绿茶还原制备纳米铁对模拟地下水中Cr(Ⅵ)的去除效果
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摘要
利用绿茶提取液还原制备的纳米铁(GT-NIP)对水中六价铬具有良好的去除效果的原理,通过向含水层中注入GT-NIP可望实现六价铬在地下水中的原位去除,但尚未得到验证。为此,首先利用绿茶提取液还原法制备纳米铁,然后考察了其对水中六价铬的还原效果,再利用柱试验研究GT-NIP对模拟地下水中六价铬的去除效果。结果表明:利用绿茶提取液制备的纳米铁为圆球形,大小均匀,直径约为10～20nm,且分散性较好,其中Fe2+含量为55.6%,Fe3+含量为44.4%。GT-NIP悬浮液在水中对Cr(Ⅵ)具有良好的降解能力,当GT-NIP浓度为1.0g/L时,反应1h,初始浓度为100mg/L的Cr(Ⅵ)去除率达到96.8%;在柱试验中,GT-NIP可以顺利穿透砂柱,平均出流百分比为68.6%。浓度为100mg/L的Cr(Ⅵ)溶液流过该纳米铁砂柱后,流出液中Cr3+浓度约为0.20mg/L,Cr6+浓度为0.10～0.25mg/L,即六价铬去除率达到99%以上。
Nano-iron produced by reduction with green tea extract(GT-NIP)has good removal efficiency of hexavalent chromium in water.It is expected that the removal of hexavalent chromium from groundwater can be achieved in situ by injecting GTNIP into the aquifer;but this has not been verified yet.In this paper,we prepared nano-iron by reduction with green tea extract,measured its reduction effect on hexavalent chromium in water,and then used sand column to study its removal efficiency on hexavalent chromium in simulated groundwater.The GT-NIP we made were spherical and uniform in size,with a diameter of 10-20 nm and good dispersion stability in water.They consisted of 55.6% Fe~(2+)and 44.4% Fe~(3+).When GT-NIP concentration was 1-0g/L,after 1h of reaction,the removal rate of Cr(VI)with an initial concentration of 100mg/L reached 96-8%.In the column test,GT-NIP could pass through the sand column,with an average outflow percentage of 68.6%.When a Cr(Ⅵ)solution of 100mg/L was injected into the sand column,the concentration of Cr~(3+) was about 0.20mg/L,and the concentration of Cr6+in the effluent was 0.10-0.25mg/L;that is,the total removal rate of hexavalent chromium by GT-NIP was more than 99%.
Nano-iron produced by reduction with green tea extract(GT-NIP)has good removal efficiency of hexavalent chromium in water.It is expected that the removal of hexavalent chromium from groundwater can be achieved in situ by injecting GTNIP into the aquifer;but this has not been verified yet.In this paper,we prepared nano-iron by reduction with green tea extract,measured its reduction effect on hexavalent chromium in water,and then used sand column to study its removal efficiency on hexavalent chromium in simulated groundwater.The GT-NIP we made were spherical and uniform in size,with a diameter of 10-20 nm and good dispersion stability in water.They consisted of 55.6% Fe~(2+)and 44.4% Fe~(3+).When GT-NIP concentration was 1-0g/L,after 1h of reaction,the removal rate of Cr(VI)with an initial concentration of 100mg/L reached 96-8%.In the column test,GT-NIP could pass through the sand column,with an average outflow percentage of 68.6%.When a Cr(Ⅵ)solution of 100mg/L was injected into the sand column,the concentration of Cr~(3+) was about 0.20mg/L,and the concentration of Cr6+in the effluent was 0.10-0.25mg/L;that is,the total removal rate of hexavalent chromium by GT-NIP was more than 99%.
引文
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[2]秦泽敏,董黎明,刘平,等.零价纳米铁吸附去除水中六价铬的研究[J].中国环境科学.2014,34(12):3106-3111.(QIN Z M,DONG L M,LIU P,et al.Removal Cr6+from water using nanoscale zero-valent iron[J].China Environmental Science,2014,34(12):3106-3111.(in Chinese))
[3] GENG B,JIN Z,LI T,et al.Kinetics of hexavalent chromium removal from water by chitosan-Fe0nanoparticles[J].Chemosphere,2009,75(6):825-830.DOI:10.1016/j.chemosphere.2009.01.009.
[4] XING Y,CHEN X,WANG D.Electric1ally regenerated iron exchange for removal and recovery of Cr(VI)from wastewater[J].Water Science and Technology,2007,41(4):1439-1443.DOI:10.1021/es061499l.
[5]李政红,张胜,张翠云,等.土壤铬(VI)污染硫酸盐还原菌修复试验研究[J].南水北调与水利科技,2010,8(6):63-65.(LI Z H,ZHANG S,ZHANG C Y,et al.Experimental study of sulfate-reducing bacteria remediation for chromium(VI)contaminated soil[J].Southto-North Water Transfers and Water Science&Technology,2010,8(6):63-65.(in Chinese))
[6]MYTYCH P,CIES′A P,STASICKA Z.Photoredox processes in the Cr(VI)-Cr(III)-oxalate system and their environmental relevance[J].Applied Catalysis B Environmental,2005,59(3-4):161-170.DOI:10.1016/j.apcatb.2014.12.015.
[7] HSU C L,WANG S L,TZOU Y M.Photocatalytic reduction of Cr(VI)in the presence of NO3-and Cl-electrolytes as influenced by Fe[J].Environmental Science and Technology,2007,41(22):7907-7914.DOI:10.1021/es0718164.
[8]李山,杜梅先.活性炭表面改性及其对Cr(VI)的吸附性能[J].环境工程学报,2012,6(7):2367-2372.(LI S,DU M X.Surface modification of activated carbon and its adsorption for Cr(VI)[J].Chinese Journal of Environmental Engineering,2012,6(7):2367-2372.(in Chinese))
[9]汪婷,高滢,王晓英,等.纳米四氧化三铁同步去除水中的Pb(II)和Cr(III)离子[J].环境工程学报,2013,7(9):3476-3482.(WANG T,GAO Y,JIN X Y,et al.Simultaneous removal of Pb(II)and Cr(III)from wastewater by magnetite nanoparticles[J].Chinese Journal of Environmental Engineering,2013,7(9):3476-3482.(in Chinese))
[10]张威.韩占涛,许广明.纳米零价铁用于地下水污染修复时存在的问题与对策[J].南水北调与水利科技,2012,10(4):34-38.(ZHANG W,HAN Z T,XU G M.Problems and countermeasures of using nanoscale zero-valent iron in groundwater contamination remediation[J].South-to-North Water Transfers and Water Science&Technology,2012,10(4):34-38.(in Chinese))
[11]向林,黄文章,李林,等.纳米铁、纳米铁·铜对水体中芴的去除[J].科学技术与工程,2017,17(24):314-318.(XIANG L,HUANG W Z,LI L,et al.Nano iron,Nano-Fe-Cu removal of fluorene in water[J].Science Technology and Engineering,2017,17(24):314-318.(in Chinese))
[12]崔海炜,孙继朝,陈玺,等.PRB技术在垃圾渗滤液污染地下水修复中的可行性研究[J].南水北调与水利科技,2010,8(6):66-69.(CUI H W,SUN J C,CHEN X,et al.Feasibility study of mixture PRB technology in situ remediation of groundwater polluted by land fill leachate[J].South-to-North Water Transfers and Water Science&Technology,2010,8(6):66-69.(in Chinese))
[13] YAN W L,HERZING A A,KIELY C J,et al.Nanoscale zero-valent iron(nZVI):aspects of the core-shell structure and reactions with inorganic species in water[J].Journal of Contaminant Hydrology,2010,118(3/4):96-104.DOI:10.1016/j.conhyd.2010.09.003.
[14] SINGH R,MISRA V,SINGH R P.Removal of Cr(Ⅵ)by nanoscale zerovalent iron(nZVI)from soil contaminated with tannery wastes[J].Bulletin of Environmental Contamination and Toxicology,2012,88:210214.DOI:10.1007/s00128-011-0425-6.
[15]冯婧微.纳米零价铁及铁(氢)氧化物去除水中Cr(Ⅵ)和Cu2+的机制研究[D].沈阳:沈阳农业大学,2012.(FENG J W.Mechanisms of chromium and copper removal with nanoscale zero-valent iron and iron oxides/hydroxides[D].Shenyang:Shenyang Agricultural University,2012.(in Chinese))
[16]潘峰,尤奇中,王万峰,等.粉末碳负载纳米铁去除水中橙黄G的研究[J].科学技术与工程,2013,13(24):7126-7130.(PAN F,YOU Q Z,WANG W F,et al.Study on removal of orange G in aqueous solution using carbon powder supported nanoscale zero-valent iron particles[J].Science Technology and Engineering,2013,13(24):7126-7130.(in Chinese))
[17] MYSTRIOTI C,XENIDIS A,PAPSSSIOPI N.Application of iron nanoparticles synthesized by green tea for the removal of hexavalent chromium in column tests[J].Journal of Geoscience and Environment Protection,2014,2(4):28-36.DOI:10.4236/gep.2014.24005.
[18] BENNETT P,HE F,ZHAO D,et al.In situ testing of metallic iron nanoparticle mobility and reactivity in a shallowgranular aquifer[J].Journal of Contaminant Hydrology,2010,116(1).DOI:10.1016/j.jconhyd.2010.05.006.
[19]王棣,魏文侠,王琳玲,等.纳米铁原位注入技术对六价铬污染地下水的修复[J].环境工程学报,2018,12(2):521-526(WANG D,WEI W X,WANG L L,et al.Remediation of chromium(VI)contaminated groundwater by in-situ injection of nanoscale zero valent iron[J].Chinese Journal of Environmental Engineering.2018,12(2):521-526.(in Chinese))
[20] KRAJANGPAN S,JARABEK L,JEPPERSON J,et al.Polymer modified iron nanoparticles for environmental remediation.Polymer Preprints[J].PolymPrepr,2008,49(2):921-922.
[21] HWANG Y H,KIM D G,AHN Y T,et al.Fate of nitrogen species in nitrate reduction by nanoscale zero valent iron and characterization of the reaction kinetics[J].Water science and technology,2010,61(3):705-712.DOI:10.2166/wst.2010.895.
[22] MACHADO S,PACHECO J G,NOUWS H P A,et al.Characterization of green zero-valent iron nanoparticles produced with tree leaf extracts[J].Science of the Total Environment,2015,533:76-81.DOI:10.10616/j.scitotenv.2015.06.091.
[23] TRUSKEWYCZ A,SHUKLA R,BALL A S.Iron nanoparticles synthesized using green tea extracts for the fenton-like degradation of concentrated dye mixtures at elevated temperatures[J].Journal of Environmental Chemical Engineering.2016,4(4):4409-4417.DOI:10.1016/j.jece.2016.10.008.
[24] FAZLZADEH M,RAHMANI K,ZAREI A,et al.A novel green synthesis of zero valent iron nanoparticles(NZVI)using three plant extracts and their efficient application for removal of Cr(VI)from aqueous solutions[J].Advanced Powder Technology,2016,28(1):122-130.DOI:10.1016/j.apt.2016.09.003.
[25] ZHENGLI XIAO,MIN YUAN,BIN YANG,et al.Plant-mediated synthesis of highly active iron nanoparticles for Cr(VI)removal:Investigation of the leading biomolecules[J].Chemosphere.2016,02,05.DOI:10.1016/j.chemosphere.2016.02.056.
[26] LIN J W,WENG X L,DHARMARAJAN R,et al.Characterization and reactivity of iron based nanoparticles synthesized by tea extracts under various atmospheres[J].Chemosphere,2017,169.DOI:10.1016/j.chemosphere.2017.11.092.
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