零价铝/酸/氧体系H_2O_2积累对降解活性黑5效果的研究
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摘要
研究了铝粉投加量、初始pH、多金属氧酸盐(POM)及Fe~(2+)添加对零价铝/酸/氧体系中H_2O_2浓度的变化和染料降解的影响。研究表明,不同条件下H_2O_2浓度变化呈现出一定规律性。在初始阶段,H_2O_2浓度逐渐上升,达到最大值后开始下降,最终浓度值趋于稳定。增加铝粉的投加量有助于提高零价铝/酸/氧体系中H_2O_2浓度;酸性越强,H_2O_2产生量越多,浓度达到最大值时所用的时间也越短;在实验研究的POM浓度范围内,零价铝/酸/氧体系中H_2O_2浓度随着POM的添加而增大;Fe~(2+)能与H_2O_2发生芬顿反应,产生·OH,因此,零价铝/酸/氧体系中H_2O_2的积累量随着Fe~(2+)浓度的升高而降低,而活性黑5的降解率却随着Fe~(2+)浓度的升高而升高。
Effects of aluminum loading, initial pH value, POM and ferrous ions on the changes of hydrogen peroxide concentration and dye degradation in the zero valent-aluminum/acid//oxygen system were investigated. The study showed that the changes of H_2O_2 concentration presented certain regularity in different experiments. H_2O_2 concentration gradually increased at the initial stage and decreased after it reached a maximum point, finally H_2O_2 concentration tended to be stable. The increase of aluminum loading was helpful to improve H_2O_2 concentration in the zero-valent aluminum/acid/oxygen system.The stronger the acid, the more H_2O_2 generation was, and it required shorter time to reach the maximum concentration; among the study range of POM concentration, H_2O_2 concentration increased with the addition of POM. Fe~(2+)can occur Fenton reaction with H_2O_2 and generated ·OH, therefore, accumulation of H_2O_2 decreased with the increase of Fe2 +concentration while the Reactive Black 5 degradation efficiency increased in the zero valent-aluminum/acid/oxygen system.
Effects of aluminum loading, initial pH value, POM and ferrous ions on the changes of hydrogen peroxide concentration and dye degradation in the zero valent-aluminum/acid//oxygen system were investigated. The study showed that the changes of H_2O_2 concentration presented certain regularity in different experiments. H_2O_2 concentration gradually increased at the initial stage and decreased after it reached a maximum point, finally H_2O_2 concentration tended to be stable. The increase of aluminum loading was helpful to improve H_2O_2 concentration in the zero-valent aluminum/acid/oxygen system.The stronger the acid, the more H_2O_2 generation was, and it required shorter time to reach the maximum concentration; among the study range of POM concentration, H_2O_2 concentration increased with the addition of POM. Fe~(2+)can occur Fenton reaction with H_2O_2 and generated ·OH, therefore, accumulation of H_2O_2 decreased with the increase of Fe2 +concentration while the Reactive Black 5 degradation efficiency increased in the zero valent-aluminum/acid/oxygen system.
引文
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[2]张惠灵,农佳莹,史文霞,等.微波诱导催化剂Cu O/γ-Al2O3处理活性艳蓝的研究[J].环境科学与技术,2010,33(1):159-162.Zhang Huiling,Nong Jiaying,Shi Wenxia,et al.Microwave induced catalyst Cu O/γ-Al2O3for treatment of Reactive Brilliant Blue[J].Environmental Science&Technology,2010,33(1):159-162.(in Chinese)
[3]张宁,邹华,吴倩云.零价铝/酸体系对活性黑染料的降解研究[J].环境工程学报,2014,8(12):5237-5244.Zhang Ning,Zou Hua,Wu Qianyun.Degradation of Reactive Black 5 in zero valent-aluminum acid system[J].Journal of Environmental Engineering,2014,8(12):5237-5244.(in Chinese)
[4]唐孟姣,薛秀玲,赖小丽.Al0-O2体系降解活性黄3RS溶液[J].环境化学,2015,34(7):1350-1355.Tang Mengjiao,Xue Xiuling,Lai Xiaoli.Degradation of Reactive Yellow 3RS by Al0-O2system[J].Environmental Chemistry,2015,34(7):1350-1355.(in Chinese)
[5]Lin K D,Cai J J,Sun J Q,et al.Removal of 2,4-dichlorophenol by aluminum/O2/acid system[J].J Chem Technol Biotechnol,2013,88:2181-2187.
[6]Bokare A D,Choi W.Zero-valent aluminum for oxidative degradation of aqueous organic pollutants[J].Environmental Science&Technology,2009,43(18):7130-7135.
[7]Louit G,Foley S,Cabillic J,et al.The reaction of coumarin with the OH radical revisited:hydroxylation product analysis determined by fluorescence and chromatography[J].Radiation Physics and Chemistry,2005,72:119-124.
[8]Kim M H,Hwang C,Kang S B,et al.Removal of hydrolyzed Reactive Black 5 from aqueous solution using a polyethylenimine-polyvinyl chloride composite fiber[J].Chemical Engineering Journal,2015,280:18-25.
[9]Tunc Q,Tanaci H,Aksu Z.Potential use of cotton plant wastes for the removal of Azo Black B reactive dye[J].Journal of Hazardous Materials,2009,163:187-198.
[10]邱丽娟,陈亮,黄满红,等.3种污泥对活性黑KN-B的生物吸附及降解研究[J].环境工程学报,2010,4(1):96-100.Qiu Lijuan,Chen Liang,Huang Manhong,et al.Study on adsorption and degradation of Reactive Black KN-B by three kinds of sludge[J].Journal of Environmental Engineering,2010,4(1):96-100.(in Chinese)
[11]Kosaka K,Yamda H,Matsui S,et al.Comparison among the methods for hydrogen peroxide measurements to evaluate advanced oxidation processes:application of a epectrophotometric method using copper(Ⅱ)ion and 2,9-dimethyl-1,10-phenanthroline[J].Environmental Science and Technology,1998,32(23):3821-3824.
[12]Zhang H H,Cao B P,Liu W P,et al.Oxidative removal of acetaminophen using ZVAl/H+/air system:efficacy,influencing factors and reaction mechanisms[J].Journal of Environmental Sciences,2012,24(2):314-319.
[13]刘万鹏.酚类化合物降解新方法研究[D].杭州:浙江工业大学,2011.Liu Wanpeng.New Methods for the Degradation of Phenolic Compounds[D].Hangzhou:Zhejiang University of Technology,2011.(in Chinese)
[14]Neumann R,Levin M.Aerobic oxidative dehydrogenations catalyzed by the mixed-addenda heteropolyanion PV2Mo10-O405-s a kinetic and mechanistic study[J].J Am Chem Soc,1992,114:7278-7286.
[15]Lee J,Kim J,Choi W.Oxidation on zero valent iron promoted by polyoxometalate as an electron shuttle[J].Environmental Science and Technology,2007,41(9):3335-3340.
[16]Marcus R A.The theory of electron-transfer reactions.VI.Unified treatment for homogeneous and electrode reactions[J].Journal of Chemical Physics,1965,43:679-691.
[17]Lin C J,Wang S L,Huang P M,et al.Chromate reduction by zero-valent Al metal as catalyzed by polyoxometalate[J].Water Research,2009,43(20):5015-5022.
[18]曹贝佩.零价铝/氧界面活性氧的原位生成及其对水中对乙酰氨基酚的去除作用[D].杭州:浙江工业大学,2012.Cao Beipei.In Situ Generation of Reactive Oxygen Species on the Interface of Zero-valent Aluminum and Oxygen and Its Application to the Removal of Aqueous Acetaminophen[D].Hangzhou:Zhejiang University of Technology,2012.(in Chinese)
[19]杜卫平.(羟基)氧化铁光催化降解有机物的反应机理[D].杭州:浙江大学,2007.Du Weiping.Reaction Mechanism of Photocatalytic Degradation of Organic Dye over Iron(Hygr)Oxides[D].Hangzhou:Zhejiang University,2007.(in Chinese)