3种氧化铁矿物/亚铁体系还原转化芳香硝基化合物的比较
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摘要
氧化铁矿物和亚铁广泛存在于厌氧环境中。亚铁-氧化铁共存的表面结合铁反应体系可由氧化铁矿物表面吸附部分亚铁离子形成。实验研究了磁铁矿、针铁矿和赤铁矿3种氧化铁矿物表面结合铁对硝基苯的反应活性及其动力学。在p H 7.5时,3种氧化铁矿物对Fe(Ⅱ)离子的吸附能力强弱顺序为针铁矿>磁铁矿>赤铁矿。氧化铁矿物对Fe(Ⅱ)的吸附能力是表面结合Fe(Ⅱ)体系还原硝基苯反应的前提条件,而吸附Fe(Ⅱ)形成的表面活性物质种类是体系还原硝基苯能力的关键因素。3种氧化铁矿物的还原能力依Fe2O3/Fe(Ⅱ)、α-Fe OOH/Fe(Ⅱ)、Fe3O4/Fe(Ⅱ)次序增强。氧化铁矿物/Fe(Ⅱ)体系对硝基苯的还原转化可用准一级动力学模拟。
Ferric minerals and Fe( Ⅱ) are ubiquitous species. Iron oxide-bound Fe( Ⅱ) systems( IOBSs)may comprise ferric minerals and adsorbed Fe( Ⅱ). Experiments were conducted to examine the reductive reactivity and kinetics of three IOBS associated with different ferric minerals( goethite,hematite,and magnetite). At p H 7. 5,the Fe( Ⅱ) adsorption capacity of the three ferric minerals followed the sequence: goethite,magnetite,and hematite in descending order. The ability of the ferric mineral to adsorb Fe( Ⅱ) was a prerequisite,while the presence of reactive substances on the IOBS surface was critical for the reduction of nitroaromatic compounds by these species. The reduction rate of nitrobenzene increased in the order: Fe( Ⅱ) associated with hematite
Ferric minerals and Fe( Ⅱ) are ubiquitous species. Iron oxide-bound Fe( Ⅱ) systems( IOBSs)may comprise ferric minerals and adsorbed Fe( Ⅱ). Experiments were conducted to examine the reductive reactivity and kinetics of three IOBS associated with different ferric minerals( goethite,hematite,and magnetite). At p H 7. 5,the Fe( Ⅱ) adsorption capacity of the three ferric minerals followed the sequence: goethite,magnetite,and hematite in descending order. The ability of the ferric mineral to adsorb Fe( Ⅱ) was a prerequisite,while the presence of reactive substances on the IOBS surface was critical for the reduction of nitroaromatic compounds by these species. The reduction rate of nitrobenzene increased in the order: Fe( Ⅱ) associated with hematite
引文
[1]PERCHET G.,SANGELY M.,GONI M.,et al.Microbial population changes during bioremediation of nitroaromatic-and nitramine-contaminated lagoon.International Biodeterioration&Biodegradation,2008,61(4):304-312
[2]李杏茹,何孟常,孙艳,等.硝基苯类化合物在黄河小浪底至高村河段水体中的分布特征.环境科学,2006,27(3):513-518LI Xingru,HE Mengchang,SUN Yan,et al.Distribution of nitrobenzenes in the Yellow River from Xiaolangdi to Gaocun reach.Environmental Science,2006,27(3):513-518(in Chinese)
[3]王斌,赵劲松,王晓栋,等.应用受体学说模型研究硝基苯类化合物的致毒机理.环境化学,2004,23(1):80-84WANG Bin,ZHAO Jinsong,WANG Xiaodong,et al.Using receptor theory model to study the mechanism of toxicity of nitrobenzene derivatives.Environmental Chemistry,2004,23(1):80-84(in Chinese)
[4]KLAUSEN J.,TROBER S.P.,HADERLEIN S.B.,et al.Reduction of substituted nitrobenzenes by Fe(Ⅱ)in aqueous mineral suspensions.Environmental Science and Technology,1995,29(9):2396-2404
[5]LUAN Fubo,XIE Li,LI Jun,et al.Abiotic reduction of nitroaromatic compounds by Fe(Ⅱ)associated with iron oxides and humic acid.Chemosphere,2013,91(7):1035-1041
[6]JEON B.H.,DEMPSEY B.A.,BURGOS W.D.Kinetics and mechanisms for reactions of Fe(Ⅱ)with iron(III)oxides.Environmental Science&Technology,2003,37(15):3309-3315
[7]CHARLET L.,SILVESTER E.,LIGER E.N-compound reduction and actinide immobilisation in surficial fluids by Fe(Ⅱ):The surface Fe(Ⅲ)O Fe(Ⅱ)OH degrees species,as major reductant.Chemical Geology,1998,151(1/2/3/4):85-93
[8]PERES C.M.,NAVEAU H.,AGATHOS S.N.Biodegradation of nitrobenzene by its simultaneous reduction into aniline and mineralization of the aniline formed.Applied Microbiology and Biotechnology,1998,49(3):343-349
[9]KLUPINSKI T.P.,CHIN Y.P.,TRAINA S.J.Abiotic degradation of pentachloronitrobenzene by Fe(Ⅱ):Reactions on goethite and iron oxide nanoparticles.Environmental Science&Technology,2004,38(16):4353-4360
[10]SCHULTZ C.A.,GRUNDL T.J.p H dependence on reduction rate of 4-Cl-nitrobenzene by Fe(Ⅱ)/montmorillonite systems.Environmental Science&Technology,2000,34(17):3641-3648
[11]AMONETTE J.E.,WORKMAN D.J.,KENNEDY D.W.,et al.Dechlorination of carbon tetrachloride by Fe(Ⅱ)associated with goethite.Environmental Science&Technology,2000,34(21):4606-4613
[12]SCHULTZ C.A.,GRUNDL T.J.p H dependence on reduction rate of 4-Cl-nitrobenzene by Fe(Ⅱ)/montmorillonite systems.Environmental Science&Technology,2000,34(17):3641-3648
[13]魏俊峰,吴大清.矿物-水界面的表面离子化和络合反应模式.地球科学进展,2000,15(1):90-96WEI Junfeng,WU Daqing.Surface ionization and surface complexation models at mineral/water interface.Advance in Earth Sciences,2000,15(1):90-96(in Chinese)
[14]LIU Hui,WEI Yu,SUN Yuhan.The formation of hematite from ferrihydrite using Fe(Ⅱ)as a catalyst.Journal of Molecular Catalysis A:Chemical,2005,226(1):135-140
[2]李杏茹,何孟常,孙艳,等.硝基苯类化合物在黄河小浪底至高村河段水体中的分布特征.环境科学,2006,27(3):513-518LI Xingru,HE Mengchang,SUN Yan,et al.Distribution of nitrobenzenes in the Yellow River from Xiaolangdi to Gaocun reach.Environmental Science,2006,27(3):513-518(in Chinese)
[3]王斌,赵劲松,王晓栋,等.应用受体学说模型研究硝基苯类化合物的致毒机理.环境化学,2004,23(1):80-84WANG Bin,ZHAO Jinsong,WANG Xiaodong,et al.Using receptor theory model to study the mechanism of toxicity of nitrobenzene derivatives.Environmental Chemistry,2004,23(1):80-84(in Chinese)
[4]KLAUSEN J.,TROBER S.P.,HADERLEIN S.B.,et al.Reduction of substituted nitrobenzenes by Fe(Ⅱ)in aqueous mineral suspensions.Environmental Science and Technology,1995,29(9):2396-2404
[5]LUAN Fubo,XIE Li,LI Jun,et al.Abiotic reduction of nitroaromatic compounds by Fe(Ⅱ)associated with iron oxides and humic acid.Chemosphere,2013,91(7):1035-1041
[6]JEON B.H.,DEMPSEY B.A.,BURGOS W.D.Kinetics and mechanisms for reactions of Fe(Ⅱ)with iron(III)oxides.Environmental Science&Technology,2003,37(15):3309-3315
[7]CHARLET L.,SILVESTER E.,LIGER E.N-compound reduction and actinide immobilisation in surficial fluids by Fe(Ⅱ):The surface Fe(Ⅲ)O Fe(Ⅱ)OH degrees species,as major reductant.Chemical Geology,1998,151(1/2/3/4):85-93
[8]PERES C.M.,NAVEAU H.,AGATHOS S.N.Biodegradation of nitrobenzene by its simultaneous reduction into aniline and mineralization of the aniline formed.Applied Microbiology and Biotechnology,1998,49(3):343-349
[9]KLUPINSKI T.P.,CHIN Y.P.,TRAINA S.J.Abiotic degradation of pentachloronitrobenzene by Fe(Ⅱ):Reactions on goethite and iron oxide nanoparticles.Environmental Science&Technology,2004,38(16):4353-4360
[10]SCHULTZ C.A.,GRUNDL T.J.p H dependence on reduction rate of 4-Cl-nitrobenzene by Fe(Ⅱ)/montmorillonite systems.Environmental Science&Technology,2000,34(17):3641-3648
[11]AMONETTE J.E.,WORKMAN D.J.,KENNEDY D.W.,et al.Dechlorination of carbon tetrachloride by Fe(Ⅱ)associated with goethite.Environmental Science&Technology,2000,34(21):4606-4613
[12]SCHULTZ C.A.,GRUNDL T.J.p H dependence on reduction rate of 4-Cl-nitrobenzene by Fe(Ⅱ)/montmorillonite systems.Environmental Science&Technology,2000,34(17):3641-3648
[13]魏俊峰,吴大清.矿物-水界面的表面离子化和络合反应模式.地球科学进展,2000,15(1):90-96WEI Junfeng,WU Daqing.Surface ionization and surface complexation models at mineral/water interface.Advance in Earth Sciences,2000,15(1):90-96(in Chinese)
[14]LIU Hui,WEI Yu,SUN Yuhan.The formation of hematite from ferrihydrite using Fe(Ⅱ)as a catalyst.Journal of Molecular Catalysis A:Chemical,2005,226(1):135-140