铸铁和椰壳活性炭混合介质修复高浓度Cr(Ⅵ)污染地下水研究
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摘要
铬是人体和动物必需的微量元素之一。但高浓度的铬,尤其是地下水中的Cr(Ⅵ)可能对人体健康和环境造成很大的危害,因此研究高浓度Cr(Ⅵ)污染地下水的修复技术至关重要。应用铸铁和椰壳活性炭作为模拟柱中渗透反应格栅(PRB)的反应介质,为了防止实验过程发生堵塞,添加适当河沙,通过铸铁的还原作用及椰壳活性炭的吸附作用研究PRB对高浓度Cr(Ⅵ)污染地下水的修复效能。结果表明:铸铁、椰壳活性炭、河沙的质量比为3∶1∶4、Cr(Ⅵ)为400 mg/L条件下,完全穿透时反应材料对Cr(Ⅵ)整体去除率为67.0%,PRB反应介质寿命为165d;侧孔Cr(Ⅵ)浓度随时间延长而逐渐增大,离进水口越近,材料去除Cr(Ⅵ)的能力降低越快;出水及沿程在没有Cr(Ⅵ)检出时pH为4.5～7.0,出水有Cr(Ⅵ)检出时pH均大于7.0;出水中无Cr(Ⅵ)检出时,总铁(TFe)含量较高,Fe(Ⅲ)含量较少,有大量Fe(Ⅱ)产生,出水有Cr(Ⅵ)检出时,对应的Fe(Ⅲ)和TFe检出浓度均较低,说明柱体内铸铁材料基本钝化完全。
Chromium is one of the essential trace elements for human and animal.But the high concentration of chromium especially the Cr(Ⅵ)in groundwater may cause great harm for human health and environment.Therefore,it is very important to study the remediation technology of groundwater contaminated by high concentration Cr(Ⅵ).In this paper,cast iron and coconut shell activated carbon were used as simulated column permeable reactive barrier(PRB)reaction medium.In order to prevent the potential clogging problem during the experiment,appropriate river sand was packed in the column to study the PRB remediation efficiency of high concentration Cr(Ⅵ)contaminated groundwater by reduction of cast iron and adsorption of coconut shell activated carbon.The results showed that mass concentration 400 mg/L Cr(Ⅵ)was remediated by cast iron,coconut shell activated carbon and river sand mass ratio of 3∶1∶4,the overall removal rate of Cr(Ⅵ)by reactive materials was 67.0% when column was fully penetrated,and the life of PRB reaction medium was 165 days.The Cr(Ⅵ)concentration in the side ports gradually increased with time,and the closer to the inlet,the faster the ability of material to remove Cr(Ⅵ)decreased.The pH of the effluent and along the way was 4.5-7.0 when no Cr(Ⅵ)was detected,and the pH was greater than 7.0 when the Cr(Ⅵ)was detected.When there was no Cr(Ⅵ)detected in the effluent,the content of total iron(TFe)was higher,Fe(Ⅲ)was less,and Fe(Ⅱ)was abundant.When Cr(Ⅵ)was detected in the effluent,the TFe and Fe(Ⅲ)content was less,which indicated that the cast iron material in the column was passivated completely.
Chromium is one of the essential trace elements for human and animal.But the high concentration of chromium especially the Cr(Ⅵ)in groundwater may cause great harm for human health and environment.Therefore,it is very important to study the remediation technology of groundwater contaminated by high concentration Cr(Ⅵ).In this paper,cast iron and coconut shell activated carbon were used as simulated column permeable reactive barrier(PRB)reaction medium.In order to prevent the potential clogging problem during the experiment,appropriate river sand was packed in the column to study the PRB remediation efficiency of high concentration Cr(Ⅵ)contaminated groundwater by reduction of cast iron and adsorption of coconut shell activated carbon.The results showed that mass concentration 400 mg/L Cr(Ⅵ)was remediated by cast iron,coconut shell activated carbon and river sand mass ratio of 3∶1∶4,the overall removal rate of Cr(Ⅵ)by reactive materials was 67.0% when column was fully penetrated,and the life of PRB reaction medium was 165 days.The Cr(Ⅵ)concentration in the side ports gradually increased with time,and the closer to the inlet,the faster the ability of material to remove Cr(Ⅵ)decreased.The pH of the effluent and along the way was 4.5-7.0 when no Cr(Ⅵ)was detected,and the pH was greater than 7.0 when the Cr(Ⅵ)was detected.When there was no Cr(Ⅵ)detected in the effluent,the content of total iron(TFe)was higher,Fe(Ⅲ)was less,and Fe(Ⅱ)was abundant.When Cr(Ⅵ)was detected in the effluent,the TFe and Fe(Ⅲ)content was less,which indicated that the cast iron material in the column was passivated completely.
引文
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[3]GHEJU M.Hexavalent chromium reduction with zero-valent iron(ZVI)in aquatic systems[J].Water,Air,&Soil Pollution,2011,222(1/2/3/4):103-148.
[4]BASU A,JOHNSON T M.Determination of hexavalent chromium reduction using Cr stable isotopes:isotopic fractionation factors for permeable reactive barrier materials[J].Environmental Science&Technology,2012,46(10):5353-5360.
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[6]陈子方,李琴,赵勇胜.Al(Ⅲ)对糖浆溶液中有机还原物质还原六价铬的影响[J].中国环境科学,2015,35(12):3628-3633.
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[8]MOLOKWANE P E,CHIRWA E M.Modelling biological Cr(Ⅵ)reduction in aquifer microcosm column systems[J].Water Science and Technology,2013,67(12):2733-2738.
[9]陈子方,赵勇胜,孙家强,等.铅和铬污染包气带及再释放规律的实验研究[J].中国环境科学,2014,34(9):2211-2216.
[10]素善治,袁勇.污染地下水原位处理方法:可渗透反应墙[J].环境污染治理技术与设备,2002,3(1):47-51.
[11]周启星,林海芳.污染土壤及地下水修复的PRB技术及展望[J].环境污染治理技术与设备,2001,2(5):48-53.
[12]徐慧,仵彦卿.六价铬在具有渗透性反应墙的渗流槽中迁移实验研究[J].生态环境学报,2010,19(8):1941-1946.
[13]USEPA.An in situ permeable reactive barrier for the treatment of hexavalent chromium and trichloroethylene in ground water,Vol.1:design and installation[R].Washington,D.C.:USEPA,1999.
[14]BLOWES D W,PTACEK C J,JAMBOR J L.In-situ remediation of Cr(Ⅵ)-contaminated groundwater using permeable reactive walls:laboratory studies[J].Environmental Science&Technology,1997,31(12):3348-3357.
[15]POWELL R M,PULS R W,HIGHTOWER S K,et al.Coupled iron corrosion and chromate reduction:mechanisms for subsurface remediation[J].Environmental Science&Technology,1995,29(8):1913-1922.
[16]PULS R W,CLARK D A,PAUL C J,et al.Transport and transformation of hexavalent chromium through soils and into ground water[J].Jouranl of Soil Contamination,1994,3(2):203-224.
[17]EARY L E,RAI D.Chromate removal from aqueous wastes by reduction with ferrous ion[J].Environmental Science&Technology,1988,22(8):972-977.
[18]SCHWERTMANN U,GASSER U,STICHER H.Chromiumfor-iron substitution in synthetic goethites[J].Geochimica et Cosmochimica Acta,1989,53(6):1293-1297.
[19]LEE J W,CHA D K,OH Y K et al.Wastewater screening method for evaluating applicability of zero-valent iron to industrial wastewater[J].Journal of Hazardous Materials,2010,180(1/2/3):354-360.
[20]PRATT A R,BLOWES D W,PTACEK C J.Products of chromate reduction on proposed subsurface remediation material[J].Environmental Science&Technology,1997,31(9):2492-2498.
[21]ROH Y,LEE S Y,ELLESS M P.Characterization of corrosion products in the permeable reactive barriers[J].Environmental Geology,2000,40(1/2):184-194.
[22]WILKINA R T,ACREEA S D,ROSSA R R,et al.Fifteenyear assessment of a permeable reactive barrier for treatment of chromate,trichloroethylene in groundwater[J].Science of the Total Environment,2014,468/469:186-194.
[23]李志红,王广才,史浙明,等.渗透反应格栅技术综述:填充材料实验研究、修复技术实例和系统运行寿命[J].环境化学,2017,36(2):316-327.
[2]GALLIOS G P,VACLAVIKOVA M.Removal of chromium(Ⅵ)from water streams:a thermodynamic study[J].Environmental Chemistry Letters,2008,6(4):235-240.
[3]GHEJU M.Hexavalent chromium reduction with zero-valent iron(ZVI)in aquatic systems[J].Water,Air,&Soil Pollution,2011,222(1/2/3/4):103-148.
[4]BASU A,JOHNSON T M.Determination of hexavalent chromium reduction using Cr stable isotopes:isotopic fractionation factors for permeable reactive barrier materials[J].Environmental Science&Technology,2012,46(10):5353-5360.
[5]生贺,于锦秋,刘登峰,等.乳化植物油强化地下水中Cr(Ⅵ)的生物地球化学还原研究[J].中国环境科学,2015,35(6):1693-1699.
[6]陈子方,李琴,赵勇胜.Al(Ⅲ)对糖浆溶液中有机还原物质还原六价铬的影响[J].中国环境科学,2015,35(12):3628-3633.
[7]BENCHEIKH LATMANI R,OBRAZTSOVA A,MACK MR,et al.Toxicity of Cr(Ⅲ)to Shewanellasp.strain MR-4during Cr(Ⅵ)reduction[J].Environmental Science&Technology,2007,41(1):214-220.
[8]MOLOKWANE P E,CHIRWA E M.Modelling biological Cr(Ⅵ)reduction in aquifer microcosm column systems[J].Water Science and Technology,2013,67(12):2733-2738.
[9]陈子方,赵勇胜,孙家强,等.铅和铬污染包气带及再释放规律的实验研究[J].中国环境科学,2014,34(9):2211-2216.
[10]素善治,袁勇.污染地下水原位处理方法:可渗透反应墙[J].环境污染治理技术与设备,2002,3(1):47-51.
[11]周启星,林海芳.污染土壤及地下水修复的PRB技术及展望[J].环境污染治理技术与设备,2001,2(5):48-53.
[12]徐慧,仵彦卿.六价铬在具有渗透性反应墙的渗流槽中迁移实验研究[J].生态环境学报,2010,19(8):1941-1946.
[13]USEPA.An in situ permeable reactive barrier for the treatment of hexavalent chromium and trichloroethylene in ground water,Vol.1:design and installation[R].Washington,D.C.:USEPA,1999.
[14]BLOWES D W,PTACEK C J,JAMBOR J L.In-situ remediation of Cr(Ⅵ)-contaminated groundwater using permeable reactive walls:laboratory studies[J].Environmental Science&Technology,1997,31(12):3348-3357.
[15]POWELL R M,PULS R W,HIGHTOWER S K,et al.Coupled iron corrosion and chromate reduction:mechanisms for subsurface remediation[J].Environmental Science&Technology,1995,29(8):1913-1922.
[16]PULS R W,CLARK D A,PAUL C J,et al.Transport and transformation of hexavalent chromium through soils and into ground water[J].Jouranl of Soil Contamination,1994,3(2):203-224.
[17]EARY L E,RAI D.Chromate removal from aqueous wastes by reduction with ferrous ion[J].Environmental Science&Technology,1988,22(8):972-977.
[18]SCHWERTMANN U,GASSER U,STICHER H.Chromiumfor-iron substitution in synthetic goethites[J].Geochimica et Cosmochimica Acta,1989,53(6):1293-1297.
[19]LEE J W,CHA D K,OH Y K et al.Wastewater screening method for evaluating applicability of zero-valent iron to industrial wastewater[J].Journal of Hazardous Materials,2010,180(1/2/3):354-360.
[20]PRATT A R,BLOWES D W,PTACEK C J.Products of chromate reduction on proposed subsurface remediation material[J].Environmental Science&Technology,1997,31(9):2492-2498.
[21]ROH Y,LEE S Y,ELLESS M P.Characterization of corrosion products in the permeable reactive barriers[J].Environmental Geology,2000,40(1/2):184-194.
[22]WILKINA R T,ACREEA S D,ROSSA R R,et al.Fifteenyear assessment of a permeable reactive barrier for treatment of chromate,trichloroethylene in groundwater[J].Science of the Total Environment,2014,468/469:186-194.
[23]李志红,王广才,史浙明,等.渗透反应格栅技术综述:填充材料实验研究、修复技术实例和系统运行寿命[J].环境化学,2017,36(2):316-327.
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