pH-Independent Production of Hydroxyl Radical from Atomic H*-Mediated Electrocatalytic H2O2 Reduction: A Green Fenton Process without Byproducts

Huabin  Zeng; Gong  Zhang; Qinghua  JiHuijuan  LiuXin  HuaHailun  XiaMika  SillanpääJiuhui  Qu

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pH-Independent Production of Hydroxyl Radical from Atomic H*-Mediated Electrocatalytic H2O2 Reduction: A Green Fenton Process without Byproducts

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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_(2)O_(2)), narrow applicable pH range, strict activator/H_(2)O_(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_(2)O_(2) into ~(•)OH and subsequent degradation of organic pollutants (80 efficiency). Operando liquid time-of-fight secondary ion mass spectrometry verified that H_(2)O_(2) activation takes place through a transition state of the Pd–H*–H_(2)O_(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_(2)O as products (ΔG _(r) = −1.344 eV). Using H~(+) or H_(2)O 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.

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《Environmental Science & Technology: ES&T》 |2020年第22期|14725-14731|共7页
作者
Huabin Zeng; Gong Zhang; Qinghua JiHuijuan LiuXin HuaHailun XiaMika SillanpääJiuhui Qu;
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作者单位

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

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

Department of Civil and Environmental Engineering, Florida International University;

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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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正文语种英语
中图分类环境科学、安全科学;
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pH-Independent Production of Hydroxyl Radical from Atomic H*-Mediated Electrocatalytic H2O2 Reduction: A Green Fenton Process without Byproducts

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