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首页> 外文期刊>Environmental Science & Technology >pH-lndependent Production of Hydroxyl Radical from Atomic H*-Mediated Electrocatalytic H_2O_2 Reduction: A Green Fenton Process without Byproducts
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pH-lndependent Production of Hydroxyl Radical from Atomic H*-Mediated Electrocatalytic H_2O_2 Reduction: A Green Fenton Process without Byproducts

机译：从原子H *介导的电催化H_2O_2减少的PH-LNDENVENDENT生产的羟基羟基羟基α0_2：没有副产品的绿色芬顿工艺

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摘要

Hydroxyl radical (•~OH) can hydroxylate or dehydrogenate organics without forming extra products and is thereby expediently applied in extensive domains. Although it can be efficiently produced through single-electron transfer from transition-metal-containing activators to hydrogen peroxide (H_2O_2), narrow applicable pH range, strict acnvator/H_2O_2 ratio requirement, and byproducts that are formed in the mixture with the background matrix necessitate the need for additional energy-intensive up/ downstream treatments. Here, we show a green Fenton process in an electrochemical cell, where the electro-generated atomic H* on a Pd/graphite cathode enables the efficient conversion of H_2O_2 into •~OH and subsequent degradation of organic pollutants (80% efficiency). Operando liquid time-of-fight secondary ion mass spectrometry verified that H_2O_2 activation takes place through a transition state of the Pd-H*-H_2O_2 adduct with a low reaction energy barrier of 0.92 eV, whereby the lone electron in atomic H* can readily cleave the peroxide bridge, with •OH and H_2O as products (△G_r = -1.344 eV). Using H~+ or H_2O as the resource, we demonstrate that the well-directed output of H* determines the pH-independent production of •~OH for stable conversion of organic contaminants in wider pH ranges (3-12). The research pioneers a novel path for eliminating the restrictions that are historically challenging in the traditional Fenton process.
机译：羟基自由基（•〜OH）可以羟基化物或脱氢有机物而不形成额外的产品，从而有利地应用于广泛的结构域。尽管可以通过从含过渡金属的活化剂到过氧化氢（H_2O_2），窄的适用的pH范围，严格的ACNVATOR / H_2O_2比率要求，以及在混合物中形成的副产物，与背景基质的副产品有效地生产。需要额外的能量沉重的上游治疗方法。在这里，我们在电化学电池中显示绿色芬顿工艺，其中PD /石墨阴极上的电生原子H *能够有效地转化为〜OH和随后的有机污染物的降解（80％效率）。 Operando液体对抗二次离子质谱法验证了H_2O_2激活通过PD-H * -H_2O_2加合物的过渡状态，其低反应能量屏障为0.92eV，由此原子H *中的孤立电子可以容易地切割过氧化物桥，用•OH和H_2O作为产品（△G_R = -1.344eV）。使用H〜+或H_2O作为资源，我们证明了H *的定向输出决定了较宽的pH范围内有机污染物的稳定转化（3-12）的pH-Importy生产。研究开拓了一种消除在传统芬邦工艺历史上挑战性挑战的限制的新型路径。

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  • 来源
    《Environmental Science & Technology》 |2020年第22期|14725-14731|共7页
  • 作者

    Huabin Zeng; Gong Zhang; Qinghua Ji; Huijuan Liu; Xin Hua; Hailun Xia; Mika Sillanpaeae; Jiuhui Qu;

  • 作者单位

    Center for Water and Ecology State Key joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China Department of Separation Science School of Engineering Science Lappeenranta-Lahti University of Technology LUT Mikkeli F1-50130 Finland;

    Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China;

    Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China;

    Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua Universitx Beiiing 100084. China;

    Key Laboratory for Advanced Materials & School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 China;

    Key Laboratory for Advanced Materials & School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai 200237 China;

    Department of Civil and Environmental Engineering Florida International University Miami EL 33199 United States;

    Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution Control School of Environment Tsinghua University Beijing 100084 China;

  • 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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