首页> 外文OA文献 >THE USE OF BORON-DOPED DIAMOND FILM ELECTRODES FOR THE OXIDATIVE DEGRADATION OF PERFLUOROOCTANE SULFONATE AND TRICHLOROETHYLENE
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THE USE OF BORON-DOPED DIAMOND FILM ELECTRODES FOR THE OXIDATIVE DEGRADATION OF PERFLUOROOCTANE SULFONATE AND TRICHLOROETHYLENE

机译:掺硼金刚石薄膜电极在全氟辛烷磺酸和三氟甲苯的氧化降解中的应用

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摘要

The current treatment of water contaminated with organic compounds includes adsorption, air stripping, and advanced oxidation processes. These methods large quantities of water and require excessive energy and time. A novel treatment process of concentrating and then electrochemically oxidizing compound would be a more feasible practice. This research investigated the oxidative destruction of perfluorooctane sulfonate (PFOS), perfluorobutane sulfonate (PFBS) and trichloroethene (TCE) at boron-doped diamond film electrodes and the adsorption of PFOS and PFBS on granular activated carbon and ion exchange resins.Experiments measuring oxidation rates of PFOS and PFBS were performed over a range in current densities and temperatures using a rotating disk electrode (RDE) reactor and a parallel plate flow-through reactor. Oxidation of PFOS was rapid and yielded sulfate, fluoride, carbon dioxide and trace levels of trifluoroacetic acid. Oxidation of PFBS was slower than that of PFOS. A comparison of the experimentally measured apparent activation energy with those calculated using Density Functional Theory (DFT) studies indicated that the most likely rate-limiting step for PFOS and PFBS oxidation was direct electron transfer. The costs for treating PFOS and PFBS solutions were compared and showed that PFOS is cheaper to degrade than PFBS.Screening studies were performed to find a viable adsorbent or ion exchange resin for concentrating PFOS or PFBS. Granular activated carbon F400 (GAC-F400) and an ion exchange resin, Amberlite IRA-458, were the best methods for adsorbing PFOS. Ionic strength experiments showed that the solubility of the compounds affected the adsorption onto solid phases. Regeneration experiments were carried out to determine the best method of recovering these compounds from the adsorbents; however, the compounds could not be effectively removed from the adsorbents using standard techniques.The electrochemical oxidation of trichloroethene (TCE) at boron-doped diamond film electrodes was studied to determine if this would be a viable degradation method for chlorinated solvents. Flow-through experiments were performed and showed TCE oxidation to be very rapid. Comparing the data from the DFT studies and the experimentally calculated apparent activation energies the mechanism for TCE oxidation was determined to be controlled by both direct electron transfer and oxidation via hydroxyl radicals.
机译:目前对被有机化合物污染的水的处理包括吸附,空气汽提和高级氧化过程。这些方法需要大量的水,并且需要过多的能量和时间。浓缩然后电化学氧化化合物的新处理方法将是更可行的实践。这项研究研究了硼掺杂金刚石薄膜电极上全氟辛烷磺酸(PFOS),全氟丁烷磺酸(PFBS)和三氯乙烯(TCE)的氧化破坏以及颗粒状活性炭和离子交换树脂上PFOS和PFBS的吸附作用。使用旋转盘电极(RDE)反应器和平行板流通式反应器在一定电流密度和温度范围内进行PFOS和PFBS的制备。 PFOS的氧化迅速,并产生硫酸盐,氟化物,二氧化碳和痕量的三氟乙酸。 PFBS的氧化速度比PFOS慢。实验测量的表观活化能与使用密度泛函理论(DFT)研究计算的表观活化能的比较表明,PFOS和PFBS氧化最可能的速率限制步骤是直接电子转移。比较了全氟辛烷磺酸和全氟辛烷磺酸溶液的处理费用,结果表明全氟辛烷磺酸的降解成本比全氟辛烷磺酸便宜。颗粒状活性炭F400(GAC-F400)和离子交换树脂Amberlite IRA-458是吸附全氟辛烷磺酸的最佳方法。离子强度实验表明,化合物的溶解度影响固相吸附。进行了再生实验,以确定从吸附剂中回收这些化合物的最佳方法。然而,使用标准技术不能有效地从吸附剂中去除这些化合物。研究了在掺硼金刚石薄膜电极上三氯乙烯(TCE)的电化学氧化,以确定这是否是可行的氯化溶剂降解方法。进行了流通实验,结果表明TCE氧化非常迅速。比较来自DFT研究的数据和实验计算的表观活化能,可以确定TCE氧化的机理受直接电子转移和羟基自由基氧化的控制。

著录项

  • 作者

    Carter Kimberly Ellen;

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  • 年度 2009
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  • 原文格式 PDF
  • 正文语种 EN
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