基于硫酸亚铁的机械化学还原法处理六价铬污染土壤
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摘要
通过机械化学还原法对六价铬污染土壤进行固化稳定化处理,采用《固体废物浸出毒性浸出方法硫酸硝酸法》(HJ/T 299-2007)对处理效果进行评价,以及使用激光粒度仪、SEM和XPS对处理前后土壤样品的粒径、形貌以及铬的价态变化等性质进行表征。分析结果显示,机械化学还原法处理可以有效降低土壤中六价铬的浸出浓度。当未添加七水合硫酸亚铁时,土壤中六价铬的浸出浓度由115 mg·L~(-1)降低至2.0 mg·L~(-1);而添加七水合硫酸亚铁作为还原剂时,六价铬浸出浓度由115 mg·L~(-1)降至0.16 mg·L~(-1)。另外,经过机械化学还原处理后的土壤样品颗粒变细并形成致密的团聚体以及发生六价铬向三价铬的转化。
In this research, the solidification and stabilization treatment of Cr(Ⅵ)-contaminated soil through mechanochemical reduction with ferrous sulfate was investigated. The properties of soil after remediation by ball milled with or without ferrous sulfate were characterized by XRD, SEM and XPS analysis. And the leachable fraction of Cr(Ⅵ) from the treated samples is also analyzed through the method HJ/T 299-2007. The results indicate that mechanochemical remediation is very effective for the solidification and stabilization of Cr(Ⅵ)-contaminated soil.Cr(Ⅵ) leaching concentration decreased from 115 to 2.0 and 0.16 mg·L~(-1), respectively, when without and with ferrous sulfate. In addition, during mechanochemical treatment, decrease in particle size, agglomeration and the conversion between Cr(Ⅵ) and Cr(Ⅲ) in contaminated soil are observed.
In this research, the solidification and stabilization treatment of Cr(Ⅵ)-contaminated soil through mechanochemical reduction with ferrous sulfate was investigated. The properties of soil after remediation by ball milled with or without ferrous sulfate were characterized by XRD, SEM and XPS analysis. And the leachable fraction of Cr(Ⅵ) from the treated samples is also analyzed through the method HJ/T 299-2007. The results indicate that mechanochemical remediation is very effective for the solidification and stabilization of Cr(Ⅵ)-contaminated soil.Cr(Ⅵ) leaching concentration decreased from 115 to 2.0 and 0.16 mg·L~(-1), respectively, when without and with ferrous sulfate. In addition, during mechanochemical treatment, decrease in particle size, agglomeration and the conversion between Cr(Ⅵ) and Cr(Ⅲ) in contaminated soil are observed.
引文
[1]GRAHAM A M,WADHAWAN A R,BOUWER E J.Chromium occurrence and speciation in Baltimore Harbor sediments and porewater,Baltimore,Maryland,USA[J].Environmental Toxicology&Chemistry,2009,28(3):471-480.DOI:10.1897/08-149.1.
[2]LINDSAY D R,FARLEY K J,CARBONARO R F.Oxidation of Cr(III)to Cr(VI)during chlorination of drinking water[J].Journal of Environmental Monitoring,2012,14(7):1789-1797.DOI:10.1039/C2EM00012A.
[3]APTE A D,TARE V,BOSE P.Extent of oxidation of Cr(III)to Cr(VI)under various conditions pertaining to natural environment[J].Journal of Hazardous Materials,2006,128(2/3):164-174.DOI:10.1016/j.jhazmat.2005.07.057.
[4]WANG Y,FANG Z,LIANG B,et al.Remediation of hexavalent chromium contaminated soil by stabilized nanoscale zero-valent iron prepared from steel pickling waste liquor[J].Chemical Engineering Journal,2014,247(6):283-290.DOI:10.1016/j.cej.2014.03.011.
[5]崔永高.铬污染土壤和地下水的修复技术研究进展[J].工程地质学报,2017,25(4):1001-1009.DOI:10.13544/j.cnki.jeg.2017.04.014.
[6]周加祥,刘铮.铬污染土壤修复技术研究进展[J].环境工程学报,2000,1(4):52-56.
[7]张蕊.六价铬在土壤中迁移转化影响因素研究及风险评价[D].长春:吉林大学,2013.
[8]姜苹红,陈灿,向仁军.铬污染土壤的单一/复合还原处理及其长期稳定性研究[J].环境工程学报,2015,9(10):5091-5095.
[9]黄莹,徐民民,李书鹏,等.还原稳定化法修复六价铬污染土壤的中试研究[J].环境工程学报,2015,9(2):951-958.
[10]DENG S,KANG S,FENG N,et al.Mechanochemical mechanism of rapid dechlorination of hexachlorobenzene[J].Journal of Hazardous Materials,2017,333:116-154.DOI:10.1016/j.jhazmat.2017.03.022.
[11]ZHANG W,WANG H,HUANG J,et al.Acceleration and mechanistic studies of the mechanochemical dechlorination of HCB with iron powder and quartz sand[J].Chemical Engineering Journal,2014,239(3):185-191.DOI:10.1016/j.cej.2013.11.018.
[12]MONTINARO S,CONCAS A,PISU M,et al.Rationale of lead immobilization by ball milling in synthetic soils and remediation of heavy metals contaminated tailings[J].Chemical Engineering Journal,2009,155(1):123-131.DOI:10.1016/j.cej.2009.07.005.
[13]MONTINARO S,CONCAS A,PISU M,et al.Immobilization of heavy metals in contaminated soils through ball milling with and without additives[J].Chemical Engineering Journal,2008,142(3):271-284.DOI:10.1016/j.cej.2007.12.003.
[14]ZHANG Z X.Immobilisation of metal in quartz sands by ball milling[D].Auckland:Auckland University of Technology,2008.
[15]CONCAS A,MONTINARO S,PISU M,et al.Mechanochemical remediation of heavy metals contaminated soils:Modelling and experiments[J].Chemical Engineering Science,2007,62(18/19/20):5186-5192.DOI:10.1016/j.ces.2007.02.024.
[16]USEPA.Test methods for evaluating solid waste,physical/chemical methods,SW-846:Method 3050B[S].Washington,D.C.,1992.
[17]CEPA.Solid waste extraction procedure for leaching toxicity sulfuric acid&nitric acid method:HJ/T299-2007[S].2007.
[18]SANTHANAM P R,DREIZIN E L.Predicting conditions for scaled-up manufacturing of materials prepared by ball milling[J].Powder Technology,2012,221(5):403-411.DOI:10.1016/j.powtec.2012.01.037.
[19]DELOGU F,ORR′U R,CAO G.A novel macrokinetic approach for mechanochemical reactions[J].Chemical Engineering Science,2003,58(3):815-821.DOI:10.1016/S0009-2509(02)00612-7.
[20]BOURSIQUOT S,MULLET M,EHRHARDT J J.XPS study of the reaction of chromium(VI)with mackinawite(Fe S)[J].Surface&Interface Analysis,2010,34(1):293-297.DOI:10.1002/sia.1303.
[21]AND L D,GUILLON E.Removal of hexavalent chromium with a lignocellulosic substrate extracted from wheat bran[J].Environmental Science&Technology,2003,37(18):4235-4241.DOI:10.1021/es0342345.
[22]ZHANG W X,LI X Q,CAO J S.Reply to comments on stoichiometry of Cr(VI)immobilization using nanoscale zerovalent iron(n ZVI):A study with high-resolution X-ray photoelectron spectroscopy(HR-XPS)[J].Industrial&Engineering Chemistry Research,2009,47(7):2297-2297.DOI:10.1021/ie061655x.
[23]LEGRAND L,EL F A,MERCIER F,et al.Reduction of aqueous chromate by Fe(II)/Fe(III)carbonate green rust:Kinetic and mechanistic studies[J].Environmental Science&Technology,2004,38(17):4587-4595.DOI:10.1021/es035447x.
[2]LINDSAY D R,FARLEY K J,CARBONARO R F.Oxidation of Cr(III)to Cr(VI)during chlorination of drinking water[J].Journal of Environmental Monitoring,2012,14(7):1789-1797.DOI:10.1039/C2EM00012A.
[3]APTE A D,TARE V,BOSE P.Extent of oxidation of Cr(III)to Cr(VI)under various conditions pertaining to natural environment[J].Journal of Hazardous Materials,2006,128(2/3):164-174.DOI:10.1016/j.jhazmat.2005.07.057.
[4]WANG Y,FANG Z,LIANG B,et al.Remediation of hexavalent chromium contaminated soil by stabilized nanoscale zero-valent iron prepared from steel pickling waste liquor[J].Chemical Engineering Journal,2014,247(6):283-290.DOI:10.1016/j.cej.2014.03.011.
[5]崔永高.铬污染土壤和地下水的修复技术研究进展[J].工程地质学报,2017,25(4):1001-1009.DOI:10.13544/j.cnki.jeg.2017.04.014.
[6]周加祥,刘铮.铬污染土壤修复技术研究进展[J].环境工程学报,2000,1(4):52-56.
[7]张蕊.六价铬在土壤中迁移转化影响因素研究及风险评价[D].长春:吉林大学,2013.
[8]姜苹红,陈灿,向仁军.铬污染土壤的单一/复合还原处理及其长期稳定性研究[J].环境工程学报,2015,9(10):5091-5095.
[9]黄莹,徐民民,李书鹏,等.还原稳定化法修复六价铬污染土壤的中试研究[J].环境工程学报,2015,9(2):951-958.
[10]DENG S,KANG S,FENG N,et al.Mechanochemical mechanism of rapid dechlorination of hexachlorobenzene[J].Journal of Hazardous Materials,2017,333:116-154.DOI:10.1016/j.jhazmat.2017.03.022.
[11]ZHANG W,WANG H,HUANG J,et al.Acceleration and mechanistic studies of the mechanochemical dechlorination of HCB with iron powder and quartz sand[J].Chemical Engineering Journal,2014,239(3):185-191.DOI:10.1016/j.cej.2013.11.018.
[12]MONTINARO S,CONCAS A,PISU M,et al.Rationale of lead immobilization by ball milling in synthetic soils and remediation of heavy metals contaminated tailings[J].Chemical Engineering Journal,2009,155(1):123-131.DOI:10.1016/j.cej.2009.07.005.
[13]MONTINARO S,CONCAS A,PISU M,et al.Immobilization of heavy metals in contaminated soils through ball milling with and without additives[J].Chemical Engineering Journal,2008,142(3):271-284.DOI:10.1016/j.cej.2007.12.003.
[14]ZHANG Z X.Immobilisation of metal in quartz sands by ball milling[D].Auckland:Auckland University of Technology,2008.
[15]CONCAS A,MONTINARO S,PISU M,et al.Mechanochemical remediation of heavy metals contaminated soils:Modelling and experiments[J].Chemical Engineering Science,2007,62(18/19/20):5186-5192.DOI:10.1016/j.ces.2007.02.024.
[16]USEPA.Test methods for evaluating solid waste,physical/chemical methods,SW-846:Method 3050B[S].Washington,D.C.,1992.
[17]CEPA.Solid waste extraction procedure for leaching toxicity sulfuric acid&nitric acid method:HJ/T299-2007[S].2007.
[18]SANTHANAM P R,DREIZIN E L.Predicting conditions for scaled-up manufacturing of materials prepared by ball milling[J].Powder Technology,2012,221(5):403-411.DOI:10.1016/j.powtec.2012.01.037.
[19]DELOGU F,ORR′U R,CAO G.A novel macrokinetic approach for mechanochemical reactions[J].Chemical Engineering Science,2003,58(3):815-821.DOI:10.1016/S0009-2509(02)00612-7.
[20]BOURSIQUOT S,MULLET M,EHRHARDT J J.XPS study of the reaction of chromium(VI)with mackinawite(Fe S)[J].Surface&Interface Analysis,2010,34(1):293-297.DOI:10.1002/sia.1303.
[21]AND L D,GUILLON E.Removal of hexavalent chromium with a lignocellulosic substrate extracted from wheat bran[J].Environmental Science&Technology,2003,37(18):4235-4241.DOI:10.1021/es0342345.
[22]ZHANG W X,LI X Q,CAO J S.Reply to comments on stoichiometry of Cr(VI)immobilization using nanoscale zerovalent iron(n ZVI):A study with high-resolution X-ray photoelectron spectroscopy(HR-XPS)[J].Industrial&Engineering Chemistry Research,2009,47(7):2297-2297.DOI:10.1021/ie061655x.
[23]LEGRAND L,EL F A,MERCIER F,et al.Reduction of aqueous chromate by Fe(II)/Fe(III)carbonate green rust:Kinetic and mechanistic studies[J].Environmental Science&Technology,2004,38(17):4587-4595.DOI:10.1021/es035447x.