Arsenic（As） is a notoriously toxic pollutant of health concern worldwide with potential risk of cancer induction, but meanwhile it is used as medicines for the treatment of different conditions including hematologic...Arsenic（As） is a notoriously toxic pollutant of health concern worldwide with potential risk of cancer induction, but meanwhile it is used as medicines for the treatment of different conditions including hematological cancers. Arsenic can undergo extensive metabolism in biological systems, and both toxicological and therapeutic effects of arsenic compounds are closely related to their metabolism. Recent studies have identified methylated thioarsenicals as a new class of arsenic metabolites in biological systems after exposure of inorganic and organic arsenicals, including arsenite, dimethylarsinic acid（DMAV）, dimethylarsinous glutathione（DMAIIIGS）, and arsenosugars. The increasing detection of thiolated arsenicals,including monomethylmonothioarsonic acid（MMMTAV）, dimethylmonothioarsinic acid（DMMTAV） and its glutathione conjugate（DMMTAVGS）, and dimethyldithioarsinic acid（DMDTAV） suggests that thioarsenicals may be important metabolites and play important roles in arsenic toxicity and therapeutic effects. Here we summarized the reported occurrence of thioarsenicals in biological systems, the possible formation pathways of thioarsenicals, and their toxicity, and discussed the biological implications of thioarsenicals on arsenic metabolism, toxicity, and therapeutic effects.展开更多
For much of the world＇s population, food is the major source of exposure to arsenic.Exposure to this non-essential metalloid at relatively low levels may be linked to a wide range of adverse health effects. Thus, eva...For much of the world＇s population, food is the major source of exposure to arsenic.Exposure to this non-essential metalloid at relatively low levels may be linked to a wide range of adverse health effects. Thus, evaluating foods as sources of exposure to arsenic is important in assessing risk and developing strategies that protect public health. Although most emphasis has been placed on inorganic arsenic as human carcinogen and toxicant, an array of arsenic-containing species are found in plants and animals used as foods. Here,we 2evaluate the contribution of complex organic arsenicals（arsenosugars, arsenolipids,and trimethylarsonium compounds） that are found in foods and consider their origins,metabolism, and potential toxicity. Commonalities in the metabolism of arsenosugars and arsenolipids lead to the production of di-methylated arsenicals which are known to exert many toxic effects. Evaluating foods as sources of exposure to these complex organic arsenicals and understanding the formation of reactive metabolites may be critical in assessing their contribution to aggregate exposure to arsenic.展开更多
Uranyl arsenate minerals,which exhibit low solubility,serve as major sinks for U and As,playing a crucial role in controlling the mobility of U and As in the environment.However,the specific mechanisms underly-ing the...Uranyl arsenate minerals,which exhibit low solubility,serve as major sinks for U and As,playing a crucial role in controlling the mobility of U and As in the environment.However,the specific mechanisms underly-ing the formation of uranyl arsenate minerals have remained largely elusive.Herein,the formation pathway of the non-charged UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O0 complex was investigated to elucidate the early formation of the UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O mineral(where n represents the stoichiometric number of H_(2)O),a representative uranyl arsenate mineral.Based on the combination experiments of U(VI)and As(V),our findings underscore the sig-nificant dependence of UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O0 formation on solution pH(4.0–10.0).Density functional theory(DFT)calculations reveal a two-step reaction involving two distinct pathways(Pathway 1 and Pathway 2)for the formation of UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O,and the intermediate was confirmed by in situ Raman and fluorescence spec-troscopy.Specifically,the hydroxyl‑connected uranyl(UO_(2)OH^(+))reacts with the protonated arsenate(H_(2)AsO_(4)^(-))species to form the intermediate UO_(2)HAsO4·H_(2)O(Pathway 1)or UO_(2)OH–H2AsO4(Pathway 2)with a U/As ratio of 1:1.Meanwhile,all the transition states also were obtained and the energy barrier suggested that the UO_(2)(H_(2)AsO_(4))_(2)·2H_(2)O0 formed by Pathway 1 is thermodynamically favored over Pathway 2,and may serve as the primary fundamental structural unit or precursor for the early formation of the UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O mineral phase.Altogether,this study contributes to advancing the understanding of the formation of uranyl arsenate min-erals at the molecular scale and provides a theoretical basis for predicting and regulating uranium and arsenic mobilization in their coexisting environment.展开更多
Industrial activities have caused widespread arsenic(As)contamination in soil and medicinal crops across south-ern Asia.This study constructed interplanting systems combing medicinal crops with Pteris vittata L.,aimin...Industrial activities have caused widespread arsenic(As)contamination in soil and medicinal crops across south-ern Asia.This study constructed interplanting systems combing medicinal crops with Pteris vittata L.,aiming to mitigate the risk of As exposure in medicinal crops,while simultaneously achieving ecological remediation of contaminated soil.The results revealed that interplanting with P.vittata significantly enhanced the yield of Gynos-temma pentaphyllum by 31.90%(P<0.05)compared with monoculture systems.Under monoculture conditions,the As concentration in G.pentaphyllum leaves reached 2.34 mg/kg,exceeding the national food safety standard(GB2762–2017,2 mg/kg).However,interplanting with P.vittata effectively reduced the As concentration in G.pentaphyllum leaves to 1.82 mg/kg.Furthermore,the interplanting of P.vittata with Rhus chinensis significantly inhibited As translocation from belowground to aboveground tissues in R.chinensis.Compared to monoculture,the stem biomass of P.vittata was significantly increased by 57.50%and 70.32%when interplanted with G.pentaphyllum and Cassia obtusifolia L.(P<0.05).So the As enrichment of P.vittata was enhanced in interplanting systems,which is beneficial for the As removal from contaminated soil.The study demonstrated that interplant-ing primarily regulates plant As uptake through modifications of rhizosphere physicochemical properties and As bioavailability,especially for water-soluble As that is easily absorbed by plants.In conclusion,the interplant-ing models integrating medicinal crops and P.vittata can achieve the goal of“remediating while producing”in As-contaminated soil.展开更多
The volatilization characteristics and kinetic mechanisms of arsenic were investigated in the temperature range of 623−773 K and pressure ranges of 10−10000 Pa.The experimental results reveal that the evaporation rate...The volatilization characteristics and kinetic mechanisms of arsenic were investigated in the temperature range of 623−773 K and pressure ranges of 10−10000 Pa.The experimental results reveal that the evaporation rate increases with increasing temperature and decreasing pressure.Surface reaction control dominates at low pressures(<100 Pa),whereas diffusion control dominates at high pressures(>5000 Pa).The evaporation behavior is successfully described by an Arrhenius-type model for temperature dependence and Logistic model for pressure dependence.Key kinetic parameters,including the critical pressure,maximum evaporation rate and evaporation coefficient,were calculated.The evaporation coefficient varies between 0.010 and 0.223,and the critical pressures vary between 281 and 478 Pa with temperature.展开更多
This study investigates the performance enhancement of super-sulfated cement(SSC)derived from arsenic-containing bio-oxidation waste(BW)through the incorporation of carbonated recycled concrete fines(CRCF).The finding...This study investigates the performance enhancement of super-sulfated cement(SSC)derived from arsenic-containing bio-oxidation waste(BW)through the incorporation of carbonated recycled concrete fines(CRCF).The findings revealed that the addition of 5wt%CRCF yields optimal performance,with compressive strengths reaching approximately 1.83,12.59,and 42.81 MPa at 1,3,and 28 d,respectively.These values represented significant increases of 408.3%,10.0%,and 14.3%compared to the reference sample.The improvement was attributed to the synergistic effects of ultrafine CRCF particles acting as fillers and nucleation sites,as well as the high reactivity of silica gels,which promoted the formation of additional hydration gels.Microstructural analysis confirmed that CRCF addition refined pore structure,and enhanced the stiffness of C-S-H gels.Furthermore,CRCF served as a net CO_(2) sink,sequestering 0.268 kg CO_(2) per kilogram of CRCF and thereby reducing the carbon footprint of SSC.In addition,the feasibility of applying CRCF-modified SSC in cemented paste backfill(CPB)is highlighted,given the high cement-related carbon footprint of conventional CPB.When 5wt%CRCFmodified SSC was employed in CPB,its 3-d compressive strength attained over 70%of that of ordinary Portland cement(OPC),while the 28-d strength was comparable to that of OPC.The proposed binder thus provides a sustainable pathway for BW valorization,combining waste utilization,carbon sequestration,and improved engineering performance.展开更多
Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for ...Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.展开更多
In this study,synthetic wastewater containing 110μg/L arsenate(As(V)),0-20 mg/L fulvic acid(FA),and 0-12.3 mg/L phosphate was treated with 3 mg/L Fe3+.The mechanisms of FA and phosphate effects on As(V)removal by fer...In this study,synthetic wastewater containing 110μg/L arsenate(As(V)),0-20 mg/L fulvic acid(FA),and 0-12.3 mg/L phosphate was treated with 3 mg/L Fe3+.The mechanisms of FA and phosphate effects on As(V)removal by ferric chloride were determined using 0.22-10μm pore-size filtration,Zetasizer analysis,and in situ flow through cell ATR-FTIR.The results showed that up to 20mg/L FA had almost no effect on the solubility of ferric hydroxide precipitates and adsorption of As(V)by the precipitates.When FA concentration increased from 0 to 20 mg/L,the adsorption of FA led to higher negative zeta potential of the precipitates and the strong electrostatic repulsion between the precipitates decreased the particle size of ferric hydroxide flocs fromlarger than 10μmto smaller than 1μm.In the presence of 5-20 mg/L FA,46%-63%As(V)was adsorbed onto the flocs with particle size in the range of 0.45-1μm.On the other hand,phosphate did not affect the size of ferric hydroxide flocs and significantly increased the dissolved As(V)concentration because it competed with As(V)for adsorption sites on ferric hydroxide precipitates.The addition of 5mg/L cationic organic flocculant significantly reduced the effect of FA on As(V)removal,but did not reduce the effect of phosphate on As(V)removal.The findings of this study will help develop effective arsenic treatment techniques and predict the mobility of arsenic in the environment.展开更多
Arsenic(As)pollution seriously threatens human and ecological health.Microalgal cell wall and extracellular polymeric substances(EPS)are known to interactwith As,but their roles in the As resistance,accumulation and s...Arsenic(As)pollution seriously threatens human and ecological health.Microalgal cell wall and extracellular polymeric substances(EPS)are known to interactwith As,but their roles in the As resistance,accumulation and speciation inmicroalgae remain unclear.Here,we used two strains of Chlamydomonas reinhardtii,namely CC-125(wild type)and CC-503(cell walldeficientmutant),to examine the algal growth,EPS synthesis,As adsorption,absorption and transformation under 10–1000μg/L As(III)and As(V)treatments for 96 h.In both strains,the As absorption increased after the EPS removal,but the growth,As adsorption,and transformation of C.reinhardtii declined.The CC-125 strain was more tolerant to As stress and more efficient in EPS production,As accumulation,and redox transformation than CC-503,irrespective of EPS presence or absence.Three-dimension excitation-emission matrix(3DEEM)and attenuated total reflectance infrared spectroscopy(ATR-IR)analyses showed that As was bound with functional groups in the EPS and cell wall,such as-COOH,NH and-OH in proteins,polysaccharides and amino acids.Together,this study demonstrated that EPS and cell wall acted as barriers to lower the As uptake by C.reinhardtii.However,the cell wall mutant strain wasmore susceptible to As toxicity due to lower EPS induction and higher As absorption.展开更多
With the increasing severity of arsenic(As)pollution,quantifying the environmental behavior of pollutant based on numerical model has become an important approach to determine the potential impacts and finalize the pr...With the increasing severity of arsenic(As)pollution,quantifying the environmental behavior of pollutant based on numerical model has become an important approach to determine the potential impacts and finalize the precise control strategies.Taking the industrialintensive Jinsha River Basin as typical area,a two-dimensional hydrodynamic water quality model coupled with Soil andWater Assessment Tool(SWAT)model was developed to accurately simulate the watershed-scale distribution and transport of As in the terrestrial and aquatic environment at high spatial and temporal resolution.The effects of hydro-climate change,hydropower station construction and non-point source emissions on Aswere quantified based on the coupled model.The result indicated that higher As concentration areas mainly centralized in urban districts and concentration slowly decreased from upstream to downstream.Due to the enhanced rainfall,the As concentration was significantly higher during the rainy season than the dry season.Hydro-climate change and the construction of hydropower station not only affected the dissolved As concentration,but also affected the adsorption and desorption of As in sediment.Furthermore,As concentration increased with the input of non-point source pollution,with the maximum increase about 30%,resulting that non-point sources contributed important pollutant impacts to waterways.The coupled model used in pollutant behavior analysis is generalwith high potential application to predict and mitigate water pollution.展开更多
Arsenic and cadmium contamination frequently coexist in the real environment.However it remains a challenge for their simultaneous removal due to their distinct physicochemica properties at low cost.To this end,a cost...Arsenic and cadmium contamination frequently coexist in the real environment.However it remains a challenge for their simultaneous removal due to their distinct physicochemica properties at low cost.To this end,a cost-effective magnetic biochar adsorbent (ITBNa800was prepared using biomass waste and iron tailings slag.This composite adsorbent exhibits excellent performance in the simultaneous removal of aqueous As(Ⅴ) and Cd(Ⅱ) even at high concentrations with removal efficiencies of up to 99.98%and 96.04%,respectively.Electro static action,precipitation,and complexation were adsorption mechanisms.As(Ⅴ) and Cd(Ⅱ were synergistic and competitive adsorption.As(Ⅴ) removal was mainly due to physical and chemical adsorption,and 42.40%-58.59%of As(Ⅴ) had been converted to As(Ⅲ ).Cd(Ⅱ) re moval was mainly due to chemical adsorption.Iron oxide and aluminum oxide in ITBNa800were the keys to As(Ⅴ),As(Ⅲ ),and Cd(Ⅱ) adsorption.DFT calculations revealed iron oxide complex As(Ⅴ),As(Ⅲ ),and Cd(Ⅱ) molecular clusters through bidentate binuclear,bidentate binuclear,and monodentate binuclear pathways,respectively.Aluminum oxide complex Cd(Ⅱ) molecular cluster through a bidentate mononuclear pathway.We hope the ITBNa800adsorbent and its involved mechanism could offer inspiration in the simultaneous treat ment of As and Cd pollution.展开更多
The Qinghai-Tibet Plateau,with its high altitude and cold climate,is one of the most fragile ecological environments in China and is distinguished by its naturally elevated arsenic(As)levels in the soil,largely due to...The Qinghai-Tibet Plateau,with its high altitude and cold climate,is one of the most fragile ecological environments in China and is distinguished by its naturally elevated arsenic(As)levels in the soil,largely due to its rich mineral and geothermal resources.This review provides a comprehensive analysis of As content,focusing on its distribution,environmental migration,and transformation behavior across the plateau.The review further evaluates the distribution of As in different functional areas,revealing that geothermal fields(107.2 mg/kg),mining areas(53.8 mg/kg),and croplands(39.3 mg/kg)have the highest As concentrations,followed by river and lake sediments and adjacent areas(33.1 mg/kg).These elevated levels are primarily attributed to the presence of As-rich minerals,such as arsenopyrite and pyrite.Additionally,human activities,including mining and geothermal energy production,exacerbate the release of As into the environment.The review also highlights the role of localmicroorganisms,particularly those fromthe phyla Proteobacteria and Actinobacteria,which possess As metabolic genes that facilitate As translocation.Given the unique climatic conditions of the plateau,conventionalmethods for As controlmay not be fully effective.However,the review identifies promising remediation strategies that are environmentally adaptable,such as the use of local microorganisms,specific adsorbents,and integrated technologies,which offer potential solutions for managing and utilizing Ascontaminated soils on the plateau.展开更多
Arsenic(As)methylation in soils affects the environmental behavior of As,excessive accumulation of dimethylarsenate(DMA)in rice plants leads to straighthead disease and a serious drop in crop yield.Understanding the m...Arsenic(As)methylation in soils affects the environmental behavior of As,excessive accumulation of dimethylarsenate(DMA)in rice plants leads to straighthead disease and a serious drop in crop yield.Understanding the mobility and transformation of methylated arsenic in redox-changing paddy fields is crucial for food security.Here,soils including unarsenic contaminated(N-As),low-arsenic(L-As),medium-arsenic(M-As),and high-arsenic(H-As)soils were incubated under continuous anoxic,continuous oxic,and consecutive anoxic/oxic treatments respectively,to profile arsenic methylating process and microbial species involved in the As cycle.Under anoxic-oxic(A-O)treatment,methylated arsenic was significantly increased once oxygen was introduced into the incubation system.The methylated arsenic concentrations were up to 2-24 times higher than those in anoxic(A),oxic(O),and oxic-anoxic(O-A)treatments,under which arsenic was methylated slightly and then decreased in all four As concentration soils.In fact,the most plentiful arsenite S-adenosylmethionine methyltransferase genes(arsM)contributed to the increase in As methylation.Proteobacteria(40.8%-62.4%),Firmicutes(3.5%-15.7%),and Desulfobacterota(5.3%-13.3%)were the major microorganisms related to this process.These microbial increasedmarkedly and played more important roles after oxygen was introduced,indicating that they were potential keystone microbial groups for As methylation in the alternating anoxic(flooding)and oxic(drainage)environment.The novel findings provided newinsights into the reoxidation-driven arsenic methylation processes and the model could be used for further risk estimation in periodically flooded paddy fields.展开更多
Arsenic(As)pollution in soils is a pervasive environmental issue.Biochar immobilization offers a promising solution for addressing soil As contamination.The efficiency of biochar in immobilizing As in soils primarily ...Arsenic(As)pollution in soils is a pervasive environmental issue.Biochar immobilization offers a promising solution for addressing soil As contamination.The efficiency of biochar in immobilizing As in soils primarily hinges on the characteristics of both the soil and the biochar.However,the influence of a specific property on As immobilization varies among different studies,and the development and application of arsenic passivation materials based on biochar often rely on empirical knowledge.To enhance immobilization efficiency and reduce labor and time costs,a machine learning(ML)model was employed to predict As immobilization efficiency before biochar application.In this study,we collected a dataset comprising 182 data points on As immobilization efficiency from 17 publications to construct three ML models.The results demonstrated that the random forest(RF)model outperformed gradient boost regression tree and support vector regression models in predictive performance.Relative importance analysis and partial dependence plots based on the RF model were conducted to identify the most crucial factors influencing As immobilization.These findings highlighted the significant roles of biochar application time and biochar pH in As immobilization efficiency in soils.Furthermore,the study revealed that Fe-modified biochar exhibited a substantial improvement in As immobilization.These insights can facilitate targeted biochar property design and optimization of biochar application conditions to enhance As immobilization efficiency.展开更多
In this study,we investigated improving the performance of a layered double hydroxide(LDH)for the adsorption of As(III)and As(V)by controlling the morphology of LDH crystals.The LDH was synthesized via a simple coprec...In this study,we investigated improving the performance of a layered double hydroxide(LDH)for the adsorption of As(III)and As(V)by controlling the morphology of LDH crystals.The LDH was synthesized via a simple coprecipitation method using barely soluble MgO as a precursor and succinic acid(SA)as a morphological control agent.Doping the LDH crystals with carboxylate ions(RCOO−)derived from SA caused the crystals to develop in a radial direction.This changed the pore characteristics and increased the density of active surface sites.Subsequently,SA/MgFe-LDH showed excellent affinity for As(III)and As(V)with maximum sorption densities of 2.42 and 1.60 mmol/g,respectively.By comparison,the pristine MgFe-LDH had sorption capacities of 1.56 and 1.31 mmol/g for As(III)and As(V),respectively.The LDH was effective over a wide pH range for As(III)adsorption(pH 3-8.5)and As(V)adsorption(pH 3-6.5).Using a combination of spectroscopy and sorption modeling calculations,the main sorption mechanism of As(III)and As(V)on SA/MgFe-LDH was identified as inner-sphere complexation via ligand exchangewith hydroxyl group(-OH)and RCOO−.Specifically,bidentate As-Fe complexeswere proposed for both As(III)and As(V)uptake,with the magnitude of formation varying with the initial As concentration.Importantly,the As-laden adsorbent had satisfactory stability in simulated real landfill leachate.These findings demonstrate that SA/MgFe-LDH exhibits considerable potential for remediation of As-contaminated water.展开更多
Rapid screening of inorganic arsenic(iAs)in groundwater used for drinking by hundreds of millions of mostly rural residents worldwide is crucial for health protection.Most commercial field test kits are based on the G...Rapid screening of inorganic arsenic(iAs)in groundwater used for drinking by hundreds of millions of mostly rural residents worldwide is crucial for health protection.Most commercial field test kits are based on the Gutzeit reaction that uses mercury-based reagents for color development,an environmental concern that increasingly limits its utilization.This study further improves the Molybdenum Blue(MB)colorimetric method to allow for faster screening with more stable reagents.More importantly,a portable three-channel colorimeter is developed for screening iAs relative to the WHO drinking water guideline value(10μg/L).Adding the reducing reagents in sequence not only prolongs the storage time to>7 days,but also accelerates the color development time to 6 min in conjunction with lowering the H_(2)SO_(4) concentration in chromogenic reagents.The optimal pH ranges from 1.2 to 1.3 and is achieved by acidifying groundwater to 1%(V/V)HCl.With detection limits of 3.7μg/L for inorganic arsenate(iAs(V))and 3.8μg/L for inorganic arsenite(iAs(Ⅲ)),testing groundwater with-10μg/L of As has a precision<20%.The method works well for a range of phosphate concentrations of 48-950μg/L(0.5-10μmol/L).Concentrations of total_iAs(6-300μg/L),iAs(V)(6-230μg/L)and iAs(Ⅲ)(0-170μg/L)for 14 groundwater samples from Yinchuan Plain,Pearl River Delta,and Jianghan Plain,are in excellent agreements(linear regression slope:0.969-1.029)with the benchmark methods.The improved chemistry here lays the foundation for the MB colorimetric method to become a commercially viable screening tool,with further engineering and design improvement of the colorimeter.展开更多
Arsenic(As)contamination in paddy soils has posed a prominent threat to rice production in Asia.Recycling of silicon(Si)from Si-rich combusted rice husk(CRH)could serve as a sustainable strategy to mitigate rice As up...Arsenic(As)contamination in paddy soils has posed a prominent threat to rice production in Asia.Recycling of silicon(Si)from Si-rich combusted rice husk(CRH)could serve as a sustainable strategy to mitigate rice As uptake through their shared transport pathway.Root(soil)application of CRH alone,however,was insufficient to decrease inorganic As(iAs)in polished rice below Chinese food standards(0.2 mg kg^(-1)).In this study,an aqueous Si solution derived from CRH was used for synergistic foliar application over the highest Si-demanding stage(reproductive stage)of rice,following root application of Si,to investigate rice As uptake in both pot and field experiments.In the pot experiment,on the basis of root application of CRH,Si supplementation before the reproductive stage of rice led to a 51%decrease in As concentration on root surface along with a prominent reduction of Fe plaque due to enhanced root suberization,relative to single root application of CRH treatment.In parallel,the expression of OsLis6 gene in the root was downregulated by 91%than that with only root application of CRH.These changes decreased As influx into root by 56%and led correspondingly to 41%lower As transfer to the straw,as compared with root application of CRH treatment.In node I,the expression of OsLis6 decreased concurrently by 71%,leading ultimately to 28%lower iAs accumulation in grains than that with root application of CRH alone.In the field experiment,with single foliar Si,the mitigation of grain iAs occurred only at lower soil As level of 40 mg kg^(-1),while promoted iAs unloading into grains was determined under higher soil As level(80 mg kg^(-1))relative to the control without Si application.It was,therefore,concluded that the mitigation of grain iAs accumulation with soil application of CRH can be strengthened critically by synergistic supply of foliar Si,serving as a more reliable pathway to secure rice production in As-contaminated paddy fields.展开更多
Arsenic-related oxidative stress and resultant diseases have attracted global concern,while longitudinal studies are scarce.To assess the relationship between arsenic exposure and systemic oxidative damage,we performe...Arsenic-related oxidative stress and resultant diseases have attracted global concern,while longitudinal studies are scarce.To assess the relationship between arsenic exposure and systemic oxidative damage,we performed two repeatedmeasures among 5236 observations(4067 participants)in theWuhan-Zhuhai cohort at the baseline and follow-up after 3 years.Urinary total arsenic,biomarkers of DNA oxidative damage(8-hydroxy-2-deoxyguanosine(8-OHdG)),lipid peroxidation(8-isoprostaglandin F2alpha(8-isoPGF2α)),and protein oxidative damage(protein carbonyls(PCO))were detected for all observations.Here we used linearmixed models to estimate the cross-sectional and longitudinal associations between arsenic exposure and oxidative damage.Exposure-response curves were constructed by utilizing the generalized additive mixed models with thin plate regressions.After adjusting for potential confounders,arsenic level was significantly and positively related to the levels of global oxidative damage and their annual increased rates in dose-response manners.In cross-sectional analyses,each 1%increase in arsenic levelwas associated with a 0.406%(95%confidence interval(CI):0.379%to 0.433%),0.360%(0.301%to 0.420%),and 0.079%(0.055%to 0.103%)increase in 8-isoPGF2α,8-OHdG,and PCO,respectively.More importantly,arsenic was further found to be associated with increased annual change rates of 8-isoPGF2α(β:0.147;95%CI:0.130 to 0.164),8-OHdG(0.155;0.118 to 0.192),and PCO(0.050;0.035 to 0.064)in the longitudinal analyses.Our study suggested that arsenic exposurewas not only positively related with global oxidative damage to lipid,DNA,and protein in cross-sectional analyses,but also associated with annual increased rates of these biomarkers in dose-dependent manners.展开更多
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
基金sponsored by the National Natural Science Foundation of China (No. 91543103)
文摘Arsenic（As） is a notoriously toxic pollutant of health concern worldwide with potential risk of cancer induction, but meanwhile it is used as medicines for the treatment of different conditions including hematological cancers. Arsenic can undergo extensive metabolism in biological systems, and both toxicological and therapeutic effects of arsenic compounds are closely related to their metabolism. Recent studies have identified methylated thioarsenicals as a new class of arsenic metabolites in biological systems after exposure of inorganic and organic arsenicals, including arsenite, dimethylarsinic acid（DMAV）, dimethylarsinous glutathione（DMAIIIGS）, and arsenosugars. The increasing detection of thiolated arsenicals,including monomethylmonothioarsonic acid（MMMTAV）, dimethylmonothioarsinic acid（DMMTAV） and its glutathione conjugate（DMMTAVGS）, and dimethyldithioarsinic acid（DMDTAV） suggests that thioarsenicals may be important metabolites and play important roles in arsenic toxicity and therapeutic effects. Here we summarized the reported occurrence of thioarsenicals in biological systems, the possible formation pathways of thioarsenicals, and their toxicity, and discussed the biological implications of thioarsenicals on arsenic metabolism, toxicity, and therapeutic effects.
文摘For much of the world＇s population, food is the major source of exposure to arsenic.Exposure to this non-essential metalloid at relatively low levels may be linked to a wide range of adverse health effects. Thus, evaluating foods as sources of exposure to arsenic is important in assessing risk and developing strategies that protect public health. Although most emphasis has been placed on inorganic arsenic as human carcinogen and toxicant, an array of arsenic-containing species are found in plants and animals used as foods. Here,we 2evaluate the contribution of complex organic arsenicals（arsenosugars, arsenolipids,and trimethylarsonium compounds） that are found in foods and consider their origins,metabolism, and potential toxicity. Commonalities in the metabolism of arsenosugars and arsenolipids lead to the production of di-methylated arsenicals which are known to exert many toxic effects. Evaluating foods as sources of exposure to these complex organic arsenicals and understanding the formation of reactive metabolites may be critical in assessing their contribution to aggregate exposure to arsenic.
基金supported by the National Natural Science Foundation of China(Nos.U20A20267 and 22376223)Hunan Provincial Natural Science Foundation(No.2023JJ0065).
文摘Uranyl arsenate minerals,which exhibit low solubility,serve as major sinks for U and As,playing a crucial role in controlling the mobility of U and As in the environment.However,the specific mechanisms underly-ing the formation of uranyl arsenate minerals have remained largely elusive.Herein,the formation pathway of the non-charged UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O0 complex was investigated to elucidate the early formation of the UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O mineral(where n represents the stoichiometric number of H_(2)O),a representative uranyl arsenate mineral.Based on the combination experiments of U(VI)and As(V),our findings underscore the sig-nificant dependence of UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O0 formation on solution pH(4.0–10.0).Density functional theory(DFT)calculations reveal a two-step reaction involving two distinct pathways(Pathway 1 and Pathway 2)for the formation of UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O,and the intermediate was confirmed by in situ Raman and fluorescence spec-troscopy.Specifically,the hydroxyl‑connected uranyl(UO_(2)OH^(+))reacts with the protonated arsenate(H_(2)AsO_(4)^(-))species to form the intermediate UO_(2)HAsO4·H_(2)O(Pathway 1)or UO_(2)OH–H2AsO4(Pathway 2)with a U/As ratio of 1:1.Meanwhile,all the transition states also were obtained and the energy barrier suggested that the UO_(2)(H_(2)AsO_(4))_(2)·2H_(2)O0 formed by Pathway 1 is thermodynamically favored over Pathway 2,and may serve as the primary fundamental structural unit or precursor for the early formation of the UO_(2)(H_(2)AsO_(4))_(2)·nH_(2)O mineral phase.Altogether,this study contributes to advancing the understanding of the formation of uranyl arsenate min-erals at the molecular scale and provides a theoretical basis for predicting and regulating uranium and arsenic mobilization in their coexisting environment.
基金supported by the National Key Research and Development Program of China(No.2020YFC1807805)the Science and Technology Planning Project of Guangzhou,Guangdong Province,China(No.202206010176).
文摘Industrial activities have caused widespread arsenic(As)contamination in soil and medicinal crops across south-ern Asia.This study constructed interplanting systems combing medicinal crops with Pteris vittata L.,aiming to mitigate the risk of As exposure in medicinal crops,while simultaneously achieving ecological remediation of contaminated soil.The results revealed that interplanting with P.vittata significantly enhanced the yield of Gynos-temma pentaphyllum by 31.90%(P<0.05)compared with monoculture systems.Under monoculture conditions,the As concentration in G.pentaphyllum leaves reached 2.34 mg/kg,exceeding the national food safety standard(GB2762–2017,2 mg/kg).However,interplanting with P.vittata effectively reduced the As concentration in G.pentaphyllum leaves to 1.82 mg/kg.Furthermore,the interplanting of P.vittata with Rhus chinensis significantly inhibited As translocation from belowground to aboveground tissues in R.chinensis.Compared to monoculture,the stem biomass of P.vittata was significantly increased by 57.50%and 70.32%when interplanted with G.pentaphyllum and Cassia obtusifolia L.(P<0.05).So the As enrichment of P.vittata was enhanced in interplanting systems,which is beneficial for the As removal from contaminated soil.The study demonstrated that interplant-ing primarily regulates plant As uptake through modifications of rhizosphere physicochemical properties and As bioavailability,especially for water-soluble As that is easily absorbed by plants.In conclusion,the interplant-ing models integrating medicinal crops and P.vittata can achieve the goal of“remediating while producing”in As-contaminated soil.
基金Yunnan Fundamental Research Project,China(No.202201BE070001-056)。
文摘The volatilization characteristics and kinetic mechanisms of arsenic were investigated in the temperature range of 623−773 K and pressure ranges of 10−10000 Pa.The experimental results reveal that the evaporation rate increases with increasing temperature and decreasing pressure.Surface reaction control dominates at low pressures(<100 Pa),whereas diffusion control dominates at high pressures(>5000 Pa).The evaporation behavior is successfully described by an Arrhenius-type model for temperature dependence and Logistic model for pressure dependence.Key kinetic parameters,including the critical pressure,maximum evaporation rate and evaporation coefficient,were calculated.The evaporation coefficient varies between 0.010 and 0.223,and the critical pressures vary between 281 and 478 Pa with temperature.
基金supports from the National Natural Science Foundation of China(No.52304148)the Youth Project of Shanxi Basic Research Program(No.202203021212262).
文摘This study investigates the performance enhancement of super-sulfated cement(SSC)derived from arsenic-containing bio-oxidation waste(BW)through the incorporation of carbonated recycled concrete fines(CRCF).The findings revealed that the addition of 5wt%CRCF yields optimal performance,with compressive strengths reaching approximately 1.83,12.59,and 42.81 MPa at 1,3,and 28 d,respectively.These values represented significant increases of 408.3%,10.0%,and 14.3%compared to the reference sample.The improvement was attributed to the synergistic effects of ultrafine CRCF particles acting as fillers and nucleation sites,as well as the high reactivity of silica gels,which promoted the formation of additional hydration gels.Microstructural analysis confirmed that CRCF addition refined pore structure,and enhanced the stiffness of C-S-H gels.Furthermore,CRCF served as a net CO_(2) sink,sequestering 0.268 kg CO_(2) per kilogram of CRCF and thereby reducing the carbon footprint of SSC.In addition,the feasibility of applying CRCF-modified SSC in cemented paste backfill(CPB)is highlighted,given the high cement-related carbon footprint of conventional CPB.When 5wt%CRCFmodified SSC was employed in CPB,its 3-d compressive strength attained over 70%of that of ordinary Portland cement(OPC),while the 28-d strength was comparable to that of OPC.The proposed binder thus provides a sustainable pathway for BW valorization,combining waste utilization,carbon sequestration,and improved engineering performance.
基金supported by the National Natural Science Foundation of China(Grant No.22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(Grant No.EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009,xtr052025002).
文摘Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.
基金financially supported by the New Jersey Department of Environmental ProtectionUS EPA。
文摘In this study,synthetic wastewater containing 110μg/L arsenate(As(V)),0-20 mg/L fulvic acid(FA),and 0-12.3 mg/L phosphate was treated with 3 mg/L Fe3+.The mechanisms of FA and phosphate effects on As(V)removal by ferric chloride were determined using 0.22-10μm pore-size filtration,Zetasizer analysis,and in situ flow through cell ATR-FTIR.The results showed that up to 20mg/L FA had almost no effect on the solubility of ferric hydroxide precipitates and adsorption of As(V)by the precipitates.When FA concentration increased from 0 to 20 mg/L,the adsorption of FA led to higher negative zeta potential of the precipitates and the strong electrostatic repulsion between the precipitates decreased the particle size of ferric hydroxide flocs fromlarger than 10μmto smaller than 1μm.In the presence of 5-20 mg/L FA,46%-63%As(V)was adsorbed onto the flocs with particle size in the range of 0.45-1μm.On the other hand,phosphate did not affect the size of ferric hydroxide flocs and significantly increased the dissolved As(V)concentration because it competed with As(V)for adsorption sites on ferric hydroxide precipitates.The addition of 5mg/L cationic organic flocculant significantly reduced the effect of FA on As(V)removal,but did not reduce the effect of phosphate on As(V)removal.The findings of this study will help develop effective arsenic treatment techniques and predict the mobility of arsenic in the environment.
基金supported by the National Natural Science Foundation of China(Nos.32171623 and 31770548)the National Key Research and Development Program of China(Nos.2016YFD0800306 and 2017YFD0800305).
文摘Arsenic(As)pollution seriously threatens human and ecological health.Microalgal cell wall and extracellular polymeric substances(EPS)are known to interactwith As,but their roles in the As resistance,accumulation and speciation inmicroalgae remain unclear.Here,we used two strains of Chlamydomonas reinhardtii,namely CC-125(wild type)and CC-503(cell walldeficientmutant),to examine the algal growth,EPS synthesis,As adsorption,absorption and transformation under 10–1000μg/L As(III)and As(V)treatments for 96 h.In both strains,the As absorption increased after the EPS removal,but the growth,As adsorption,and transformation of C.reinhardtii declined.The CC-125 strain was more tolerant to As stress and more efficient in EPS production,As accumulation,and redox transformation than CC-503,irrespective of EPS presence or absence.Three-dimension excitation-emission matrix(3DEEM)and attenuated total reflectance infrared spectroscopy(ATR-IR)analyses showed that As was bound with functional groups in the EPS and cell wall,such as-COOH,NH and-OH in proteins,polysaccharides and amino acids.Together,this study demonstrated that EPS and cell wall acted as barriers to lower the As uptake by C.reinhardtii.However,the cell wall mutant strain wasmore susceptible to As toxicity due to lower EPS induction and higher As absorption.
基金supported by the National Key Research and Development Program of China(No.2017YFC1502504)the National Natural Science Foundation of China(No.41877531).
文摘With the increasing severity of arsenic(As)pollution,quantifying the environmental behavior of pollutant based on numerical model has become an important approach to determine the potential impacts and finalize the precise control strategies.Taking the industrialintensive Jinsha River Basin as typical area,a two-dimensional hydrodynamic water quality model coupled with Soil andWater Assessment Tool(SWAT)model was developed to accurately simulate the watershed-scale distribution and transport of As in the terrestrial and aquatic environment at high spatial and temporal resolution.The effects of hydro-climate change,hydropower station construction and non-point source emissions on Aswere quantified based on the coupled model.The result indicated that higher As concentration areas mainly centralized in urban districts and concentration slowly decreased from upstream to downstream.Due to the enhanced rainfall,the As concentration was significantly higher during the rainy season than the dry season.Hydro-climate change and the construction of hydropower station not only affected the dissolved As concentration,but also affected the adsorption and desorption of As in sediment.Furthermore,As concentration increased with the input of non-point source pollution,with the maximum increase about 30%,resulting that non-point sources contributed important pollutant impacts to waterways.The coupled model used in pollutant behavior analysis is generalwith high potential application to predict and mitigate water pollution.
基金supported by the National Natural Science Foundation of China(NSFC)grants(Nos.41473122,41173113,52261145693 and 22106028)the Ministry of Science and Technology of the People’s Republic of China(MOST)+1 种基金the Fundamental Research Funds for the Central Universities(FRF-TP-19-020A1)the Hundred Talents Program of the Chinese Academy of Sciences,and China Postdoctoral Science Foundation(No.2023M730216).
文摘Arsenic and cadmium contamination frequently coexist in the real environment.However it remains a challenge for their simultaneous removal due to their distinct physicochemica properties at low cost.To this end,a cost-effective magnetic biochar adsorbent (ITBNa800was prepared using biomass waste and iron tailings slag.This composite adsorbent exhibits excellent performance in the simultaneous removal of aqueous As(Ⅴ) and Cd(Ⅱ) even at high concentrations with removal efficiencies of up to 99.98%and 96.04%,respectively.Electro static action,precipitation,and complexation were adsorption mechanisms.As(Ⅴ) and Cd(Ⅱ were synergistic and competitive adsorption.As(Ⅴ) removal was mainly due to physical and chemical adsorption,and 42.40%-58.59%of As(Ⅴ) had been converted to As(Ⅲ ).Cd(Ⅱ) re moval was mainly due to chemical adsorption.Iron oxide and aluminum oxide in ITBNa800were the keys to As(Ⅴ),As(Ⅲ ),and Cd(Ⅱ) adsorption.DFT calculations revealed iron oxide complex As(Ⅴ),As(Ⅲ ),and Cd(Ⅱ) molecular clusters through bidentate binuclear,bidentate binuclear,and monodentate binuclear pathways,respectively.Aluminum oxide complex Cd(Ⅱ) molecular cluster through a bidentate mononuclear pathway.We hope the ITBNa800adsorbent and its involved mechanism could offer inspiration in the simultaneous treat ment of As and Cd pollution.
基金supported by the Central Public-interest Scientific Institution Basal Research Fund(No.Y2024QC29)the Central Public-interest Scientific Institution Basal Research Fund(Nos.2024-jbkyywf-lwj and 2024-jbkyywf-zyj).
文摘The Qinghai-Tibet Plateau,with its high altitude and cold climate,is one of the most fragile ecological environments in China and is distinguished by its naturally elevated arsenic(As)levels in the soil,largely due to its rich mineral and geothermal resources.This review provides a comprehensive analysis of As content,focusing on its distribution,environmental migration,and transformation behavior across the plateau.The review further evaluates the distribution of As in different functional areas,revealing that geothermal fields(107.2 mg/kg),mining areas(53.8 mg/kg),and croplands(39.3 mg/kg)have the highest As concentrations,followed by river and lake sediments and adjacent areas(33.1 mg/kg).These elevated levels are primarily attributed to the presence of As-rich minerals,such as arsenopyrite and pyrite.Additionally,human activities,including mining and geothermal energy production,exacerbate the release of As into the environment.The review also highlights the role of localmicroorganisms,particularly those fromthe phyla Proteobacteria and Actinobacteria,which possess As metabolic genes that facilitate As translocation.Given the unique climatic conditions of the plateau,conventionalmethods for As controlmay not be fully effective.However,the review identifies promising remediation strategies that are environmentally adaptable,such as the use of local microorganisms,specific adsorbents,and integrated technologies,which offer potential solutions for managing and utilizing Ascontaminated soils on the plateau.
基金supported by the Shandong Province Natural Science Foundation of Major Basic Research Program (No.ZR2020ZD34)the Key Projects of the National Natural Science Foundation of China (No.42230706)+3 种基金the National Natural Science Foundation of China (No.42307164)the China Postdoctoral Science Foundation (Nos.2023TQ0191 and 2023M732060)the Shandong Postdoctoral Science Foundation (No.SDBX2023041)and the Qingdao Postdoctoral Science Foundation (No.QDBSH20230202052).
文摘Arsenic(As)methylation in soils affects the environmental behavior of As,excessive accumulation of dimethylarsenate(DMA)in rice plants leads to straighthead disease and a serious drop in crop yield.Understanding the mobility and transformation of methylated arsenic in redox-changing paddy fields is crucial for food security.Here,soils including unarsenic contaminated(N-As),low-arsenic(L-As),medium-arsenic(M-As),and high-arsenic(H-As)soils were incubated under continuous anoxic,continuous oxic,and consecutive anoxic/oxic treatments respectively,to profile arsenic methylating process and microbial species involved in the As cycle.Under anoxic-oxic(A-O)treatment,methylated arsenic was significantly increased once oxygen was introduced into the incubation system.The methylated arsenic concentrations were up to 2-24 times higher than those in anoxic(A),oxic(O),and oxic-anoxic(O-A)treatments,under which arsenic was methylated slightly and then decreased in all four As concentration soils.In fact,the most plentiful arsenite S-adenosylmethionine methyltransferase genes(arsM)contributed to the increase in As methylation.Proteobacteria(40.8%-62.4%),Firmicutes(3.5%-15.7%),and Desulfobacterota(5.3%-13.3%)were the major microorganisms related to this process.These microbial increasedmarkedly and played more important roles after oxygen was introduced,indicating that they were potential keystone microbial groups for As methylation in the alternating anoxic(flooding)and oxic(drainage)environment.The novel findings provided newinsights into the reoxidation-driven arsenic methylation processes and the model could be used for further risk estimation in periodically flooded paddy fields.
基金supported by the National Key Research and Development Program of China(No.2020YFC1808701).
文摘Arsenic(As)pollution in soils is a pervasive environmental issue.Biochar immobilization offers a promising solution for addressing soil As contamination.The efficiency of biochar in immobilizing As in soils primarily hinges on the characteristics of both the soil and the biochar.However,the influence of a specific property on As immobilization varies among different studies,and the development and application of arsenic passivation materials based on biochar often rely on empirical knowledge.To enhance immobilization efficiency and reduce labor and time costs,a machine learning(ML)model was employed to predict As immobilization efficiency before biochar application.In this study,we collected a dataset comprising 182 data points on As immobilization efficiency from 17 publications to construct three ML models.The results demonstrated that the random forest(RF)model outperformed gradient boost regression tree and support vector regression models in predictive performance.Relative importance analysis and partial dependence plots based on the RF model were conducted to identify the most crucial factors influencing As immobilization.These findings highlighted the significant roles of biochar application time and biochar pH in As immobilization efficiency in soils.Furthermore,the study revealed that Fe-modified biochar exhibited a substantial improvement in As immobilization.These insights can facilitate targeted biochar property design and optimization of biochar application conditions to enhance As immobilization efficiency.
文摘In this study,we investigated improving the performance of a layered double hydroxide(LDH)for the adsorption of As(III)and As(V)by controlling the morphology of LDH crystals.The LDH was synthesized via a simple coprecipitation method using barely soluble MgO as a precursor and succinic acid(SA)as a morphological control agent.Doping the LDH crystals with carboxylate ions(RCOO−)derived from SA caused the crystals to develop in a radial direction.This changed the pore characteristics and increased the density of active surface sites.Subsequently,SA/MgFe-LDH showed excellent affinity for As(III)and As(V)with maximum sorption densities of 2.42 and 1.60 mmol/g,respectively.By comparison,the pristine MgFe-LDH had sorption capacities of 1.56 and 1.31 mmol/g for As(III)and As(V),respectively.The LDH was effective over a wide pH range for As(III)adsorption(pH 3-8.5)and As(V)adsorption(pH 3-6.5).Using a combination of spectroscopy and sorption modeling calculations,the main sorption mechanism of As(III)and As(V)on SA/MgFe-LDH was identified as inner-sphere complexation via ligand exchangewith hydroxyl group(-OH)and RCOO−.Specifically,bidentate As-Fe complexeswere proposed for both As(III)and As(V)uptake,with the magnitude of formation varying with the initial As concentration.Importantly,the As-laden adsorbent had satisfactory stability in simulated real landfill leachate.These findings demonstrate that SA/MgFe-LDH exhibits considerable potential for remediation of As-contaminated water.
基金the National Key R&D Program of China(No.2021YFA0715900)the National Natural Science Foundation of China(No.41831279)+2 种基金the Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks(No.ZDSYS20220606100604008)the Guangdong Province Bureau of Education(No.2020KCXTD006)the Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control(No.2023B1212060002).
文摘Rapid screening of inorganic arsenic(iAs)in groundwater used for drinking by hundreds of millions of mostly rural residents worldwide is crucial for health protection.Most commercial field test kits are based on the Gutzeit reaction that uses mercury-based reagents for color development,an environmental concern that increasingly limits its utilization.This study further improves the Molybdenum Blue(MB)colorimetric method to allow for faster screening with more stable reagents.More importantly,a portable three-channel colorimeter is developed for screening iAs relative to the WHO drinking water guideline value(10μg/L).Adding the reducing reagents in sequence not only prolongs the storage time to>7 days,but also accelerates the color development time to 6 min in conjunction with lowering the H_(2)SO_(4) concentration in chromogenic reagents.The optimal pH ranges from 1.2 to 1.3 and is achieved by acidifying groundwater to 1%(V/V)HCl.With detection limits of 3.7μg/L for inorganic arsenate(iAs(V))and 3.8μg/L for inorganic arsenite(iAs(Ⅲ)),testing groundwater with-10μg/L of As has a precision<20%.The method works well for a range of phosphate concentrations of 48-950μg/L(0.5-10μmol/L).Concentrations of total_iAs(6-300μg/L),iAs(V)(6-230μg/L)and iAs(Ⅲ)(0-170μg/L)for 14 groundwater samples from Yinchuan Plain,Pearl River Delta,and Jianghan Plain,are in excellent agreements(linear regression slope:0.969-1.029)with the benchmark methods.The improved chemistry here lays the foundation for the MB colorimetric method to become a commercially viable screening tool,with further engineering and design improvement of the colorimeter.
基金supported by the National Natural Science Foundation of China(No.42377024)the Aid Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Province,Chinathe Key Project of Developmental Biology and Breeding from Hunan Province of China(No.2022XKQ0207).
文摘Arsenic(As)contamination in paddy soils has posed a prominent threat to rice production in Asia.Recycling of silicon(Si)from Si-rich combusted rice husk(CRH)could serve as a sustainable strategy to mitigate rice As uptake through their shared transport pathway.Root(soil)application of CRH alone,however,was insufficient to decrease inorganic As(iAs)in polished rice below Chinese food standards(0.2 mg kg^(-1)).In this study,an aqueous Si solution derived from CRH was used for synergistic foliar application over the highest Si-demanding stage(reproductive stage)of rice,following root application of Si,to investigate rice As uptake in both pot and field experiments.In the pot experiment,on the basis of root application of CRH,Si supplementation before the reproductive stage of rice led to a 51%decrease in As concentration on root surface along with a prominent reduction of Fe plaque due to enhanced root suberization,relative to single root application of CRH treatment.In parallel,the expression of OsLis6 gene in the root was downregulated by 91%than that with only root application of CRH.These changes decreased As influx into root by 56%and led correspondingly to 41%lower As transfer to the straw,as compared with root application of CRH treatment.In node I,the expression of OsLis6 decreased concurrently by 71%,leading ultimately to 28%lower iAs accumulation in grains than that with root application of CRH alone.In the field experiment,with single foliar Si,the mitigation of grain iAs occurred only at lower soil As level of 40 mg kg^(-1),while promoted iAs unloading into grains was determined under higher soil As level(80 mg kg^(-1))relative to the control without Si application.It was,therefore,concluded that the mitigation of grain iAs accumulation with soil application of CRH can be strengthened critically by synergistic supply of foliar Si,serving as a more reliable pathway to secure rice production in As-contaminated paddy fields.
基金supported by the National Natural Science Foundation of China(Nos.82241088 and 82203996)the China Postdoctoral Science Foundation(Nos.2022T150230 and 2021M691131).
文摘Arsenic-related oxidative stress and resultant diseases have attracted global concern,while longitudinal studies are scarce.To assess the relationship between arsenic exposure and systemic oxidative damage,we performed two repeatedmeasures among 5236 observations(4067 participants)in theWuhan-Zhuhai cohort at the baseline and follow-up after 3 years.Urinary total arsenic,biomarkers of DNA oxidative damage(8-hydroxy-2-deoxyguanosine(8-OHdG)),lipid peroxidation(8-isoprostaglandin F2alpha(8-isoPGF2α)),and protein oxidative damage(protein carbonyls(PCO))were detected for all observations.Here we used linearmixed models to estimate the cross-sectional and longitudinal associations between arsenic exposure and oxidative damage.Exposure-response curves were constructed by utilizing the generalized additive mixed models with thin plate regressions.After adjusting for potential confounders,arsenic level was significantly and positively related to the levels of global oxidative damage and their annual increased rates in dose-response manners.In cross-sectional analyses,each 1%increase in arsenic levelwas associated with a 0.406%(95%confidence interval(CI):0.379%to 0.433%),0.360%(0.301%to 0.420%),and 0.079%(0.055%to 0.103%)increase in 8-isoPGF2α,8-OHdG,and PCO,respectively.More importantly,arsenic was further found to be associated with increased annual change rates of 8-isoPGF2α(β:0.147;95%CI:0.130 to 0.164),8-OHdG(0.155;0.118 to 0.192),and PCO(0.050;0.035 to 0.064)in the longitudinal analyses.Our study suggested that arsenic exposurewas not only positively related with global oxidative damage to lipid,DNA,and protein in cross-sectional analyses,but also associated with annual increased rates of these biomarkers in dose-dependent manners.
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.
