Modeling transport of arsenic through modified granular natural siderite filters for arsenic removal
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摘要
Groundwater arsenic(As)contamination is a hot issue,which is severe health concern worldwide.Recently,many Fe-based adsorbents have been used for As removal from solutions.Modified granular natural siderite(MGNS),a special hybrid Fe(II)/Fe(III)system,had higher adsorption capacity for As(III)than As(V),but the feasibility of its application in treating high-As groundwater is still unclear.In combination with transport modeling,laboratory column studies and field pilot tests were performed to reveal both mechanisms and factors controlling As removal by MGNS-filled filters.Results show that weakly acid pH and discontinuous treatment enhanced As(Ⅲ)removal,with a throughput of 8700 bed volumes(BV)of 1.0 mg/L As(Ⅲ)water at breakthrough of 10 μg/L As at pH 6.Influent HCO_3~-inhibited As removal by the filters.Iron mineral species,SEM and XRD patterns of As-loading MGNS show that the important process contributing to high As(Ⅲ)removal was the mineral transformation from siderite to goethite in the filter.The homogeneous surface diffusion modeling(HSDM)shows that competition between As(III)and HCO_3~-with adsorption sites on MGNS was negligible.The inhibition of HCO_3~-on As(Ⅲ)removal was connected to inhibition of siderite dissolution and mineral transformation.Arsenic loadings were lower in field pilot tests than those in the laboratory experiments,showing that high concentrations of coexisting anions(especially HCO_3~-and SiO_4~(4-)),high pH,low EBCT,and low groundwater temperature decreased As removal.It was suggested that acidification and aeration of highAs groundwater and discontinuous treatment would improve the MGNS filter performance of As removal from real high-As groundwater.
Groundwater arsenic(As)contamination is a hot issue,which is severe health concern worldwide.Recently,many Fe-based adsorbents have been used for As removal from solutions.Modified granular natural siderite(MGNS),a special hybrid Fe(II)/Fe(III)system,had higher adsorption capacity for As(III)than As(V),but the feasibility of its application in treating high-As groundwater is still unclear.In combination with transport modeling,laboratory column studies and field pilot tests were performed to reveal both mechanisms and factors controlling As removal by MGNS-filled filters.Results show that weakly acid pH and discontinuous treatment enhanced As(Ⅲ)removal,with a throughput of 8700 bed volumes(BV)of 1.0 mg/L As(Ⅲ)water at breakthrough of 10 μg/L As at pH 6.Influent HCO_3~-inhibited As removal by the filters.Iron mineral species,SEM and XRD patterns of As-loading MGNS show that the important process contributing to high As(Ⅲ)removal was the mineral transformation from siderite to goethite in the filter.The homogeneous surface diffusion modeling(HSDM)shows that competition between As(III)and HCO_3~-with adsorption sites on MGNS was negligible.The inhibition of HCO_3~-on As(Ⅲ)removal was connected to inhibition of siderite dissolution and mineral transformation.Arsenic loadings were lower in field pilot tests than those in the laboratory experiments,showing that high concentrations of coexisting anions(especially HCO_3~-and SiO_4~(4-)),high pH,low EBCT,and low groundwater temperature decreased As removal.It was suggested that acidification and aeration of highAs groundwater and discontinuous treatment would improve the MGNS filter performance of As removal from real high-As groundwater.
Groundwater arsenic(As)contamination is a hot issue,which is severe health concern worldwide.Recently,many Fe-based adsorbents have been used for As removal from solutions.Modified granular natural siderite(MGNS),a special hybrid Fe(II)/Fe(III)system,had higher adsorption capacity for As(III)than As(V),but the feasibility of its application in treating high-As groundwater is still unclear.In combination with transport modeling,laboratory column studies and field pilot tests were performed to reveal both mechanisms and factors controlling As removal by MGNS-filled filters.Results show that weakly acid pH and discontinuous treatment enhanced As(Ⅲ)removal,with a throughput of 8700 bed volumes(BV)of 1.0 mg/L As(Ⅲ)water at breakthrough of 10 μg/L As at pH 6.Influent HCO_3~-inhibited As removal by the filters.Iron mineral species,SEM and XRD patterns of As-loading MGNS show that the important process contributing to high As(Ⅲ)removal was the mineral transformation from siderite to goethite in the filter.The homogeneous surface diffusion modeling(HSDM)shows that competition between As(III)and HCO_3~-with adsorption sites on MGNS was negligible.The inhibition of HCO_3~-on As(Ⅲ)removal was connected to inhibition of siderite dissolution and mineral transformation.Arsenic loadings were lower in field pilot tests than those in the laboratory experiments,showing that high concentrations of coexisting anions(especially HCO_3~-and SiO_4~(4-)),high pH,low EBCT,and low groundwater temperature decreased As removal.It was suggested that acidification and aeration of highAs groundwater and discontinuous treatment would improve the MGNS filter performance of As removal from real high-As groundwater.
引文
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Capelo-Neto,J.,SiJva Buarque,N.M.,2016.Simulation of saxitoxins adsorption in full-scale GAC filter using HSDM.Water Research 88,558—565.
Casentini,B.,Falcione.F.T.,Amalfitano,S.,Fazi,S.,Rossetti,S.,2016.Arsenic removal by discontinuous ZVI two steps system for drinking water production at household scale.Water Research 106,135-145.
Chakravarty,S.,Dureja,V.,Bhattacharyya,G.,Maity,S.,Bhattacharjee,S.,2002.Removal of arsenic from groundwater using low cost ferruginous manganese ore.Water Research 36.625-632.
Chen,X.M.,Ni,B.J.,2016.Model-based evaluation on simultaneous nitrate and arsenite removal in a membrane biofilm reactor.Chemical Engineering Science152,488-496.
Ciardelli,M.C.,Xu,H.F.,Sahai,N.,2008.Role of Fe(II),phosphate,silicate,sulfate,and carbonate in arsenic uptake by coprecipitation in synthetic and natural groundwater.Water Research 42,615-624.
Fendorf,S.,Michael,H.A.,van Geen,A.,2010.Spatial and temporal variations of groundwater arsenic in South and Southeast Asia.Science 328,1123-1127.
Gao,X.B.,Su,CL,Wang,Y.X.,Hu,Q.H.,2013.Mobility of arsenic in aquifer sediments at Datong Basin,northern China:effect of bicarbonate and phosphate.Journal of Geochemical Exploration 135,93-103.
German,M.,Seingheng,H.,SenGupta,A.K.,2014.Mitigating arsenic crisis in the developing world:role of robust,reusable and selective hybrid anion exchanger(HAIX).The Science of the Total Environment 488-489,547-553.
Giral,M.,Zagury,G.J.,Deschenes,L,Blouin,J., 2010.Comparison of four extraction procedures to assess arsenate and arsenite species in contaminated soils.Environmental Pollution 158(5),1890-1898.
Guo,H.,Liu,C.,Lu,H.,Wanty,R.B.,Wang,J.,Zhou,Y.,2013a.Pathways of coupled arsenic and iron cycling in high arsenic groundwater of the Hetao basin,Inner Mongolia,China:an iron isotope approach.Geochimica et Cosmochimica Acta112,130-145.
Guo,H.,Wen,D.,Liu,Z.,Jia,Y.,Guo,Q.,2014.A review of high arsenic groundwater in Mainland and Taiwan,China:distribution,characteristics and geochemical processes.Applied Geochemistry 41,196-217.
Guo,H., Zhang,D.,Ni,P.,Cao,Y.,Li,F.,Jia,Y.,Li,H.,Wan,L,Wang,G.,2016a.On the scalability of hydrogeochemical factors controlling arsenic mobility in three major inland basins of P.R.China.Applied Geochemistry 77,15-23.
Guo,H.M.,Zhou,Y.Z.,Jia,Y.F.,Tang,X.H.,Jiang,Y.X.,Lu,H.,Han,S.B.,Zheng,H.,Cao,Y.S.,Zhao,W.G.,Zhang,D.,Wei,C.,Norra,S.,Zhang,F.C.,2016b.Sulfur cycling-related biogeochemical processes of arsenic mobilization in the western Hetao basin,China:evidences from multiple isotope approaches.Environmental Science and Technology 50(23),12650-12659.
Guo,H.,Zhang,Y.,Jia,Y.,Zhao,K.,Li,Y.,Tang,X.,2013b.Dynamic behaviors of water levels and arsenic concentration in shallow groundwater from the Hetao Basin,Inner Mongolia.Journal of(Geochemical Exploration 135,130-140.
Guo,H.M.,Li,Y.,Zhao,K.,2010.Arsenate removal from aqueous solution using synthetic siderite.Journal of Hazardous Materials 176,174-180.
Guo,H.M.,Li,Y.A.,Zhao,K.,Ren,Y.,Wei,C.,2011.Removal of arsenite from water by synthetic siderite:behaviors and mechanisms.Journal of Hazardous Materials186.,1847-1854.
Guo,H.M.,Ren,Y.,Liu,Q,,Zhao,K.,Li,Y.,2013c.Enhancement of arsenic adsorption during mineral transformation from siderite to goethite:mechanism and application.Environmental Science and Technology 47.,1009-1016.
Guo,H.M.,Stuben,D.,Bemer,Z.,Kramar,U.,2008.Adsorption of arsenic species from water using activated siderite-hematite column filters.Journal of Hazardous Materials 151,628—635.
Guo,H.M.,Stuben,D.,Berner,Z.,2007a.Adsorption of arsenic(Ⅲ)and arsenic(V)from groundwater using natural siderite as the adsorbent.Journal of Colloid and Interface Science 315.,47-53.
Guo,H.M.,Stuben,D.,Berner,Z.,2007b.Arsenic removal from water using natural iron mineral-quartz sand columns.The Science of the Total Environment 377,142-151.
Guo,H.M.,Stuben,D.,Berner,Z.,2007c.Removal of arsenic from aqueous solution by natural siderite and hematite.Applied Geochemistry 22,1039-1051.
Hou,J.T.,Luo,J.L,Hu,Z.Q.,Li,Y.Z.,Mao,M.Y.,Song,S.X.,Liao,Q.L,Li,Q.Z.,2016.Tremendous efFect of oxygen vacancy defects on the oxidation of arsenite to arsenate on cryptomelane-type manganese oxide.Chemical Engineering Journal 306.597-606.
Hug,S.J.,Leupin,O.,2003.Iron-catalyzed oxidation of arsenic(Ⅲ)by oxygen and by hydrogen peroxide:pH-dependent formation of oxidants in the Fenton reaction.Environmental Science and Technology 37,2734-2742.
Jadhav,S.V.,Bringas,E.,Yadav,G.D.,Rathod,V.K.,Ortiz,I.,Marathe,K.V.,2015.Arsenic and fluoride contaminated groundwaters:a review of current technologies for contaminants removal.Journal of Environmental Management 162,306-325.
Jessen,S.,Larsen,F.,Koch,C.B.,Arvin,E.,2005.Sorption and desorption of arsenic to ferrihydrite in a sand filter.Environmental Science and Technology 39,8045-8051.
Kanematsu,M.,Young,T.M.,Fukushi,K.,Green,P.G.,Darby,J.L,2012.Individual and combined effects of water quality and empty bed contact time on As(V)removal by a fixed-bed iron oxide adsorber:implication for silicate precoating.Water Research 46,5061-5070.
Kim,D.H..Bokare,A.D.,Koo,M.S.,Choi,W.,2015.Heterogeneous catalytic oxidation of As(Ⅲ)on nonferrous metal oxides in the presence of H_2O_2.Environmental Science and Technology 49,3506-3513.
Kim,E.J.,Yoo,J.C.,Baek,K.,2014.Arsenic speciation and bioaccessibility in arseniccontaminated soils:sequential extraction and mineralogical investigation.Environmental Pollution 186,29-35.
Kulkarni,H.V.,Mladenov,N.,McKnight,D.M.,Zheng,Y.,Kirk,M.F.,Nemergut,D.R.,2018.Dissolved fulvic acids from a high arsenic aquifer shuttle electrons to enhance microbial iron reduction.The Science of the Total Environment 615,1390-1395.
Kulkarni,H.V.,Mladenov,N.,Johannesson,K.H.,Datta,S.,2017.Contrasting dissolved organic matter quality in groundwater in holocene and pleistocene aquifers and implications for influencing arsenic mobility.Applied Geochemistry 77,194-205.
Kumar,N.,Couture,R.M.,Millot,R.,Battaglia-Brunet,F.,Rose,J.,2016a.Microbial sulfate reduction enhances arsenic mobility downstream of zerovalent-ironbased permeable reactive barrier.Environmental Science and Technology 50(14).7610-7617.
Kumar,N.,Millot,R.,Battaglia-Brunet,F.,Omoregie,E.,Chaurand,P.,Borschneck,D.,Bastiaens,L,Rose,J.,2016b.Microbial and mineral evolution in zero valent iron-based permeable reactive barriers during long-term operations.Environmental Science and Pollution Research 23,5960-5968.
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