CIESC Journal ›› 2018, Vol. 69 ›› Issue (5): 2250-2254.doi: 10.11949/j.issn.0438-1157.20171274

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Main active substances and useless consumption path of free radicals in Fe (Ⅱ)/H2O2 system during NO oxidation process

ZHAO Haiqian1, LIU Chenghao1, ZHOU Wei2, WANG Zhonghua1, QI Hanbing1, GAO Jihui2   

  1. 1. Institute of Civil Engineering & Architecture, Northeast Petroleum University, Daqing 163318, Heilongjiang, China;
    2. College of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China
  • Received:2017-09-19 Revised:2017-12-13 Online:2018-05-05 Published:2018-01-16
  • Supported by:

    supported by the National Natural Science Foundation of China(51606036, 91434134) and Innovative Talents Training Plan for Youth Scholars in Heilongjiang Province (UNPYSCT-2016085).


Low utilization of H2O2 is a bottleneck in the application of Fe(Ⅱ)/H2O2 oxidation system. Free radicals useless consumption is one of the main reasons for the low utilization of H2O2. In this paper, the effect of H2O2 and various free radicals on oxidation of NO and the useless consumption pathways of the free radicals in Fe(Ⅱ)/H2O2 system were studied based on NO oxidation background. The results showed that the ability of directly oxidize NO by H2O2 was very weak. Although both ·OH and HO2· had the ability to oxidize NO, the oxidation ability of ·OH was greater than that of HO2·. In the process of NO oxidation, the vast majority of ·OH and HO2· was uselessly consumed through the rapid recombination of these two kinds of radicals, which seriously affected the utilization of H2O2. Therefore, simultaneous presence of both ·OH and HO2· radicals should be avoided when Fe(Ⅱ)/H2O2 system was adopted to degrade the pollutants.

Key words: Fe (Ⅱ)/H2O2 system, NO, active substance, useless consumption, ·OH

CLC Number: 

  • O643

[1] 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(1):85-87.
[2] HUANG D, HU C, ZENG G, et al. Combination of Fenton processes and biotreatment for wastewater treatment and soil remediation[J]. Science of the Total Environment, 2017, 574:1599-1610.
[3] TANG P, JI B, SUN G. Whiteness improvement of citric acid crosslinked cotton fabrics:H2O2 bleaching under alkaline condition[J]. Carbohydrate Polymers, 2016, 147:139-145.
[4] WALLING C. Fenton's reagent revisited[J]. Accounts of Chemical Research, 1975, 8(4):125-131.
[5] FISCHBACHER A, VON SONNTAG C, SCHMIDT T C. Hydroxyl radical yields in the Fenton process under various pH, ligand concentrations and hydrogen peroxide/Fe (Ⅱ) ratios[J]. Chemosphere, 2017, 182:738-744.
[6] COLLINS M M, COOPER C D, DIETZ J D, et al. Pilot-scale evaluation of H2O2 injection to control NOx emissions[J]. Journal of Environmental Engineering, 2001, 127(4):329-336.
[7] LIMVORANUSOM P, COOPER C D, DIETZ J D, et al. Kinetic modeling of the gas-phase oxidation of nitric oxide using hydrogen peroxide[J]. Journal of Environmental Engineering, 2005, 131(4):518-525.
[8] 王洪升. 燃煤烟气脱硫脱硝一体化工艺试验研究[D]. 南京:南京师范大学, 2011. WANG H S. Experimental study on entegrated process of flue gas desulfurization and denitrification[D]. Nanjing:Nanjing Normal University, 2011.
[9] GUO R T, PAN W G, ZHANG X B, et al. Removal of NO by using Fenton reagent solution in a lab-scale bubbling reactor[J]. Fuel, 2011, 90(11):3295-3298.
[10] 范春贞, 李彩亭, 路培, 等. 类芬顿试剂液相氧化法脱硝的实验研究[J]. 中国环境科学, 2012, 32(6):988-993. FAN C Z, LI C T, LU P, et al. Experimental research of purification NO-containing gas by aqueous oxidation with Fenton-like agent[J]. China Environmental Science, 2012, 32(6):988-993.
[11] ZHAO Y, HAO R L, GUO Q, et al. Simultaneous removal of SO2 and NO by a vaporized enhanced-Fenton reagent[J]. Fuel Processing Technology, 2015, 137:8-15.
[12] 刘杨先, 潘剑锋, 刘勇. UV/H2O2氧化联合CaO吸收脱除NO的传质-反应动力学[J]. 化工学报, 2013, 64(3):1062-1068. LIU Y X, PAN J F, LIU Y. Mass transfer-reaction kinetics for NO removal by process of UV/H2O2 oxidation and CaO absorption[J]. CIESC Journal, 2013, 64(3):1062-1068.
[13] KIM H H, TSUNODA K, KATSURA S, et al. A novel plasma reactor for NO control using photocatalyst and hydrogen peroxide injection[J]. Industry Application, 1999, 35(6):1306-1310.
[14] COOPER C D, CLAUSEN Ⅲ C A, PETTEY L, et al. Investigation of ultraviolet light-enhanced H2O2 oxidation of NOx emissions[J]. Journal of Environmental Engineering, 2002, 128(1):68-72.
[15] 马双忱, 马京香, 赵毅, 等. 采用UV/H2O2体系进行烟气脱硫脱硝的实验研究[J]. 中国电机工程学报, 2009, 29(5):28-31. MA S C, MA J X, ZHAO Y, et al. Experimental study on desulfurization and denitrification using UV/H2O2 system[J]. Proceedings of the CSEE, 2009, 29(5):28-31.
[16] 郭天祥. 新型复合吸收剂液相同时脱硫脱硝的实验研究[D]. 北京:华北电力大学, 2011. GUO T X. Experimental investigation on simultaneous removal of SO2 and NOx in liquid phase by new-type complex absorbent[D]. Beijing:North China Electric Power University, 2011.
[17] ZHAO Y, HAO R, YUAN B, et al. Simultaneous removal of SO2, NO and Hg0 through an integrative process utilizing a cost-effective complex oxidant[J]. Journal of Hazardous Materials, 2016, 301:74-83.
[18] WANG Z, WANG Z, YE Y, et al. Study on the removal of nitric oxide (NO) by dual oxidant (H2O2/S2O82-) system[J]. Chemical Engineering Science, 2016, 145:133-140.
[19] CHEN L W, MA J, LI X C, et al. Strong enhancement on Fenton oxidation by addition of hydroxylamine to accelerate the ferric and ferrous iron cycles[J]. Environmental Science & Technology, 2011, 45(9):3925-3930.
[20] MA J, SONG W, CHEN C, et al. Fenton degradation of organic compounds promoted by dyes under visible irradiation[J]. Environmental Science & Technology, 2005, 39(15):5810-5815.
[21] 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.
[22] 刘瑞恒, 付时雨, 詹怀宇. 氯化硝基四氮唑蓝显色检测超氧阴离子自由基的研究[J]. 分析测试学报, 2008, 27(4):355-359. LIU R H, FU S Y, ZHAN H Y. Spectrophotometric determination of superoxide anion radical with nitroblue tetrazolium[J]. Journal of Instrumental Analysis, 2008, 27(4):355-359.
[23] MERCHANT M, HARDY R, WILLIAMS S. Quantitative detection of superoxide ions in whole blood of the American alligator (alligator mississippiensis)[J]. Spectroscopy Letters, 2008, 41(5):199-203.
[24] 姜成春, 庞素艳, 马军, 等. 钛盐光度法测定Fenton氧化中的过氧化氢[J]. 中国给水排水, 2006, 22(4):88-91. JIANG C C, PANG S Y, MA J, et al. Spectrophotometric determination of hydrogen peroxide in Fenton reaction with titanium oxalate[J]. China Water &Waste Water, 2006, 22(4):88-91.
[25] 石宁, 谢传欣, 于丽明, 等. 双氧水分解危险特性的定量研究[J]. 大氮肥, 2010, 33(1):53-55. SHI N, XIE C X, YU L M, et al. Quantitative research of hazardous property in hydrogen peroxide decomposition[J]. Large Scale Nitrogenous Fertilizer Industry, 2010, 33(1):53-55.
[26] HE J, YANG X, MEN B, et al. Interfacial mechanisms of heterogeneous Fenton reactions catalyzed by iron-based materials:a review[J]. Journal of Environmental Sciences, 2016, 39:97-109.
[27] DING X, HO W, SHANG J, et al. Self doping promoted photocatalytic removal of no under visible light with Bi2MoO6:indispensable role of superoxide ions[J]. Applied Catalysis B:Environmental, 2016, 182:316-325.
[28] PERES-BENITO J F. Iron (Ⅲ)-hydrogen peroxide reaction:kinetic evidence of a hydroxyl-mediated chain mechanism[J]. The Journal of Physical Chemistry A, 2004, 108(22):4853-4858.
[29] DE LAAT J, GALLARD H É. 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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