenocholine, arsenosugar and arsenolipid. The average ratios of inorganic As contents to total As contents in clams ranged from 12.3% to 14.0% which are much higher than that found in the farmed oyster (Crassostrea gigas), indicating that humans may expose to larger quantities of inorganic As by ingesting the same amount of clam as oyster. Using different ingestion rates derived by the average consumption method and the questionnaire method, the estimated risks to human health associated with consuming clams from the BFD area ranging from slightly to largely exceed the standard target risk. Based on the estimation of the TR model, a 0.18g/day-person of the safe ingestion rate of clams in the BFD region is recommended.

This study applied multivariate factorial kriging to derive the characteristics of the spatial variations of groundwater arsenic distributions at different scales on the ChiaNan floodplain, Taiwan. Seven variables (dissolved oxygen, oxidation-reduction potential, alkalinity, sulfate, iron cations, manganese cations and total organic carbon) and Arsenic were adopted to analyze the mechanisms of arsenic enrichments in groundwater. The hydrogeological environment had spatial and quantitative influences on arsenic enrichments at different scales. The regional scale was set to 32 km referring to the extension distance of flow paths to reflect the effects of flushing in the aquifer, while the local scale was set to 16 km referring to the farthest distance of seawater intrusion to determine the influence of seawater intrusion. The results of factorial kriging suggested that arsenic releases resulted partially from pyrite oxidation during the flushing at the regional scale and partially due to the siderite dissolution at the local scale. Overall, the alkalinity dominated arsenic distribution in groundwater at both the regional and local scales. The multivariate factorial kriging results also demonstrated that seawater intrusion slightly affected the increase of arsenic in groundwater, accounting for only 17.3% of total variation. However, the interaction of seawater intrusion and arsenic distribution in space indicated that seawater intrusion restrained the distribution of arsenic from the areas where seawater was located. High dissolved oxygen was found at where over-pumping induced drawdown cones occurred and also limited the spatial variation of arsenic. Our findings indicate that multivariate factorial kriging can be a useful mapping tool to improve understanding of the mechanism of arsenic release in groundwater at different scales. And the results conducted from the application of multivariate factorial kriging in southwestern Taiwan reveal the important influences of the hydrogeological processes, either artificial or natural, on the arsenic variations in groundwater.

This study estimated the human health risk associated with ingesting inorganic arsenic through consumption of farmed oysters in Taiwan. Two hundred fifty-four samples of oyster (Crassostrea gigas) were collected from four townships in southwest coastal areas, where 90% of Taiwan's oysters are produced. The concentrations of total arsenic and arsenic species including As(V), As(III), monomethylarsonic acid (MMA) and dimethylarsinic acid (DMA) were analyzed. The analytical results reveal that the ratio of mean concentration among the four townships of inorganic As to total concentration of As in oysters is approximately 1.64%. The mean concentrations of As(III) and As(V) in oysters from the four townships range from 0.071 to 0.145 microg/g, and 0.032 to 0.062 microg/g respectively. The estimated target cancer risks (TR), based on a 95% occurrence probability from ingesting inorganic As by consuming oysters at a rate of 18.6-56 g/day, range from 1.26 x 10(-5) to 3.82 x 10(-5). The probabilities of TR fell within the range 10(-6)-10(-4), suggesting that inorganic As uptake from farmed oysters is associated with a potential cancer risk. Moreover, a target hazard quotient (THQ) was used to evaluate the non-carcinogenic risk associated with ingesting inorganic As through oyster consumption at a rate of 18.6-56 g/day. The THQ values based on a 95% probability of exposure range from 0.071 to 0.214. All THQ values are below unity, indicating that farmed oyster consumption contributes only a little to the non-carcinogenic risk. Based on the estimation of the TR model, an ingestion rate of 1.6 g/day is recommended to meet the 95th percentile of carcinogenic risk, 10(-6), for exposure to inorganic As through the consumption of oysters in Taiwan.

This work analyzed spatially potential carcinogenic risks associated with ingesting arsenic (As) contents in aquacultural tilapia (Oreochromis mossambicus) in coastal regions of southwestern Taiwan, where the blackfoot disease prevails. Sequential indicator simulation (SIS) was used to reproduce As exposure distributions in groundwater based on their three-dimensional variability. A target cancer risk (TR) associated with ingesting As in aquacultural tilapia was calculated to evaluate the potential risk to human health. Owing to sparse measured data, Monte Carlo simulation and SIS properly accounted for the uncertainty of assessed parameters. The probabilistic risk assessment formulated suitable strategies under various remedial stages. Aquacultural regions with high risks were mapped to elucidate the safety of groundwater use at different depths. Many TRs determined from the risks at the 75th and 95th percentiles exceed one millionth in the regions, indicating that ingesting tilapia farmed in the highly As-polluted regions poses potential cancer threats to human health. The 75th percentile of TR is considered in formulating a remedial strategy for the aquacultural use of groundwater in the preliminary stage. Additionally, this study suggests reducing the use of groundwater in aquaculture or changing the depths from which groundwater is withdrawn in the areas with high risks of cancer.

An investigation of shallow ground water quality revealed that high arsenic (As) concentrations were found in both aquifers and aquitards in the southern Choushui River alluvial fan of Taiwan. A total of 655 geological core samples from 13 drilling wells were collected and analyzed. High As contents were found primarily in aquitards, to a maximum of 590 mg/kg. The contents were correlated with the locations of the marine sequences. Additionally, strong correlations among the As concentrations of core samples, the clay, and the geological age of the Holocene transgression were identified. Most of the As in ground water originated from the aquitard of the marine sequence. The high As content in marine formations with high clay contents may be attributable to the bioaccumulation of As in the sea organisms, which accrued and were deposited in the formation. A preliminary geogenic model of the origin of the high As concentration in the shallow sedimentary basin of the Choushui River alluvial fan of Taiwan is proposed.

Data on the quality of groundwater obtained from several multi-level monitoring wells indicated that arsenic (As) concentration far exceeds the drinking water supply standard in the coastal aquifer of the Yun-Lin, Taiwan. In this study, an estimated As probability risk was computed using indicator kriging to assess the As contamination potential of exceeding the drinking water supply standard in the Yun-Lin county. A three-dimensional (3D) spatial variability model was presented to analyze anisotropically the variation of As concentration using a multi-level threshold indicator variable. This 3D estimator overcomes the scarcity of the data and establishes a vertical correlation of measured As data. The results indicate high As pollution probability in the coastal area and in the Pei-Kang river basin. The highest probability, 0.92, of the As pollution is in the shallow aquifer of the Kou-Hu. The contamination potential of As is primarily within an aquifer depth of 180 m. The contaminated aquifer (<180 m) is not suitable for supplying drinking water. The contamination potential of As is low at the depths of more than 190 m. However, the probabilities associated with the As pollution still exceed 0.2 in the deep aquifer of four coastal townships of the Yun-Lin, and may pose risks to human health if the groundwater is used for drinking.

A study was conducted to measure the arsenic species in farmed mouthbreeder (Oreochromis mossambicus) and culture ponds in water in blackfoot disease (BFD) hyperendemic areas in Taiwan. The relationships between arsenic species of aquaculture ponds and farmed fish were also explored. Biota samples were extracted with methanol/water (1/1, v/v) using a Soxhlet extraction apparatus. The concentrations of arsenite As (III), arsenate As (V), monomethylarsonic acid (MMA), and dimethylarsinic acid (DMA) of extracts were measured by high-performance liquid chromatography (HPLC) linked to a hydride generator and atomic absorption spectrometry (HG-AAS). Moreover, arsenobetaine (AB) was analyzed by HPLC linked to ultra violet (UV) and HG-AAS. Concentrations of arsenic species were determined in 68 mouthbreeder (O. mossambicus) samples and 21 culture ponds from Putai and Yichu Townships of Chiayi County and Hsuehchia and Peimen Townships of Tainan County. The mean arsenic levels of culture ponds in Putai, Yichu, Hsuehchia, and Peimen were 75.8, 15.1, 14.4, and 221.0 microg/l, respectively. The water of culture ponds was dominated by As (V). The inorganic arsenic percentage of fish (7.4%) was higher than that reported by other seafood surveys. Except for the MMA and As (III) levels, As (V), DMA, AB, and total arsenic levels in fish significantly increased with inorganic and total arsenic concentrations of the pond water. Inorganic arsenic species are more toxic than methyl arsenic species. Therefore the effect of inorganic arsenic species might result in a greater number of adverse health effects to the general public. It is of importance to evaluate the inorganic arsenic levels of farmed seafood in arsenic-contaminated areas.

Factor analysis is applied to 28 groundwater samples collected from wells in the coastal blackfoot disease area of Yun-Lin, Taiwan. Correlations among 13 hydrochemical parameters are statistically examined. A two-factor model is suggested and explains over 77.8% of the total groundwater quality variation. Factor 1 (seawater salinization) includes concentrations of EC, TDS, Cl(-), SO(4)(2-), Na(+), K(+) and Mg(2+), and Factor 2 (arsenic pollutant) includes concentrations of Alk, TOC and arsenic. Maps are drawn to show the geographical distribution of the factors. These maps delineate high salinity and arsenic concentrations. The geographical distribution of the factor scores at individual wells does not reveal the sources of the constituents, which are instead, deduced from geological and hydrological evidence. The areas of high seawater salinization and arsenic pollution correspond well to the groundwater over-pumping area. Over-pumping of the local groundwater causes land subsidence and gradual salinization by seawater. The over-pumping also introduces excess dissolved oxygen that oxidizes the immobile minerals, releases arsenic by reductive dissolution of arsenic-rich iron oxyhydroxides and increases the arsenic concentration in water. The over-extraction of groundwater is the major cause of groundwater salinization and arsenic pollution in the coastal area of Yun-Lin, Taiwan.

The general objective of our work was to determine the acute toxicity and bioaccumulation of arsenic (As) in tilapia (Oreochromis mossambicus) from the blackfoot disease (BFD) area in Taiwan. The average concentration of As in pond water ranged from 17.8 to 49 microg L(-1). Acute toxicity tests showed that the As concentration that caused toxicity to tilapia ranged from 69 060 microg As L(-1), in the 24-h toxicity test, to 28 680 microg As L(-1), in the 96-h toxicity test. We measured As concentrations in various tissues of tilapia to identify the affinities of tissues for As. Significant correlations were found among the As concentrations in all tissues. The highest bioconcentration factor (BCF) was found in the intestine (maximum value: 2270). The order of BCFs was: intestine > stomach > liver approximately gill > muscle. Arsenic concentrations in all tissues were allometric, negatively correlating with fish body weight [r(2) = 0.63 +/- 0.045 (mean +/- SE), p < 0.05]. Our results also revealed that As concentrations in muscle tissue were positively correlated with As accumulation in the viscera (r(2) = 0.85, p < 0.05). Significantly higher concentrations of As were obtained in the viscera of tilapia [12.65 +/- 10.17 microg g(-1) dry wt (mean +/- SD)] than in the muscle tissue (3.55 +/- 0.42 microg g(-1) dry wt). Our results suggest that a simple way of reducing the health risk associated with consuming tilapia is to trim and cook the fish properly, that is, removing the viscera of tilapia can greatly reduce the amount of As ingested and consequently reduce the health risks., (Copyright 2003 Wiley Periodicals, Inc. Environ Toxicol 18: 252-259, 2003.)