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首页> 外文期刊>Environmental Science & Technology >Electrochemical Oxidation of N-Nitrosodimethylamine with Boron-doped Diamond Film Electrodes
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Electrochemical Oxidation of N-Nitrosodimethylamine with Boron-doped Diamond Film Electrodes

机译：掺硼金刚石薄膜电极对N-亚硝基二甲胺的电化学氧化

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摘要

This research investigated NDMA oxidation by boron-doped diamond (BDD) film electrodes. Oxidation rates were measured as a function of electrode potential, current density, and temperature using rotating disk and flow-through reactors. Final NOMA reaction products were carbon dioxide, ammonium, and nitrate, with dimethylamine and methylamine as intermediate products. Reaction rates were first-order with respect to NDMA concentration and surface area normalized oxidation rates as high as 850 ± 50 L/m~2-hr were observed at a current density of 10 mA/cm~2. The flow-through reactor yielded mass transfer limited reaction rates that were first-order in NDMA concentration, with a half-life of 2.1 ±0.1 min. Experimental evidence indicates that NDMA oxidation proceeds via a direct electron transfer at potentials >1.8 V/SHEwith a measured apparent activation energy of 3.1 ± 0.5 kJ/mol at a potential of 2.5 V/SHE. Density functional theory calculations indicate that a direct two-electron transfer can produce a stable NDMA~((+2)) species that is stabilized by forming an adduct with water. The transfer of two electrons from NDMA to the electrode allows an activation-less attack of hydroxyl radicals on the NDMA~((+2)) water adduct At higher overpotentials the oxidation of NDMA occurs by a combination of direct electron transfer and hydroxyl radicals produced via water electrolysis.
机译：这项研究研究了掺硼金刚石（BDD）薄膜电极对NDMA的氧化作用。使用旋转盘式反应器和流通式反应器测量氧化速率与电极电位，电流密度和温度的关系。最终的NOMA反应产物为二氧化碳，铵盐和硝酸盐，中间产物为二甲胺和甲胺。反应速率相对于NDMA浓度是一阶的，在10 mA / cm〜2的电流密度下，表面积归一化的氧化速率高达850±50 L / m〜2-hr。流通式反应器产生的传质受限反应速率在NDMA浓度中为一级，半衰期为2.1±0.1分钟。实验证据表明，NDMA氧化是通过在> 1.8 V / SHE的电势下通过直接电子转移进行的，在2.5 V / SHE的电势下测得的表观活化能为3.1±0.5 kJ / mol。密度泛函理论计算表明，直接的两电子转移可产生稳定的NDMA〜（（+ 2））物种，该物种通过与水形成加合物而得以稳定。两个电子从NDMA到电极的转移使NDMA〜（（+ 2））水加合物上的羟基自由基受到较少活化的攻击。在较高的超电势下，NDMA的氧化是通过直接电子转移和产生的羟基自由基的结合而发生的通过水电解。

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  • 来源
    《Environmental Science & Technology》 |2009年第21期|8302-8307|共6页
  • 作者

    BRIAN P. CHAPLIN; GLENN SCHRADER; JAMES FARRELL;

  • 作者单位

    Department of Chemical and Environmental Engineering, University of Arizona, Tucson, Arizona 85721;

    Department of Chemical and Environmental Engineering, University of Arizona, Tucson, Arizona 85721;

    Department of Chemical and Environmental Engineering, University of Arizona, Tucson, Arizona 85721;

  • 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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