Fe2+/H2O2体系内各种自由基在氧化NO中的作用

doi:10.11949/j.issn.0438-1157.20140976

化工学报 ›› 2015, Vol. 66 ›› Issue (1): 449-454.DOI: 10.11949/j.issn.0438-1157.20140976

Fe²⁺/H₂O₂体系内各种自由基在氧化NO中的作用

赵海谦^1,2, 高继慧¹, 周伟¹, 王忠华², 吴少华¹

1 哈尔滨工业大学能源科学与工程学院, 黑龙江哈尔滨 150001;
2 东北石油大学土木建筑工程学院, 黑龙江大庆 163318

收稿日期:2014-06-27 修回日期:2014-08-26 出版日期:2015-01-05 发布日期:2015-01-05
通讯作者: 高继慧
基金资助:
国家自然科学基金项目(51176043, 91434134, 51134015);黑龙江省青年科学基金项目(QC2014C047);黑龙江省教育厅项目(12541093)。

Roles of varied radicals in NO oxidation by Fe²⁺/H₂O₂ system

ZHAO Haiqian^1,2, GAO Jihui¹, ZHOU Wei¹, WANG Zhonghua², WU Shaohua¹

1 College of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China;
2 Institute of Civil Engineering & Architecture, Northeast Petroleum University, Daqing 163318, Heilongjiang, China

Received:2014-06-27 Revised:2014-08-26 Online:2015-01-05 Published:2015-01-05
Supported by:
supported by the National Natural Science Foundation of China(51176043, 91434134, 51134015), Heilongjiang Science Funds for Youths (QC2014C047), Heilongjiang Province Department of Education Funds (12541093).

摘要/Abstract

摘要：

Fe²⁺/H₂O₂体系可分解产生多种氧化性自由基, 主要包括O₂^-·、·OH和HO₂·。本文实验研究了O₂^-·、·OH及HO₂·在Fe²⁺/H₂O₂体系氧化NO气体过程中的作用。结果表明:在本实验条件下, O₂^-·对NO气体的氧化作用不明显;·OH及HO₂·是该体系氧化NO气体的主要活性物质, 其中·OH的氧化作用更大。加快自由基的生成速率可以增强Fe²⁺/H₂O₂体系对NO气体的氧化能力, 但O₂的生成速率同时加快。只有少量·OH及HO₂·参与NO的氧化, ·OH与HO₂·之间的快速反应是Fe²⁺/H₂O₂体系氧化NO过程中H₂O₂利用率低的主要原因。

关键词: Fe²⁺/H₂O₂体系, 自由基, 无效分解, NO

Abstract:

Fe²⁺/H₂O₂ system contains a variety of oxidizing free radicals, such as O₂^-·,·OH and HO₂·. In this paper, the behaviors of O₂^-·, ·OH and HO₂· played in NO oxidation by Fe²⁺/H₂O₂ system were investigated experimentally. The results demonstrated that the ability oxidizing NO of O₂^-· was weak at the experimental conditions adopted by this paper, while ·OH and HO₂· were the main active species for NO oxidation in Fe²⁺/H₂O₂ system, and the role of ·OH was more important. Acceleration of generating radical rate could not only promote the ability oxidizing NO gas of Fe²⁺/H₂O₂ system, but also accelerated O₂ generation rate. Only a small amount of ·OH and HO₂· participate in NO oxidation. In the process of NO oxidation by Fe²⁺/H₂O₂ system, the rapid reaction between ·OH and HO₂· was the major reason of for low utilization of H₂O₂ (invalid decomposition).

Key words: Fe²⁺/H₂O₂ system, radical, invalid decomposition, NO

中图分类号:

X511

赵海谦, 高继慧, 周伟, 王忠华, 吴少华. Fe²⁺/H₂O₂体系内各种自由基在氧化NO中的作用[J]. 化工学报, 2015, 66(1): 449-454.

ZHAO Haiqian, GAO Jihui, ZHOU Wei, WANG Zhonghua, WU Shaohua. Roles of varied radicals in NO oxidation by Fe²⁺/H₂O₂ system[J]. CIESC Journal, 2015, 66(1): 449-454.

参考文献 23

[1]	Zhang Xiaohui, Sun Shaozeng, Sun Rui, Li Xiaoli, Zeng Guang. Effects of bias combustion on volatile nitrogen transformation [J]. Asia-pacific Journal of Chemical Engineering, 2010, 5(3): 473-478
[2]	Barbut F, Yezli S, Otter J A. Activity in vitro of hydrogen peroxide vapour against clostridium difficile spores [J]. Journal of Hospital Infection, 2012, 80: 85-87
[3]	Christopherk Duesterberg, Stevene Mylon, David Waite T. pH effects on iron-catalyzed oxidation using Fenton's reagent [J]. Environ. Sci. Technol., 2008, 42: 8522-8527
[4]	Huang Guang, Wang Junhua, Dong Fengchun, Jia Yongtang. Application of activators for hydrogen peroxide bleaching at low temperature//2nd International Conference on Electronic & Mechanical Engineering and Information Technology[C]. Atlantis Press, 2012
[5]	Liu Yangxian(刘杨先), Pan Jianfeng(潘剑锋), Liu Yong(刘勇). Mass transfer-reaction kinetics for NO removal by process of UV/H2O2 oxidation and CaO absorption [J]. CIESC Journal (化工学报), 2013, 64(3): 1062-1068
[6]	Cooper C D, Clausen Ⅲ C A, Pettey L, Collins M, Pozo de Fernandez M. Investigation of ultraviolet light-enhanced H2O2 oxidation of NOx emissions [J]. Journal of Environmental Engineering, 2002, 128(1): 68-72
[7]	Hyun Ha Kim, Kazuhiko Tsunoda, Shinji Katsura. A novel plasma reactor for NO control using photocatalyst and hydrogen peroxide injection [J]. Industry Application, 1999, 35(6): 1306-1310
[8]	Collins M M, Cooper C D, Dietz J D, Clausen Ⅲ C A, Tazi L M. Pilot-scale evaluation of H2O2 injection to control NOx emissions [J]. Journal of Environmental Engineering, 2001, 127(4): 329-336
[9]	Piyavadee Limvoranusorn, David Cooper C, John D Dietz, Christian A Clausen, Lucas Pettey. Kinetic modeling of the gas-phase oxidation of nitric oxide using hydrogen peroxide [J]. Journal of Environmental Engineering, 2005, 131:518-525
[10]	Zhu Xian(朱贤), Zhou Yuegui(周月桂), Liu Yaobin(柳瑶斌), Peng Jun(彭军), Zhang Mingchuan(章明川). Experimental investigation on the flue gas desulfurization and denitrification of Ca(OH)2 humidified by hydrogen peroxide solution [J]. Boiler Technology(锅炉技术), 2010, 41(6): 75-78
[11]	Yang Liu(杨柳), Wang Hongsheng(王洪升), Liao Weiping(廖伟平). Simultaneous desulfurization and denitrification from flue gas of power plant by H2O2 [J]. Power Engineering(动力工程学报), 2011, 31(9): 689-692
[12]	Liu Yangxian(刘杨先), Zhang Jun(张军), Wang Zhuliang(王助良). Simultaneous desulfurization and denitrification by using combination of UV/H2O2 oxidation with Ca(OH)2 absorption [J]. CIESC Journal (化工学报), 2012, 63(10): 3277-3283
[13]	Walling C. Fenton's reagent revisited [J]. Accounts of Chemical Research, 1975, 8(4): 125-131
[14]	Mark Merchant, Ross Hardy, Stetson Williams. Quantitative detection of superoxide ions in whole blood of the American alligator [J]. Spectroscopy Letters, 2008, 41: 199-203
[15]	Babbs C F, Griffin D W. Scatchard analysis of methane sulfinic acid production from dimethyl sulfoxide: A method to quantify hydroxyl radical formation in physiologic systems [J]. Free Radical Biology and Medicine, 1989, 6(5): 493-503
[16]	Jiang Chengchun(姜成春), Pang Sunyan(庞素艳), Ma Jun(马军), Xie Weiping(谢炜平), Zou Yuan(邹原). Spectrophotometric determination of hydrogen peroxide in Fenton reaction with titanium oxalate [J]. China Water &Wastewater(中国给水排水), 2006, 22(4): 88-91
[17]	Sun Chu(孙楚), Li Shaofeng(李绍峰), Craig Williams, Tao Huchun(陶虎春). Spectrophotometric determination of hydrogen peroxide in O3/H2O2 advanced oxidation system with titanium oxalate [J]. Chemical Engineer(化学工程师), 2011, 189(6): 27-37
[18]	Liu Ruiheng(刘瑞恒), Fu Shiyu(付时雨), Zhan Huaiyu(詹怀宇). Spectrophotometric determination of superoxide anion radical with nitroblue tetrazolium [J]. Journal of Instrumental Analysis(分析测试学报), 2008, 27(4): 355-359
[19]	Mark Merchant, Ross Hardy, Stetson Williams. Quantitative detection of superoxide ions in whole blood of the American alligator (alligator mississippiensis) [J]. Spectroscopy Letters, 2008, 41: 199-203
[20]	Huie R E, Padmaja S. The reaction of NO with superoxide [J]. Free Radical Research, 1993, 18(4): 195-199
[21]	Yusuf G Adewuyi, Md A Khan, Nana Y Sakyi. Kinetics and modeling of the removal of nitric oxide by aqueous sodium persulfate simultaneously activated by temperature and Fe2+ [J]. Industrial & Engineering Chemistry Research, 2014, 53: 828-839
[22]	Pignatello J J. Dark and photoassisted iron(3+)-catalyzed degradation of chlorophenoxy herbicides by hydrogen peroxide [J]. Environmental Science & Technology, 1992, 26(5): 944-951
[23]	De Laat J, Gallard H. Catalytic decomposition of hydrogen peroxide by Fe(Ⅲ) in homogeneous aqueous solution: Mechanism and kinetic modeling [J]. Environmental Science & Technology, 1999, 33(16): 2726-2732

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Fe²⁺/H₂O₂体系内各种自由基在氧化NO中的作用

Roles of varied radicals in NO oxidation by Fe²⁺/H₂O₂ system

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