零价铁/过二硫酸盐去除水中硝基苯的还原与氧化机理

杨世迎; 马楠; 王静; 石超; 冯琳玉

doi:10.7524/j.issn.0254-6108.2013.11.016

环境化学

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杨世迎, 马楠, 王静, 石超, 冯琳玉. 零价铁/过二硫酸盐去除水中硝基苯的还原与氧化机理[J]. 环境化学, 2013, 32(11): 2127-2133. doi: 10.7524/j.issn.0254-6108.2013.11.016

引用本文:

YANG Shiying, MA Nan, WANG Jing, SHI Chao, FENG Linyu. Reduction and oxidation reaction mechanism of nitrobenzene removal by zero-valent iron and persulfate[J]. Environmental Chemistry, 2013, 32(11): 2127-2133. doi: 10.7524/j.issn.0254-6108.2013.11.016

Citation:

YANG Shiying, MA Nan, WANG Jing, SHI Chao, FENG Linyu. Reduction and oxidation reaction mechanism of nitrobenzene removal by zero-valent iron and persulfate[J]. Environmental Chemistry, 2013, 32(11): 2127-2133. doi: 10.7524/j.issn.0254-6108.2013.11.016

零价铁/过二硫酸盐去除水中硝基苯的还原与氧化机理

1.
海洋环境与生态教育部重点实验室, 青岛, 266100;
2.
中国海洋大学环境科学与工程学院, 青岛, 266100
基金项目:
中国海洋大学“中央高校基本科研业务费青年教师科研专项基金项目”(201113005)；国家自然科学基金(21107101)资助。

Reduction and oxidation reaction mechanism of nitrobenzene removal by zero-valent iron and persulfate

1.
Key Laboratory of Marine Environment and Ecology, Ministry of Education, Qingdao, 266100, China;
2.
College of Environmental Science and Engineering, Ocean University of China, Qingdao, 266100, China
Fund Project:

摘要: 探讨了零价铁(Fe0)/过二硫酸盐(PS)去除水中硝基苯(NB)体系中还原反应和氧化反应之间的相互影响机制.实验表明，采用依次投加Fe0和PS的方式去除NB，随着PS投加时间的推后，Fe0还原NB产生更多的苯胺(AN)，加入PS后，氧化去除AN更彻底;在NB/Fe0/PS的反应体系中，当NB和AN同时存在，SO4-·易和AN反应，而基本不去除NB.酸性条件和增加Fe0投加量，利于Fe0还原NB产生更多的AN，增加PS投加量利于AN的氧化去除.投加PS后AN的去除可能主要是发生了Fe2+催化PS的类Fenton氧化反应.
- 硝基苯 /
- 苯胺 /
- 零价铁 /
- 过二硫酸盐 /
- 还原与氧化
Abstract: This paper discussed the interaction between reduction and oxidation in the process of nitrobenzene (NB) removal by zero-valent iron (Fe0)/persulfate (PS) system. The results showed four trends. Firstly, when sequential additions of Fe0 and PS were adopted, the longer the delay of PS addition, the more aniline (AN) was produced by the reduction of NB by Fe0, and the more thorough oxidation of AN by adding PS seemed to occur. Secondly, in the system of NB/Fe0/PS where AN and NB both existed, sulfate radicals (SO4-·) tended to oxidize AN and little NB was oxidized. Thirdly, the initial pH and the dosage of Fe0 mainly influenced the reduction of NB by Fe0. Acidic environment and more Fe0 were conducive to the reduction of NB. Finally, the removal of AN in the system after introduction of PS seemed to be a Fenton-like reaction resulting from the catalyzed decomposition of PS by Fe2+ and the production of SO4-·.
- nitrobenzene /
- aniline /
- zero-valent iron /
- persulfate /
- reduction and oxidation

[1]	杨世迎, 杨鑫, 梁婷, 等. 零价铁还原和过硫酸盐氧化联合降解水中硝基苯[J]. 环境化学, 2012, 31(5): 682-686
[2]	Ambient Water Qualify Criteria[S]. U.S. Environmental protection Agency (USEPA), Washington, DC, 1980
[3]	Li Y P, Cao H B, Liu C M, et al. Electrochemical reduction of nitrobenzene at carbon nanotube electrode[J]. Journal of Hazardous Materials, 2007, 148(1/2): 158-163
[4]	Nefso E K, Burns S E, McGrathb C J. Degradation kinetics of TNT in the presence of six mineral surfaces and ferrous iron[J]. Journal of Hazardous Materials, 2005, 123(1/3): 79-88
[5]	Cao J S, Zhang W X, Brown D G, et al. Oxidation of lindane with Fe(Ⅱ)-activated sodium persulfate[J]. Environmental Science and Technology, 2008, 25(2): 221-228
[6]	Yang S Y, Wang P, Yang X, et al. Degradation efficiencies of azo dye Acid Orange 7 by the interaction of heat, UV and anions with common oxidants: persulfate, peroxymonosulfate and hydrogen peroxide[J]. Journal of Hazardous Materials, 2010, 179(1/3): 552-558
[7]	Liang C, Huang C F, Mohanty N, et al. A rapid spectrophotometric determination of persulfate anion in ISCO[J]. Chemosphere, 2008, 73(9): 1540-1543
[8]	Lee Y, Lo S L, Chiueh P T, et al. Microwave-hydrothermal decomposition of perfluorooctanoic acid in water by iron-activated persulfate oxidation[J]. Water Research, 2010, 44(3): 886-892
[9]	Michelle M S, Kathleen M J, John C W, et al. Mass transport effects on the kinetics of nitrobenzene reduction by iron metal[J]. Environmental Science and Technology, 2001, 35 (13): 2804-2811
[10]	Liang C, Bruell C, Marley M, et al. Persulfate oxidation for in situ remediation of TCE.Ⅱ. Activated by chelated ferrousion[J]. Chemosphere, 2004, 55(9): 1225-1233
[11]	Przemysaw D, Leonidas P. Impact of peroxydisulfate in the presence of zero valent iron on the oxidation of cyclohexanoic acid and naphthenic acids from oil sands process-affected water[J]. Environmental Science and Technology, 2012, 46(6): 8984-8991
[12]	Liang C, Bruell C, Marley M, et al. Persulfate oxidation for in situ remediation of TCE. I. Activated by ferrous ion with and without a persulfate-thiosulfate redox couple[J]. Chemosphere, 2004, 55(9): 1213-1223
[13]	Furukawa Y, Kim J, Watkins J, et al. Fromation of ferrihydrite and associated iron corrosion products in permeable reactive barriers of zero-valent iron[J]. Environmental Science and Technology, 2002, 36(24): 5469-5475
[14]	Guan Y, Ma J. Influence of pH on the formation of sulfate and hydroxyl radicals in the UV/peroxymonosulfate system[J]. Environmental Science and Technology, 2011, 45(10): 9308-9314
[15]	Zhang Y Q, Huang W L. In situ chemical oxidation of aniline by persulfate with iron(Ⅱ) activation at ambient temperature[J]. Chinese Chemical Letters, 2010, 21(9): 911-913
[16]	Moon B, Park Y, Park K. Fenton oxidation of Orange Ⅱ by pre-reduction using nanoscale zero-valent iron[J]. Desalination, 2011, 268(9): 249-252
[17]	吕国晓, 尹军, 刘蕾, 等. pH值对零价铁还原降解模拟地下水中硝基苯的影响[J]. 环境化学, 2009, 28(3): 355-359
[18]	Liang C, Lai M C. Trichloroethylene degradation by zero valent iron activated persulfate oxidation[J]. Environmental Engineering Science, 2008, 25(7): 1071-1077

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Citation:

零价铁/过二硫酸盐去除水中硝基苯的还原与氧化机理

1. 海洋环境与生态教育部重点实验室, 青岛, 266100;
2. 中国海洋大学环境科学与工程学院, 青岛, 266100

收稿日期: 2013-02-03

基金项目:

中国海洋大学“中央高校基本科研业务费青年教师科研专项基金项目”(201113005)；国家自然科学基金(21107101)资助。

关键词:

摘要: 探讨了零价铁(Fe0)/过二硫酸盐(PS)去除水中硝基苯(NB)体系中还原反应和氧化反应之间的相互影响机制.实验表明，采用依次投加Fe0和PS的方式去除NB，随着PS投加时间的推后，Fe0还原NB产生更多的苯胺(AN)，加入PS后，氧化去除AN更彻底;在NB/Fe0/PS的反应体系中，当NB和AN同时存在，SO4-·易和AN反应，而基本不去除NB.酸性条件和增加Fe0投加量，利于Fe0还原NB产生更多的AN，增加PS投加量利于AN的氧化去除.投加PS后AN的去除可能主要是发生了Fe2+催化PS的类Fenton氧化反应.

English Abstract

Reduction and oxidation reaction mechanism of nitrobenzene removal by zero-valent iron and persulfate

1. Key Laboratory of Marine Environment and Ecology, Ministry of Education, Qingdao, 266100, China;
2. College of Environmental Science and Engineering, Ocean University of China, Qingdao, 266100, China

Received Date: 2013-02-03

Fund Project:

Keywords:

Abstract: This paper discussed the interaction between reduction and oxidation in the process of nitrobenzene (NB) removal by zero-valent iron (Fe0)/persulfate (PS) system. The results showed four trends. Firstly, when sequential additions of Fe0 and PS were adopted, the longer the delay of PS addition, the more aniline (AN) was produced by the reduction of NB by Fe0, and the more thorough oxidation of AN by adding PS seemed to occur. Secondly, in the system of NB/Fe0/PS where AN and NB both existed, sulfate radicals (SO4-·) tended to oxidize AN and little NB was oxidized. Thirdly, the initial pH and the dosage of Fe0 mainly influenced the reduction of NB by Fe0. Acidic environment and more Fe0 were conducive to the reduction of NB. Finally, the removal of AN in the system after introduction of PS seemed to be a Fenton-like reaction resulting from the catalyzed decomposition of PS by Fe2+ and the production of SO4-·.

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零价铁/过二硫酸盐去除水中硝基苯的还原与氧化机理

Reduction and oxidation reaction mechanism of nitrobenzene removal by zero-valent iron and persulfate

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零价铁/过二硫酸盐去除水中硝基苯的还原与氧化机理

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Reduction and oxidation reaction mechanism of nitrobenzene removal by zero-valent iron and persulfate

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