We report here arsenic speciation in 1643 freshwater fish samples,representing 14 common fish species from 53 waterbodies in Alberta,Canada.Arsenic species were extracted from fish muscle tissue.Arsenic species in the...We report here arsenic speciation in 1643 freshwater fish samples,representing 14 common fish species from 53 waterbodies in Alberta,Canada.Arsenic species were extracted from fish muscle tissue.Arsenic species in the extracts were separated using anion-exchange high-performance liquid chromatography(HPLC)and quantified using inductively coupled plasma mass spectrometry(ICPMS).The total arsenic concentrations in fish ranged from 2.8 to 1200μg/kg(in wet weight of sample)(mean 71±101μg/kg),which are all below the 2000μg/kg(wet weight)maximum allowable total arsenic in fish,recommended by the Ontario Ministry of the Environment.In 99.7%,or 1638 of all 1643 freshwater fish samples analyzed,arsenobetaine(AsB)was detectable,with concentrations higher than the method detection limit of 0.25μg/kg(wet weight).Dimethylarsinic acid(DMA)was detectable(concentration>0.25μg/kg)in 92.1%,or 1514 of the 1643 freshwater fish samples.Inorganic arsenate(iAs^(Ⅴ))was detectable(>0.25μg/kg)in 1119 fish(i.e.,68.1% of 1643 samples).Monomethylarsonic acid(MMA)was detectable(>0.25μg/kg)in 418 fish(25.4%of 1643 samples).The concentrations of arsenic species in the 1643 fish samples varied by as much as three orders of magnitude,ranging from below the method detection limit of 0.25μg/kg to the maximum concentrations of 380μg/kg for AsB,150μg/kg for DMA,70μg/kg for iAs^(Ⅴ),and 51μg/kg for MMA.AsB made up 46.1%±26.2% of total arsenic species.Arsenic speciation patterns varied between lake whitefish,northern pike,and walleye,the three most common types of fish analyzed.The relative proportion of DMA in northern pike was larger than in lake whitefish and walleye,and conversely,the relative proportion of iAs^(Ⅴ) was lower in northern pike.Seven unknown arsenic species were detected,and their chromatographic retention time did not match with those of available arsenic standards.At least one unknown arsenic species was detected in 33.4%,or 549 of 1643 freshwater fish samples.The concentrations of unknown arsenic species were as high as 61μg/kg.Future research is necessary to identify unknown arsenic species and to determine contributing factors to the observed arsenic species patterns and concentrations.展开更多
Arsenic speciation in freshwater fish is crucial for providing meaningful consumption guidelines that allow the public to make informed decisions regarding its consumption.While marine fish have attractedmuch research...Arsenic speciation in freshwater fish is crucial for providing meaningful consumption guidelines that allow the public to make informed decisions regarding its consumption.While marine fish have attractedmuch research interest due to their higher arsenic content,research on freshwater fish is limited due to the challenges in quantifying and identifying arsenic species present at trace levels.We describe here a sensitivemethod and its application to the quantification of arsenic species in freshwater fish.Arsenic species from fish tissues were extracted using a methanol/water mixture(1:1 vol.ratio)and ultrasound sonication.Anion-exchange high-performance liquid chromatography(HPLC)enabled separation of arsenobetaine(AsB),inorganic arsenite(iAs^(Ⅲ)),dimethylarsinic acid(DMA),monomethylarsonic acid(MMA),inorganic arsenate(iAs^(Ⅴ)),and three new arsenic species.Inductively coupled plasma mass spectrometry(ICPMS)provided highly sensitive and specific detection of arsenic.A limit of detection of 0.25μg/kg(wet weight fish tissue)was achieved for the five target arsenic species:AsB,iAs^(Ⅲ),DMA,MMA,and iAs^(Ⅴ).A series of experimentswere conducted to ensure the accuracy and validity of the analytical method.The method was successfully applied to the determination of arsenic species in lakewhitefish,northern pike,and walleye,with AsB,DMA,and iAs^(Ⅴ) being frequently detected.Three new arsenic species were detected,but their chromatographic retention times did not match with those of any available arsenic standards.Future research is necessary to elucidate the identity of these new arsenic species detected in freshwater fish.展开更多
Methylmercury （MeHg） is an organic form of the global pollutant mercury （Hg） which readily accumulates in fish tissue. A majority of Hg methylation is a result of microbial activity and the abundance of inorganic ...Methylmercury （MeHg） is an organic form of the global pollutant mercury （Hg） which readily accumulates in fish tissue. A majority of Hg methylation is a result of microbial activity and the abundance of inorganic Hg within the water reservoirs （Eckley et al., 2017）. Compared to natural lakes and rivers, reservoirs have elevated Hg levels from the decompo- sition of recently flooded organic material which promote Hg release and enhance microbial methylation of Hg （Eckley et al., 2017）. Microorganisms containing the gene clusters hgcA and hgcB, such as sulfate reducing bacteria （SRB） and iron reducing bacteria （FeRB）.展开更多
Cadmium (Cd) is a toxic metal with high mobility from soil and known translocation into plants (Song et al., 2015).Because the main source of human exposure to Cd is from food consumption, there has been increased res...Cadmium (Cd) is a toxic metal with high mobility from soil and known translocation into plants (Song et al., 2015).Because the main source of human exposure to Cd is from food consumption, there has been increased research examining Cd uptake in agricultural plants (Li et al., 2014;Rizwan et al., 2016;Song et al., 2015).展开更多
Food and water are the main sources of human exposure to arsenic.It is important to determine arsenic species in food because the toxicities of arsenic vary greatly with its chemical speciation.Extensive research has ...Food and water are the main sources of human exposure to arsenic.It is important to determine arsenic species in food because the toxicities of arsenic vary greatly with its chemical speciation.Extensive research has focused on high concentrations of arsenic species in marine organisms.The concentrations of arsenic species in freshwater fish are much lower,and their determination presents analytical challenges.In this review,we summarize the current state of knowledge on arsenic speciation in freshwater fish and discuss challenges and research needs.Fish samples are typically homogenized,and arsenic species are extracted using water/methanol with the assistance of sonication and enzyme treatment.Arsenic species in the extracts are commonly separated using high-performance liquid chromatography(HPLC)and detected using inductively coupled plasma mass spectrometry(ICPMS).Electrospray ionization tandem mass spectrometry,used in combination with HPLC and ICPMS,provides complementary information for the identification and characterization of arsenic species.The methods and perspectives discussed in this review,covering sample preparation,chromatography separation,and mass spectrometry detection,are directed to arsenic speciation in freshwater fish and applicable to studies of other food items.Despite progress made in arsenic speciation analysis,a large fraction of the total arsenic in freshwater fish remains unidentified.It is challenging to identify and quantify arsenic species present in complex sample matrices at very low concentrations.Further research is needed to improve the extraction efficiency,chromatographic resolution,detection sensitivity,and characterization capability.展开更多
基金supported by Alberta Health,Alberta Innovates,the Canada Research Chairs program,the Canadian Institutes of Health Research,and the Natural Sciences and Engineering Research Council of Canada.
文摘We report here arsenic speciation in 1643 freshwater fish samples,representing 14 common fish species from 53 waterbodies in Alberta,Canada.Arsenic species were extracted from fish muscle tissue.Arsenic species in the extracts were separated using anion-exchange high-performance liquid chromatography(HPLC)and quantified using inductively coupled plasma mass spectrometry(ICPMS).The total arsenic concentrations in fish ranged from 2.8 to 1200μg/kg(in wet weight of sample)(mean 71±101μg/kg),which are all below the 2000μg/kg(wet weight)maximum allowable total arsenic in fish,recommended by the Ontario Ministry of the Environment.In 99.7%,or 1638 of all 1643 freshwater fish samples analyzed,arsenobetaine(AsB)was detectable,with concentrations higher than the method detection limit of 0.25μg/kg(wet weight).Dimethylarsinic acid(DMA)was detectable(concentration>0.25μg/kg)in 92.1%,or 1514 of the 1643 freshwater fish samples.Inorganic arsenate(iAs^(Ⅴ))was detectable(>0.25μg/kg)in 1119 fish(i.e.,68.1% of 1643 samples).Monomethylarsonic acid(MMA)was detectable(>0.25μg/kg)in 418 fish(25.4%of 1643 samples).The concentrations of arsenic species in the 1643 fish samples varied by as much as three orders of magnitude,ranging from below the method detection limit of 0.25μg/kg to the maximum concentrations of 380μg/kg for AsB,150μg/kg for DMA,70μg/kg for iAs^(Ⅴ),and 51μg/kg for MMA.AsB made up 46.1%±26.2% of total arsenic species.Arsenic speciation patterns varied between lake whitefish,northern pike,and walleye,the three most common types of fish analyzed.The relative proportion of DMA in northern pike was larger than in lake whitefish and walleye,and conversely,the relative proportion of iAs^(Ⅴ) was lower in northern pike.Seven unknown arsenic species were detected,and their chromatographic retention time did not match with those of available arsenic standards.At least one unknown arsenic species was detected in 33.4%,or 549 of 1643 freshwater fish samples.The concentrations of unknown arsenic species were as high as 61μg/kg.Future research is necessary to identify unknown arsenic species and to determine contributing factors to the observed arsenic species patterns and concentrations.
基金supported by Alberta Health,Alberta Innovates,the Canada Research Chairs Program,the Canadian Institutes of Health Research,and the Natural Sciences and Engineering Research Council of Canada。
文摘Arsenic speciation in freshwater fish is crucial for providing meaningful consumption guidelines that allow the public to make informed decisions regarding its consumption.While marine fish have attractedmuch research interest due to their higher arsenic content,research on freshwater fish is limited due to the challenges in quantifying and identifying arsenic species present at trace levels.We describe here a sensitivemethod and its application to the quantification of arsenic species in freshwater fish.Arsenic species from fish tissues were extracted using a methanol/water mixture(1:1 vol.ratio)and ultrasound sonication.Anion-exchange high-performance liquid chromatography(HPLC)enabled separation of arsenobetaine(AsB),inorganic arsenite(iAs^(Ⅲ)),dimethylarsinic acid(DMA),monomethylarsonic acid(MMA),inorganic arsenate(iAs^(Ⅴ)),and three new arsenic species.Inductively coupled plasma mass spectrometry(ICPMS)provided highly sensitive and specific detection of arsenic.A limit of detection of 0.25μg/kg(wet weight fish tissue)was achieved for the five target arsenic species:AsB,iAs^(Ⅲ),DMA,MMA,and iAs^(Ⅴ).A series of experimentswere conducted to ensure the accuracy and validity of the analytical method.The method was successfully applied to the determination of arsenic species in lakewhitefish,northern pike,and walleye,with AsB,DMA,and iAs^(Ⅴ) being frequently detected.Three new arsenic species were detected,but their chromatographic retention times did not match with those of any available arsenic standards.Future research is necessary to elucidate the identity of these new arsenic species detected in freshwater fish.
文摘Methylmercury （MeHg） is an organic form of the global pollutant mercury （Hg） which readily accumulates in fish tissue. A majority of Hg methylation is a result of microbial activity and the abundance of inorganic Hg within the water reservoirs （Eckley et al., 2017）. Compared to natural lakes and rivers, reservoirs have elevated Hg levels from the decompo- sition of recently flooded organic material which promote Hg release and enhance microbial methylation of Hg （Eckley et al., 2017）. Microorganisms containing the gene clusters hgcA and hgcB, such as sulfate reducing bacteria （SRB） and iron reducing bacteria （FeRB）.
文摘Cadmium (Cd) is a toxic metal with high mobility from soil and known translocation into plants (Song et al., 2015).Because the main source of human exposure to Cd is from food consumption, there has been increased research examining Cd uptake in agricultural plants (Li et al., 2014;Rizwan et al., 2016;Song et al., 2015).
基金This work was supported by Alberta Health,Alberta Innovates,the Canada Research Chairs Program,the Canadian Institutes of Health Research,and the Natural Sciences and Engineering Research Council of Canada.
文摘Food and water are the main sources of human exposure to arsenic.It is important to determine arsenic species in food because the toxicities of arsenic vary greatly with its chemical speciation.Extensive research has focused on high concentrations of arsenic species in marine organisms.The concentrations of arsenic species in freshwater fish are much lower,and their determination presents analytical challenges.In this review,we summarize the current state of knowledge on arsenic speciation in freshwater fish and discuss challenges and research needs.Fish samples are typically homogenized,and arsenic species are extracted using water/methanol with the assistance of sonication and enzyme treatment.Arsenic species in the extracts are commonly separated using high-performance liquid chromatography(HPLC)and detected using inductively coupled plasma mass spectrometry(ICPMS).Electrospray ionization tandem mass spectrometry,used in combination with HPLC and ICPMS,provides complementary information for the identification and characterization of arsenic species.The methods and perspectives discussed in this review,covering sample preparation,chromatography separation,and mass spectrometry detection,are directed to arsenic speciation in freshwater fish and applicable to studies of other food items.Despite progress made in arsenic speciation analysis,a large fraction of the total arsenic in freshwater fish remains unidentified.It is challenging to identify and quantify arsenic species present in complex sample matrices at very low concentrations.Further research is needed to improve the extraction efficiency,chromatographic resolution,detection sensitivity,and characterization capability.
