异相草酸铁光降解五氯酚过程中的铁物种分配

兰青, 叶志钧, 陈熠熠, 张艳林. 异相草酸铁光降解五氯酚过程中的铁物种分配[J]. 环境化学, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506
引用本文: 兰青, 叶志钧, 陈熠熠, 张艳林. 异相草酸铁光降解五氯酚过程中的铁物种分配[J]. 环境化学, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506
LAN Qing, YE Zhijun, CHEN Yiyi, ZHANG Yanlin. Distribution of Fe species during the photodegradation of pentachlorophenol in heterogeneous Fe-oxalate system[J]. Environmental Chemistry, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506
Citation: LAN Qing, YE Zhijun, CHEN Yiyi, ZHANG Yanlin. Distribution of Fe species during the photodegradation of pentachlorophenol in heterogeneous Fe-oxalate system[J]. Environmental Chemistry, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506

异相草酸铁光降解五氯酚过程中的铁物种分配

  • 基金项目:

    国家自然科学基金(41201503),高等学校博士学科点专项科研基金(20110171120025),广东环境保护工程职业学院院长基金(KY201301003),广东省高等职业教育品牌专业建设项目(2016gzpp036),广东省环保专项资金,广东省高等学校优秀青年教师培养计划(YQ2015203)资助.

Distribution of Fe species during the photodegradation of pentachlorophenol in heterogeneous Fe-oxalate system

  • Fund Project: Supported by the National Natural Science Foundation of China (41201503), Research Fund for the Doctoral Program of Higher Education(20110171120025), Foundation of President of Guangdong Polytechnic of Environmental Protection Engineering (KY201301003), Guangdong Province Higher Vocational Education Brand Specialty Construction Project (2016gzpp036), Guangdong Province Special Fund For Environmental Protection and the Outstanding Young Teacher Training Program for Higher Education of Guangdong Province (YQ2015203).
  • 摘要: 草酸铁光化学体系在自然界中广泛存在,此体系可以内源生成过氧化氢,构成Fenton体系,产生羟基自由基(·OH),用于降解有机污染物.通过测定赤铁矿(α-Fe2O3)和针铁矿(α-FeOOH)两种铁氧化物-草酸体系在光降解五氯酚(PCP)过程中草酸和pH的变化,计算反应过程中各种Fe(Ⅲ)和Fe(Ⅱ)物种的分配情况,分析影响体系活性的关键因素.研究表明,体系中的铁物种分配和pH通过影响体系的铁循环直接影响体系的反应活性.相同初始pH,不同草酸初始浓度下,高活性的Fe(Ⅱ)物种分配具有较大差异从而影响体系的铁循环速率和反应活性.不同初始pH,达到饱和吸附的相同草酸初始浓度下,高活性的Fe(Ⅱ)和Fe(Ⅲ)物种均为体系控制物种,而pH通过影响Fe(Ⅲ)的还原速率从而影响体系的铁循环速率和反应活性.
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    [2] ZUO Y, HOIGNE J. Formation of hydrogen peroxide and depletion of oxalic acid in atmospheric water by photolysis of iron(Ⅲ)-oxalato complexes[J]. Environmental Science & Technology, 1992, 26(5):1014-1022.
    [3] JEONG J, YOON J. Dual roles of CO2 for degrading synthetic organic chemicals in the photo/ferrioxalate system[J]. Water Research, 2004, 38(16):3531-3540.
    [4] LEE W, BATCHELOR B. Reductive capacity of natural reductants[J]. Environmental Science & Technology, 2003, 37(3):535-541.
    [5] JEONG J S, YOON J Y. pH effect on OH radical production in photo/ferrioxalate system[J]. Water Res, 2005, 39(13):2893-2900.
    [6] BALMER M E, SULZBERGER B. Atrazine degradation in irradiated iron/oxalate systems:Effects of pH and oxalate[J]. Environmental Science & Technology, 1999, 33(14):2418-2424.
    [7] MAZELLIER P, SULZBERGER B. Diuron degradation in irradiated heterogeneous iron/oxalate systems the rate-determining step[J]. Environmental Science & Technology, 2001, 35(16):3314-3320.
    [8] FAUST B C, ZEPP R G. Photochemistry of aqueous iron(Ⅲ)-polycarboxylate complexes:roles in the chemistry of atmospheric and surface waters[J]. Environmental Science & Technology, 1993, 27(12):2517-2522.
    [9] PANIAS D, TAXIARCHOU M, PASPALIARIS I, et al. Mechanisms of dissolution of iron oxides in aqueous oxalic acid solutions[J]. Hydrometallurgy, 1996, 42(2):257-265.
    [10] LAN Q, LIU H, LI F B, et al. Effect of pH on pentachlorophenol degradation in irradiated iron/oxalate systems[J]. Chemical Engineering Journal, 2011, 168(3):1209-1216.
    [11] LAN Q, LI F B, LIU C S, et al. Heterogeneous photodegradation of pentachlorophenol with maghemite and oxalate under UV illumination[J]. Environmental Science & Technology, 2008, 42(21):7918-7923.
    [12] LAN Q, LI F B, SUN C X, et al. Heterogeneous photodegradation of pentachlorophenol and iron cycling with goethite, hematite and oxalate under UVA illumination[J]. Journal of Hazardous Materials, 2010, 174(1/3):64-70.
    [13] LI F B, LI X Z, LI X M, et al. Heterogeneous photodegradation of bisphenol A with iron oxides and oxalate in aqueous solution[J]. Journal of Colloid and Interface Science, 2007, 311:481-490.
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出版历程
  • 收稿日期:  2016-04-05
  • 刊出日期:  2017-02-15
兰青, 叶志钧, 陈熠熠, 张艳林. 异相草酸铁光降解五氯酚过程中的铁物种分配[J]. 环境化学, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506
引用本文: 兰青, 叶志钧, 陈熠熠, 张艳林. 异相草酸铁光降解五氯酚过程中的铁物种分配[J]. 环境化学, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506
LAN Qing, YE Zhijun, CHEN Yiyi, ZHANG Yanlin. Distribution of Fe species during the photodegradation of pentachlorophenol in heterogeneous Fe-oxalate system[J]. Environmental Chemistry, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506
Citation: LAN Qing, YE Zhijun, CHEN Yiyi, ZHANG Yanlin. Distribution of Fe species during the photodegradation of pentachlorophenol in heterogeneous Fe-oxalate system[J]. Environmental Chemistry, 2017, 36(2): 336-344. doi: 10.7524/j.issn.0254-6108.2017.02.2016040506

异相草酸铁光降解五氯酚过程中的铁物种分配

  • 1.  广东环境保护工程职业学院环境监测系, 佛山, 528216;
  • 2.  广东环境保护工程职业学院, 广东省固体废弃物资源化与重金属污染控制工程技术研究中心, 佛山, 528216;
  • 3.  中山大学化学与化学工程学院, 广州, 510275
基金项目:

国家自然科学基金(41201503),高等学校博士学科点专项科研基金(20110171120025),广东环境保护工程职业学院院长基金(KY201301003),广东省高等职业教育品牌专业建设项目(2016gzpp036),广东省环保专项资金,广东省高等学校优秀青年教师培养计划(YQ2015203)资助.

摘要: 草酸铁光化学体系在自然界中广泛存在,此体系可以内源生成过氧化氢,构成Fenton体系,产生羟基自由基(·OH),用于降解有机污染物.通过测定赤铁矿(α-Fe2O3)和针铁矿(α-FeOOH)两种铁氧化物-草酸体系在光降解五氯酚(PCP)过程中草酸和pH的变化,计算反应过程中各种Fe(Ⅲ)和Fe(Ⅱ)物种的分配情况,分析影响体系活性的关键因素.研究表明,体系中的铁物种分配和pH通过影响体系的铁循环直接影响体系的反应活性.相同初始pH,不同草酸初始浓度下,高活性的Fe(Ⅱ)物种分配具有较大差异从而影响体系的铁循环速率和反应活性.不同初始pH,达到饱和吸附的相同草酸初始浓度下,高活性的Fe(Ⅱ)和Fe(Ⅲ)物种均为体系控制物种,而pH通过影响Fe(Ⅲ)的还原速率从而影响体系的铁循环速率和反应活性.

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