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Removal of Persistent Organic Contaminants by Electrochemically Activated Sulfate

机译：电化学活化的硫酸盐去除持久性有机污染物

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Solutions of sulfate have often been used as background electrolytes in the electrochemical degradation of contaminants and have been generally considered inert even when high-oxidation-power anodes such as boron-doped diamond (BDD) were employed. This study examines the role of sulfate by comparing electro-oxidation rates for seven persistent organic contaminants at BDD anodes in sulfate and inert nitrate anolytes. Sulfate yielded electro-oxidation rates 10-15 times higher for all target contaminants compared to the rates of nitrate anolyte. This electrochemical activation of sulfate was also observed at concentrations as low as 1.6 mM, which is relevant for many wastewaters. Electrolysis of diatrizoate in the presence of specific radical quenchers (tert- butanol and methanol) had a similar effect on electro-oxidation rates, illustrating a possible role of the hydroxyl radical (~•OH) in the anodic formation of sulfate radical (SO_4~(•-)) species. The addition of 0.55 mM persulfate increased the electro-oxidation rate of diatrizoate in nitrate from 0.94 to 9.97 h~(-1), suggesting a nonradical activation of persulfate. Overall findings indicate the formation of strong sulfate-derived oxidant species at BDD anodes when polarized at high potentials. This may have positive implications in the electro-oxidation of wastewaters containing sulfate. For example, the energy required for the 10-fold removal of diatrizoate was decreased from 45.6 to 2.44 kWh m~(-3) by switching from nitrate to sulfate anolyte.
机译：硫酸盐溶液在污染物的电化学降解中经常被用作背景电解质，即使使用高氧化能力的阳极（例如掺硼金刚石（BDD）），也通常被认为是惰性的。这项研究通过比较硫酸盐和惰性硝酸盐阳极液中BDD阳极处的7种持久性有机污染物的电氧化速率，研究了硫酸盐的作用。与硝酸盐阳极电解液的比率相比，所有目标污染物的硫酸盐产生的电氧化比率高10-15倍。在低至1.6 mM的浓度下也观察到硫酸盐的这种电化学活化，这与许多废水有关。在特定的自由基猝灭剂（叔丁醇和甲醇）存在下，泛影酸盐的电解对电氧化速率具有相似的影响，这说明了羟基自由基（〜•OH）在硫酸根（SO_4〜）的阳极形成中的可能作用。 （•-））物种。 0.55 mM过硫酸盐的添加将泛影酸盐在硝酸盐中的电氧化速率从0.94 h增至9.97 h〜（-1），表明过硫酸盐的非自由基活化。总体发现表明，当在高电势下极化时，在BDD阳极上会形成强硫酸盐衍生的氧化剂。这可能会对含硫酸盐废水的电氧化产生积极影响。例如，通过从硝酸盐转换为硫酸盐阳极电解液，将十倍数次泛影酸盐去除所需的能量从45.6 kWh m·（-3）降低到2.44 kWh m〜（-3）。

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  • 来源
    《Environmental Science & Technology》 |2015年第24期|14326-14333|共8页
  • 作者

    Ali Farhat; Jurg Keller; Stephan Tait; Jelena Radjenovic;

  • 作者单位

    Advanced Water Management Centre, The University of Queensland, Brisbane, Queensland 4072, Australia;

    Advanced Water Management Centre, The University of Queensland, Brisbane, Queensland 4072, Australia;

    Advanced Water Management Centre, The University of Queensland, Brisbane, Queensland 4072, Australia;

    Advanced Water Management Centre, The University of Queensland, Brisbane, Queensland 4072, Australia,Catalan Institute for Water Research (ICRA), Scientific and Technological Park of the University of Girona, 17003 Girona, Spain;

  • 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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