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Electrochemical Transformation of Trace Organic Contaminants in the Presence of Halide and Carbonate Ions

机译:卤化物和碳酸盐离子存在下痕量有机污染物的电化学转化

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摘要

Electrochemical treatment on anodes shows promise for the oxidation of organic contaminants in industrial wastewater and reverse osmosis concentrate from municipal wastewater recycling due to the high conductivity of the matrix and the concomitant low energy demand. The effect of background electrolyte composition (Cl~-, HCO_3~-, and NH_4~+) on the formation and fate of electrochemically produced heterogeneous (HO~._(ads) and Cl~._(ads)) and homogeneous (HOCl and HOBr) oxidants was evaluated on Ti-IrO_2 and boron-doped diamond (BDD) electrodes using a suite of trace organic contaminants that exhibited varying reactivity with HO~., CO_3~(.-), HOCl, and HOBr. The contributions of adsorbed and bulk oxidants to contaminant degradation were investigated. Results show that transformation rates for most contaminants increased in the presence of chloride and trace amounts of bromide; however, elevated concentrations of HCO_3~- often altered transformation rates due to formation of selective oxidants, with decreases in reactivity observed for electron-poor contaminants and increases in reactivity observed for compounds with amine and phenolic moieties. Using this information, rates of reactions on anode surfaces and measured production and loss rates for reactive homogeneous species were used to predict contaminant removal in municipal wastewater effluent. Despite some uncertainty in the reaction mechanisms, the model accurately predicted rates of removal of electron-rich contaminants but underestimated the transformation rates of compounds that exhibited low reactivity with HOCl and HOBr, possibry due to the formation of halogen radicals. The approach employed in mis study provides a means of identifying key reactions for different classes of contaminants and for predicting the conditions under which anodic treatment of wastewater will be practical.
机译:阳极上的电化学处理显示出有望将工业废水中的有机污染物氧化,以及由于基质的高电导率和随之而来的低能源需求,使市政废水回收产生的反渗透浓缩物。背景电解质成分(Cl〜-,HCO_3〜-和NH_4〜+)对电化学生成的多相(HO〜._(ads)和Cl〜._(ads))和均相(HOCl)的形成和命运的影响在Ti-IrO_2和硼掺杂的金刚石(BDD)电极上使用一系列痕量有机污染物(与HO〜,CO_3〜(-),HOCl和HOBr具有不同的反应性)对氧化剂和HOBr)进行了评估。研究了吸附氧化剂和本体氧化剂对污染物降解的贡献。结果表明,在存在氯化物和痕量溴化物的情况下,大多数污染物的转化率都会增加;然而,高浓度的HCO 3-经常由于形成选择性氧化剂而改变转化率,对于电子贫乏的污染物观察到反应性降低,而对于具有胺和酚部分的化合物则观察到反应性增加。利用这些信息,阳极表面上的反应速率以及反应性均质物质的测得产率和损失率可用于预测市政废水中污染物的去除。尽管反应机理存在一些不确定性,该模型仍能准确预测富电子污染物去除的速率,但低估了由于形成卤素自由基而与HOCl和HOBr发生低反应性的化合物的转化率。错误研究中使用的方法提供了一种方法,该方法可以识别针对不同类别污染物的关键反应,并预测对废水进行阳极处理的实际条件。

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  • 来源
    《Environmental Science & Technology》 |2016年第18期|10143-10152|共10页
  • 作者单位

    Department of Civil and Environmental, Engineering University of California, Berkeley, California 94720, United States;

    Department of Civil and Environmental, Engineering University of California, Berkeley, California 94720, United States;

    Department of Civil and Environmental, Engineering University of California, Berkeley, California 94720, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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