Distribution and chemical speciation of dissolved inorganic arsenic were examined in Yellow Sea and East China Sea. Results demonstrated that： （1） both As（Ⅲ） and As（Ⅴ） were detected, with As（V） dominated at...Distribution and chemical speciation of dissolved inorganic arsenic were examined in Yellow Sea and East China Sea. Results demonstrated that： （1） both As（Ⅲ） and As（Ⅴ） were detected, with As（V） dominated at 40% stations of surface water and 51% stations of bottom water; （2） influenced by the exchange of fresh and sea water, the type of surface sediment and the transport of various water masses, large values in surface water were observed along the coastal region and in the same latitude of Changjiang River Estuary and Hangzhou Bay, and in bottom water found in the southern area where the Taiwan Warm Current and Kuroshio Current influenced; （3） As（Ⅲ） behaved non-conservatively in Changjiang River Estuary. Man-derived inputs cause substantial positive deviation from the theoretical dilution. The negative correlation of As（Ⅴ） to salinity in surface water suggested that it behaved conservatively during the transportation along Changjiang River Estuary. While, the occurrence of As（Ⅴ） up to the linear fit in bottom water indicated the eventual transfer from dissolved phase to particulate phase, which was impossible to be determined without the knowledge of arsenic level and speciation in suspended particulate matter. Further study is needed on the arsenic source/sink relationships based on the distribution profiles.展开更多
A novel 1-methylimidazole ionic liquid modified SBA15 mesoporous silica(1-MIIL@SBA15) was synthesized and applied to selective separation of inorganic arsenic(iAs) in rice by dispersive solid phase extraction(DSPE), f...A novel 1-methylimidazole ionic liquid modified SBA15 mesoporous silica(1-MIIL@SBA15) was synthesized and applied to selective separation of inorganic arsenic(iAs) in rice by dispersive solid phase extraction(DSPE), followed by hydride generation-atomic fluorescence spectrometric(HG-AFS) quantification. The prepared sorbent was characterized by FTIR, FESEM, BET and Zeta potential. Key parameters of adsorption and desorption in DSPE were optimized using standard reference material 1568 b rice flour. Under optimal conditions, the limit of detection was 8.776 ng/kg, relative standard deviation was ≤2.0%, and recoveries of iAs were in the 92.3～94.4% range. This method was successfully applied to the determination of iAs in rice. Under acidic condition, the electrostatic interaction between the positively charged 1-MIIL@SBA15 and anionic iAs played an important role in selective iAs separation, rendering this method suitable for iAs analysis.展开更多
Water samples were collected in the coastal area of the Changjiang Estuary on four cruises from August 2002 to May 2003. The seasonal variations of dissolved inorganic arsenic (DIAs) distributions were analyzed. The r...Water samples were collected in the coastal area of the Changjiang Estuary on four cruises from August 2002 to May 2003. The seasonal variations of dissolved inorganic arsenic (DIAs) distributions were analyzed. The results showed that the distributions of DIAs were mainly influenced by the terrestrial input and the intrusion of the Kuroshio Subsurface Water (KSSW). The concentration of the total dissolved inorganic arsenic (TDIAs) decreased consecutively from winter to summer, while it increased in autumn. The distributions of TDIAs showed some relationships with salinity and suspended particulate matter (SPM). The relationships between DIAs speciation (including arsenite [As(Ⅲ)] and arsenate [As(Ⅴ)]), biological activity and the availabilities of the phosphate were investigated in the study area for the cruise August 2002. The ratio of As (Ⅲ)/TDIAs increased with the decrease of phosphate concentrations. In the bottom water, the As(Ⅲ)/TDIAs ratio decreased with the increasing of N/P. The concentration of TDIAs decreased 28.7% approximately after the occurrence of harmful algal blooms (HAB) because of the uptake of arsenate by algae. Further study is needed about the arsenic source/sink relationships in their vertical or horizontal profiles and the uptake mechanism during the occurrence of harmful algal blooms.展开更多
Selenium(Se)in paddy rice is one of the significant sources of human Se nutrition.However,the effect of arsenic(As)pollution in soil on the translocation of Se species in rice plants is unclear.In this research,a pot ...Selenium(Se)in paddy rice is one of the significant sources of human Se nutrition.However,the effect of arsenic(As)pollution in soil on the translocation of Se species in rice plants is unclear.In this research,a pot experiment was designed to examine the effect of the addition of 50 mg As/kg soil as arsenite or arsenate on the migration of Se species from soil to indica Minghui 63 and Luyoumingzhan.The results showed that the antagonism between inorganic As and Se was closely related to the rice cultivar and Se oxidation state in soil.Relative to the standalone selenate treatment,arsenite significantly(p<0.05)decreased the accumulation of selenocystine,selenomethionine and selenate in the roots,stems,sheaths,leaves,brans and kernels of both cultivars by 21.4%-100.0%,40.0%-100.0%,41.0%-100%,5.4%-96.3%,11.3%-100.0% and 26.2%-39.7% respectively,except for selenocystine in the kernels of indica Minghui 63 and selenomethionine in the leaves of indica Minghui 63 and the stems of indica Luyoumingzhan.Arsenate also decreased(p<0.05)the accumulation of selenocystine,selenomethionine and selenate in the roots,stems,brans and kernels of both cultivars by 34.9%-100.0%,30.2%-100.0%,11.3%-100.0% and 5.6%-39.6%respectively,except for selenate in the stems of indica Minghui 63.However,relative to the standalone selenite treatment,arsenite and arsenate decreased(p<0.05)the accumulation of selenocystine,selenomethionine and selenite only in the roots of indica Minghui 63 by 45.5%-100.0%.Our results suggested that arsenite and arsenate had better antagonism toward Se species in selenate-added soil than that in selenite-added soil;moreover,arsenite had a higher inhibiting effect on the accumulation of Se species than arsenate.展开更多
Approximately 94 to 220 million people worldwide are at risk of drinking well water containing arsenic > 10 μg/L, the WHO guideline value. To identify non-compliant domestic wells, assess health risks and reduce e...Approximately 94 to 220 million people worldwide are at risk of drinking well water containing arsenic > 10 μg/L, the WHO guideline value. To identify non-compliant domestic wells, assess health risks and reduce exposure, accurate and rapid on-site inorganic arsenic screening methods are desirable because all domestic wells worldwide need to be tested.Here, the principles, advantages and limitations of commonly used colorimetry, electrochemistry, and biosensing methods are critically reviewed, with the performance compared with laboratory-based benchmark methods. Most commercial kits are based on the classic Gutzeit reaction. Despite being semi-quantitative, the more recent and more expensive products display improved and acceptable accuracy and shorter testing time (~10 min). Carried out by trained professionals, electrochemical methods are also feasible for on-site analysis, although miniaturization is desirable yet challenging. Biosensing using whole bacterial cells or bio-engineered materials such as aptamers is promising, if incorporated with function specific nanomaterials and biomaterials. Since arsenic is frequently found as arsenite in reducing groundwater and subject to oxidation during sampling, transportation and storage, on-site separation and sample preservation are feasible but the specific methods should be chosen based on sample matrix and tested before use. To eliminate arsenic exposure among hundreds of millions of mostly rural residents worldwide, we call for concerted efforts in research community and regulatory authority to develop accurate, rapid, and affordable tests for on-site screening and monitoring of arsenic in drinking water. Access to affordable testing will benefit people who are socioeconomically disadvantaged.展开更多
p-Arsanilic acid（p-ASA） is widely used in China as livestock and poultry feed additive for promoting animal growth.The use of organoarsenics poses a potential threat to the environment because it is mostly excreted ...p-Arsanilic acid（p-ASA） is widely used in China as livestock and poultry feed additive for promoting animal growth.The use of organoarsenics poses a potential threat to the environment because it is mostly excreted by animals in its original form and can be transformed by UV–Vis light excitation.This work examined the initial rate and efficiency of p-ASA phototransformation under UV-C disinfection lamp.Several factors influencing p-ASA phototransformation,namely,p H,initial concentration,temperature,as well as the presence of Na Cl,NH4＋,and humic acid,were investigated.Quenching experiments and LC–MS were performed to investigate the mechanism of p-ASA phototransformation.Results show that p-ASA was decomposed to inorganic arsenic（including As（Ⅲ） and As（V））and aromatic products by UV-C light through direct photolysis and indirect oxidation.The oxidation efficency of p-ASA by direct photosis was about 32%,and those by HOU and1O2 were 19% and 49%,respectively.Cleavage of the arsenic–benzene bond through direct photolysis,HOU oxidation or1O2 oxidation results in simultaneous formation of inorganic As（Ⅲ）,As（IV）,and As（V）.Inorganic As（Ⅲ） is oxidized to As（IV） and then to As（V） by1O2 or HOU.As（IV） can undergo dismutation or simply react with oxygen to produce As（V） as well.Reactions of the organic moieties of p-ASA produce aniline,aminophenol and azobenzene derivatives as main products.The photoconvertible property of p-ASA implies that UV disinfection of wastewaters from poultry and swine farms containing p-ASA poses a potential threat to the ecosystem,especially agricultural environments.展开更多
It has been estimated that between 94 million and 220 million people around the world are at risk of consuming drinking water that contain arsenic concentrations higher than 10μg/L(Podgorski and Berg,2020).
Our previous data have shown that inorganic arsenic concentrations were high in Dianchi Lake,China,where Microcystis blooms often occur.To explore the relationship between arsenic and the growth of Microcystis,the eff...Our previous data have shown that inorganic arsenic concentrations were high in Dianchi Lake,China,where Microcystis blooms often occur.To explore the relationship between arsenic and the growth of Microcystis,the effects of arsenite[As(III)]and arsenate[As(V)]on the growth and toxin production of M.aeruginosa strain FACHB 905 were tested.Results showed that M.aeruginosa FACHB 905 was tolerant to inorganic arsenic and its growth was not inhibited when the concentration of As(III)was below 10-5 mol L-1 or that of As(V)below 10-3 mol L-1.Total microcystin production was stimulated in the presence of 10-7 mol L-1 As(III)and the response of this M.aeruginosa strain to As(III)seemed to be a typical inverted U-shaped hormesis.The content increase of microcystin-LR per cell indicated that the toxicity was enhanced as M.aeruginosa FACHB 905 was exposed to As(V).Considering the relatively high concentration of inorganic arsenic in Dianchi Lake(139μg L-1 in epilimnetic water),the origin of the M.aeruginosa strain,inorganic arsenic favors survival of M.aeruginosa FACHB 905 and may stimulate its microcystin production and cellular toxicity.展开更多
Chromium and/or arsenate removal by Fe（Ⅱ） as a function of pH, Fe（Ⅱ） dosage and initial Cr（Ⅵ）/As（Ⅴ） ratio were examined in batch tests. The presence of arsenate reduced the removal efficiency of chromium b...Chromium and/or arsenate removal by Fe（Ⅱ） as a function of pH, Fe（Ⅱ） dosage and initial Cr（Ⅵ）/As（Ⅴ） ratio were examined in batch tests. The presence of arsenate reduced the removal efficiency of chromium by Fe（Ⅱ）, while the presence of chromate significantly increased the removal efficiency of arsenate by Fe（Ⅱ） at pH 6-8, In the absence of arsenate, chromium removal by Fe（Ⅱ） increased to a maximum with increasing pH from 4 to 7 and then decreased with a further increase in pH. The increment in Fe（Ⅱ） dosage resulted in an improvement in chromium removal and the improvement was more remarkable under alkaline conditions than that under acidic conditions. Chromium removal by Fe（Ⅱ） was reduced to a larger extent under neutral and alkaline conditions than that under acidic conditions due to the presence of 10 μtmol/L arsenate. The presence of 20 μmol/L arsenate slightly improved chromium removal by Fe（Ⅱ） at pH 3.9-5,8, but had detrimental effects at pH 6.7-9.8. Arsenate removal was improved significantly at pH 4-9 due to the presence of 10μmol/L chromate at Fe（Ⅱ） dosages of 20-60 μmol/L. Elevating the chromate concentration from 10 to 20μmol/L resulted in a further improvement in arsenate removal at pH 4.0-4.6 when Fe（Ⅱ） was dosed at 30-60 μmol/L.展开更多
基金The Strategic Priority Research Program of the Chinese Academy of Sciences under contract No.XDA11020102the National Natural Science Foundation of China under contract Nos 41306055 and U1406403
文摘Distribution and chemical speciation of dissolved inorganic arsenic were examined in Yellow Sea and East China Sea. Results demonstrated that： （1） both As（Ⅲ） and As（Ⅴ） were detected, with As（V） dominated at 40% stations of surface water and 51% stations of bottom water; （2） influenced by the exchange of fresh and sea water, the type of surface sediment and the transport of various water masses, large values in surface water were observed along the coastal region and in the same latitude of Changjiang River Estuary and Hangzhou Bay, and in bottom water found in the southern area where the Taiwan Warm Current and Kuroshio Current influenced; （3） As（Ⅲ） behaved non-conservatively in Changjiang River Estuary. Man-derived inputs cause substantial positive deviation from the theoretical dilution. The negative correlation of As（Ⅴ） to salinity in surface water suggested that it behaved conservatively during the transportation along Changjiang River Estuary. While, the occurrence of As（Ⅴ） up to the linear fit in bottom water indicated the eventual transfer from dissolved phase to particulate phase, which was impossible to be determined without the knowledge of arsenic level and speciation in suspended particulate matter. Further study is needed on the arsenic source/sink relationships based on the distribution profiles.
基金Financially supported by the National Natural Science Foundation of China(No.31701708)the Outstanding Youth Foundation Project of Fujian Agriculture and Forestry University of China(No.xjq201710)
文摘A novel 1-methylimidazole ionic liquid modified SBA15 mesoporous silica(1-MIIL@SBA15) was synthesized and applied to selective separation of inorganic arsenic(iAs) in rice by dispersive solid phase extraction(DSPE), followed by hydride generation-atomic fluorescence spectrometric(HG-AFS) quantification. The prepared sorbent was characterized by FTIR, FESEM, BET and Zeta potential. Key parameters of adsorption and desorption in DSPE were optimized using standard reference material 1568 b rice flour. Under optimal conditions, the limit of detection was 8.776 ng/kg, relative standard deviation was ≤2.0%, and recoveries of iAs were in the 92.3～94.4% range. This method was successfully applied to the determination of iAs in rice. Under acidic condition, the electrostatic interaction between the positively charged 1-MIIL@SBA15 and anionic iAs played an important role in selective iAs separation, rendering this method suitable for iAs analysis.
基金This research was supported by the National Basic Research Program of China （Nos. 2001CB409703 and G1999043705） the National Natural Science Foundation of China （Nos. 40036010 and 40206017）.
文摘Water samples were collected in the coastal area of the Changjiang Estuary on four cruises from August 2002 to May 2003. The seasonal variations of dissolved inorganic arsenic (DIAs) distributions were analyzed. The results showed that the distributions of DIAs were mainly influenced by the terrestrial input and the intrusion of the Kuroshio Subsurface Water (KSSW). The concentration of the total dissolved inorganic arsenic (TDIAs) decreased consecutively from winter to summer, while it increased in autumn. The distributions of TDIAs showed some relationships with salinity and suspended particulate matter (SPM). The relationships between DIAs speciation (including arsenite [As(Ⅲ)] and arsenate [As(Ⅴ)]), biological activity and the availabilities of the phosphate were investigated in the study area for the cruise August 2002. The ratio of As (Ⅲ)/TDIAs increased with the decrease of phosphate concentrations. In the bottom water, the As(Ⅲ)/TDIAs ratio decreased with the increasing of N/P. The concentration of TDIAs decreased 28.7% approximately after the occurrence of harmful algal blooms (HAB) because of the uptake of arsenate by algae. Further study is needed about the arsenic source/sink relationships in their vertical or horizontal profiles and the uptake mechanism during the occurrence of harmful algal blooms.
基金supported by the National Natural Science Foundation of China(No.21677033)the Natural Science Foundation of Science and Technology Department of Fujian Government(No.2021N0005)Fujian Agriculture and Forestry University Innovation Fund(Nos.CXZX2020049A,KFb22047XA)。
文摘Selenium(Se)in paddy rice is one of the significant sources of human Se nutrition.However,the effect of arsenic(As)pollution in soil on the translocation of Se species in rice plants is unclear.In this research,a pot experiment was designed to examine the effect of the addition of 50 mg As/kg soil as arsenite or arsenate on the migration of Se species from soil to indica Minghui 63 and Luyoumingzhan.The results showed that the antagonism between inorganic As and Se was closely related to the rice cultivar and Se oxidation state in soil.Relative to the standalone selenate treatment,arsenite significantly(p<0.05)decreased the accumulation of selenocystine,selenomethionine and selenate in the roots,stems,sheaths,leaves,brans and kernels of both cultivars by 21.4%-100.0%,40.0%-100.0%,41.0%-100%,5.4%-96.3%,11.3%-100.0% and 26.2%-39.7% respectively,except for selenocystine in the kernels of indica Minghui 63 and selenomethionine in the leaves of indica Minghui 63 and the stems of indica Luyoumingzhan.Arsenate also decreased(p<0.05)the accumulation of selenocystine,selenomethionine and selenate in the roots,stems,brans and kernels of both cultivars by 34.9%-100.0%,30.2%-100.0%,11.3%-100.0% and 5.6%-39.6%respectively,except for selenate in the stems of indica Minghui 63.However,relative to the standalone selenite treatment,arsenite and arsenate decreased(p<0.05)the accumulation of selenocystine,selenomethionine and selenite only in the roots of indica Minghui 63 by 45.5%-100.0%.Our results suggested that arsenite and arsenate had better antagonism toward Se species in selenate-added soil than that in selenite-added soil;moreover,arsenite had a higher inhibiting effect on the accumulation of Se species than arsenate.
基金Support was provided by NSFC grants 41831279 and 41772265 to Yan Zhenggrant 2021YFA0715900 from the National Key Research and Development Program of China。
文摘Approximately 94 to 220 million people worldwide are at risk of drinking well water containing arsenic > 10 μg/L, the WHO guideline value. To identify non-compliant domestic wells, assess health risks and reduce exposure, accurate and rapid on-site inorganic arsenic screening methods are desirable because all domestic wells worldwide need to be tested.Here, the principles, advantages and limitations of commonly used colorimetry, electrochemistry, and biosensing methods are critically reviewed, with the performance compared with laboratory-based benchmark methods. Most commercial kits are based on the classic Gutzeit reaction. Despite being semi-quantitative, the more recent and more expensive products display improved and acceptable accuracy and shorter testing time (~10 min). Carried out by trained professionals, electrochemical methods are also feasible for on-site analysis, although miniaturization is desirable yet challenging. Biosensing using whole bacterial cells or bio-engineered materials such as aptamers is promising, if incorporated with function specific nanomaterials and biomaterials. Since arsenic is frequently found as arsenite in reducing groundwater and subject to oxidation during sampling, transportation and storage, on-site separation and sample preservation are feasible but the specific methods should be chosen based on sample matrix and tested before use. To eliminate arsenic exposure among hundreds of millions of mostly rural residents worldwide, we call for concerted efforts in research community and regulatory authority to develop accurate, rapid, and affordable tests for on-site screening and monitoring of arsenic in drinking water. Access to affordable testing will benefit people who are socioeconomically disadvantaged.
基金supported by the National Natural Science Foundation of China(Nos 51508423 and 21477090)
文摘p-Arsanilic acid（p-ASA） is widely used in China as livestock and poultry feed additive for promoting animal growth.The use of organoarsenics poses a potential threat to the environment because it is mostly excreted by animals in its original form and can be transformed by UV–Vis light excitation.This work examined the initial rate and efficiency of p-ASA phototransformation under UV-C disinfection lamp.Several factors influencing p-ASA phototransformation,namely,p H,initial concentration,temperature,as well as the presence of Na Cl,NH4＋,and humic acid,were investigated.Quenching experiments and LC–MS were performed to investigate the mechanism of p-ASA phototransformation.Results show that p-ASA was decomposed to inorganic arsenic（including As（Ⅲ） and As（V））and aromatic products by UV-C light through direct photolysis and indirect oxidation.The oxidation efficency of p-ASA by direct photosis was about 32%,and those by HOU and1O2 were 19% and 49%,respectively.Cleavage of the arsenic–benzene bond through direct photolysis,HOU oxidation or1O2 oxidation results in simultaneous formation of inorganic As（Ⅲ）,As（IV）,and As（V）.Inorganic As（Ⅲ） is oxidized to As（IV） and then to As（V） by1O2 or HOU.As（IV） can undergo dismutation or simply react with oxygen to produce As（V） as well.Reactions of the organic moieties of p-ASA produce aniline,aminophenol and azobenzene derivatives as main products.The photoconvertible property of p-ASA implies that UV disinfection of wastewaters from poultry and swine farms containing p-ASA poses a potential threat to the ecosystem,especially agricultural environments.
文摘It has been estimated that between 94 million and 220 million people around the world are at risk of consuming drinking water that contain arsenic concentrations higher than 10μg/L(Podgorski and Berg,2020).
基金supported by the State Key Laboratory of Freshwater Ecology and Biotechnology(2009FBZ09)National Major Science and Technology Program of China(2009ZX07104-005-03)the Hubei Key Laboratory of Crop Diseases,Insect Pests and Weeds Control(2011CDIWC-1-1)
文摘Our previous data have shown that inorganic arsenic concentrations were high in Dianchi Lake,China,where Microcystis blooms often occur.To explore the relationship between arsenic and the growth of Microcystis,the effects of arsenite[As(III)]and arsenate[As(V)]on the growth and toxin production of M.aeruginosa strain FACHB 905 were tested.Results showed that M.aeruginosa FACHB 905 was tolerant to inorganic arsenic and its growth was not inhibited when the concentration of As(III)was below 10-5 mol L-1 or that of As(V)below 10-3 mol L-1.Total microcystin production was stimulated in the presence of 10-7 mol L-1 As(III)and the response of this M.aeruginosa strain to As(III)seemed to be a typical inverted U-shaped hormesis.The content increase of microcystin-LR per cell indicated that the toxicity was enhanced as M.aeruginosa FACHB 905 was exposed to As(V).Considering the relatively high concentration of inorganic arsenic in Dianchi Lake(139μg L-1 in epilimnetic water),the origin of the M.aeruginosa strain,inorganic arsenic favors survival of M.aeruginosa FACHB 905 and may stimulate its microcystin production and cellular toxicity.
基金supported by the National Natural Science Foundation of China (No. 50908060,50821002)the Ph.D Program Foundation of Ministry of Education of China for New Faculty (No. 200802131053)
文摘Chromium and/or arsenate removal by Fe（Ⅱ） as a function of pH, Fe（Ⅱ） dosage and initial Cr（Ⅵ）/As（Ⅴ） ratio were examined in batch tests. The presence of arsenate reduced the removal efficiency of chromium by Fe（Ⅱ）, while the presence of chromate significantly increased the removal efficiency of arsenate by Fe（Ⅱ） at pH 6-8, In the absence of arsenate, chromium removal by Fe（Ⅱ） increased to a maximum with increasing pH from 4 to 7 and then decreased with a further increase in pH. The increment in Fe（Ⅱ） dosage resulted in an improvement in chromium removal and the improvement was more remarkable under alkaline conditions than that under acidic conditions. Chromium removal by Fe（Ⅱ） was reduced to a larger extent under neutral and alkaline conditions than that under acidic conditions due to the presence of 10 μtmol/L arsenate. The presence of 20 μmol/L arsenate slightly improved chromium removal by Fe（Ⅱ） at pH 3.9-5,8, but had detrimental effects at pH 6.7-9.8. Arsenate removal was improved significantly at pH 4-9 due to the presence of 10μmol/L chromate at Fe（Ⅱ） dosages of 20-60 μmol/L. Elevating the chromate concentration from 10 to 20μmol/L resulted in a further improvement in arsenate removal at pH 4.0-4.6 when Fe（Ⅱ） was dosed at 30-60 μmol/L.
