基于亚硫酸盐的六价铬-苯酚污染废水协同处理研究
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摘要
探讨基于亚硫酸盐的六价铬-苯酚复合污染废水协同处理的可行性。探究重金属-六价铬、有机物-苯酚协同处理的效果、影响因素及机理。研究结果表明:该体系可以快速且同时实现六价铬还原和苯酚降解;降解效率随体系初始pH降低而逐渐增大,本实验条件范围内最佳pH为3.0;Fe2+,Fe3+和Mn2+均在不同程度上抑制六价铬还原和苯酚降解,Al3+对该体系处理效果没有显著影响;仅当有氧气存在时体系能生成羟基自由基和硫酸根自由基进而氧化降解苯酚,其中起主要作用的是硫酸根自由基。该体系可以为复合污染废水的处理提供有效的依据,实现协同、绿色的水处理。
The feasibility of sulfite-based synergistic treatment of hexavalent chromium and phenol polluted wastewater was investigated. The synergetic transformation efficiency, influencing factors and correlated mechanisms were analysed. The results show that this system can achieve the simultaneous and rapid effect of hexavalent chromium reduction and phenol oxidation. The transformation efficiency of both pollutants gradually increases with the decrease of pH, and the optimum pH is 3.0 in this series of experiments. Fe2+, Fe3+, Mn2+ all inhibit hexavalent chromium reduction and phenol degradation to some extent, but Al3+ has little influence on the treatment. In this synergistic reaction system, oxygen is necessary in generating the free radicals, such as hydroxyl radical and sulfate radical. Sulfate radical plays a major role in degrading phenol. This study can provide a basis for remediation of composite wastewater contamination, as a realization of synergistic and green wastewater treatment.
The feasibility of sulfite-based synergistic treatment of hexavalent chromium and phenol polluted wastewater was investigated. The synergetic transformation efficiency, influencing factors and correlated mechanisms were analysed. The results show that this system can achieve the simultaneous and rapid effect of hexavalent chromium reduction and phenol oxidation. The transformation efficiency of both pollutants gradually increases with the decrease of pH, and the optimum pH is 3.0 in this series of experiments. Fe2+, Fe3+, Mn2+ all inhibit hexavalent chromium reduction and phenol degradation to some extent, but Al3+ has little influence on the treatment. In this synergistic reaction system, oxygen is necessary in generating the free radicals, such as hydroxyl radical and sulfate radical. Sulfate radical plays a major role in degrading phenol. This study can provide a basis for remediation of composite wastewater contamination, as a realization of synergistic and green wastewater treatment.
引文
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[15]JIANG Bo,LIU Yukun,ZHENG Jingtang,et al.Synergetic transformations of multiple pollutants driven by Cr(VI)-sulfite reactions[J].Environmental Science&Technology,2015,49:12363-12371.
[16]VOLPE A,PAGANO M,MASCOLO G,et al.Simultaneous Cr(VI)reduction and non-ionic surfactant oxidation by peroxymonosulphate and iron powder[J].Chemosphere,2013,91:1250-1256.
[17]NETA P,HUIE R E,ROSS A B.Rate constants for reactions of inorganic radicals in aqueous solution[J].Journal of Physical and Chemical Reference Data,1988,17(3):1027-1284.
[18]BUXTON G V,GREENSTOCK C L,HELMAN W P,et al.Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms,and hydroxyl radicals(·OH/O·-in aqueous solution[J].Journal of Physical and Chemical Reference Data,1988,17(2):513-886.
[19]HAIGHT G P,PERCHONOCK E,EMMENEGGER F,et al.The mechanism of the oxidation of sulfur(IV)by chromium in acid solution[J].Journal of the American Chemical Society,1965,87:3835-3840.
[20]ZHANG Wensheng,SINGH P,MUIR P,et al.Iron(II)oxidation by SO2/O2 in acidic media:part I.kinetics and mechanism[J].Hydrometallurgy,2000,55:229-245.
[2]孙洪良.复合改性膨润土对水中有机物和重金属的协同吸附研究[D].杭州:浙江大学环境与资源学院,2010:95-119.SUN Hongliang.Study on simultaneous sorption of organic pollutants and heavy metals to bentonite modified by surfactant and organic ligands from water[D].Hangzhou:Zhejiang University.College of Environment and Resources,2010:95-119.
[3]潘翠.混合细菌群体对六价铬和苯酚的同时去除[D].长沙:湖南大学环境科学与工程学院,2008:1-62.PAN Cui.Simultaneous removal of Cr(VI)and phenol in a consortium bacterial culture[D].Changsha:Hunan University.College of Environmental Science and Engineering,2008:1-62.
[4]段国凤.粘质沙雷氏菌去除水中Cr(VI)-邻二氯苯复合污染的研究[D].长沙:湖南大学环境科学与工程学院,2014:1-69.DUAN Guofeng.A research on the Removal of combined contamination of Cr(VI)and o-dichlorobenzene in water by S.marcescens ZD0559[D].Changsha:Hunan University.College of Environmental Science and Engineering,2014:1-69.
[5]刘作华,刘仁龙,牟天明,等.微波促进含铬废渣催化H2O2降解甲基橙溶液研究[J].光谱学与光谱分析,2008,1(8):1900-1904.LIU Zuohua,LIU Renlong,MOU Tianming,et al.Degradation of methyl orange solution by microwave-assisted catalysis of H2O2 with chromium residue[J].Spectroscopy and Spectral Analysis,2008,1(8):1900-1904.
[6]刁增辉,徐向荣.一种利用零价铁-过硫酸盐同时去除重金属-有机物复合污染水体的方法:中国,CN105110448A[P].2015-12-02.DIAO Zenghui,XU Xiangrong.A method of using zero valent iron-persulfate to simultaneously remove heavy metal-organic compound polluted water:China,CN105110448A[P].2015-12-02.
[7]BOKARE A D,CHOI W.Chromate-induced activation of hydrogen peroxide for oxidative degradation of aqueous organic pollutants[J].Environmental Science&Technology,2010,44(19):7232-7237.
[8]ZHANG Li,CHEN Long,XIAO Mei,et al.Enhanced decolorization of Orange II solutions by the Fe(II)-sulfite system under xenon lamp irradiation[J].Industrial&Engineering Chemistry Research,2013,52(30):10089-10094.
[9]吉冰冰,肖玫,张琳,等.铁-亚硫酸盐配合物体系氧化处理硫酸厂的含砷废水[J].水处理技术,2014,40(9):52-56.JI Bingbing,XIAO Mei,ZHANG Lin,et al.Oxidation and removal of arsenic-containing wastewater from sulfuric acid factory by iron-sulfite complex system[J].Technology of Water Treatment,2014,40(9):52-56.
[10]范文娟,董红钰,关小红.Cr(VI)/亚硫酸钠体系快速氧化活性蓝4的动力学研究[J].四川环境,2016,35(3):1-7.FAN Wenjuan,DONG Hongyu,GUAN Xiaohong.Rapid oxidation of reactive blue 4 by the Cr(VI)/sulfite system:Kinetics and mechanisms[J].Sichuan Environment,2016,35(3):1-7.
[11]GB 7467-87,水质·六价铬的测定·二苯碳酰二肼分光光度法[S].GB 7467-87,Water quality-determination of chromium(VI)-1,5 diphenylcarbohydrazide spectrophotometric method[S].
[12]HJ 503-2009,水质·挥发酚的测定·4-氨基安替比林分光光度法[S].HJ 503-2009,Water quality-determination of volatile phenolic compounds-4-AAP spectrophotometric method[S].
[13]YUAN Yanan,YANG Shaojie,ZHOU Danna,et al.A simple Cr(VI)-S(IV)-O2 system for rapid and simultaneous reduction of Cr(VI)and oxidative degradation of organic pollutants[J].Journal of Hazardous Materials,2016,307:294-301.
[14]CHEN Long,PENG Xinzi,LIU Jihao,et al.Decolorization of dyes in aqueous solution by Fe(II)/sulfite system:replacement of persulfate[J].Industrial&Engineering Chemistry Research,2012,51:13632-13638.
[15]JIANG Bo,LIU Yukun,ZHENG Jingtang,et al.Synergetic transformations of multiple pollutants driven by Cr(VI)-sulfite reactions[J].Environmental Science&Technology,2015,49:12363-12371.
[16]VOLPE A,PAGANO M,MASCOLO G,et al.Simultaneous Cr(VI)reduction and non-ionic surfactant oxidation by peroxymonosulphate and iron powder[J].Chemosphere,2013,91:1250-1256.
[17]NETA P,HUIE R E,ROSS A B.Rate constants for reactions of inorganic radicals in aqueous solution[J].Journal of Physical and Chemical Reference Data,1988,17(3):1027-1284.
[18]BUXTON G V,GREENSTOCK C L,HELMAN W P,et al.Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms,and hydroxyl radicals(·OH/O·-in aqueous solution[J].Journal of Physical and Chemical Reference Data,1988,17(2):513-886.
[19]HAIGHT G P,PERCHONOCK E,EMMENEGGER F,et al.The mechanism of the oxidation of sulfur(IV)by chromium in acid solution[J].Journal of the American Chemical Society,1965,87:3835-3840.
[20]ZHANG Wensheng,SINGH P,MUIR P,et al.Iron(II)oxidation by SO2/O2 in acidic media:part I.kinetics and mechanism[J].Hydrometallurgy,2000,55:229-245.