Unveiling the spatially confined oxidation processes in reactive electrochemical membranes

Yuyang Kang, Zhenao Gu (), Baiwen Ma, Wei Zhang, Jingqiu Sun, Xiaoyang Huang, Chengzhi Hu, Wonyong Choi and Jiuhui Qu ()
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Yuyang Kang: Chinese Academy of Sciences
Zhenao Gu: Chinese Academy of Sciences
Baiwen Ma: Chinese Academy of Sciences
Wei Zhang: Chinese Academy of Sciences
Jingqiu Sun: Chinese Academy of Sciences
Xiaoyang Huang: Korea Institute of Energy Technology (KENTECH)
Chengzhi Hu: Chinese Academy of Sciences
Wonyong Choi: Korea Institute of Energy Technology (KENTECH)
Jiuhui Qu: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Electrocatalytic oxidation offers opportunities for sustainable environmental remediation, but it is often hampered by the slow mass transfer and short lives of electro-generated radicals. Here, we achieve a four times higher kinetic constant (18.9 min−1) for the oxidation of 4-chlorophenol on the reactive electrochemical membrane by reducing the pore size from 105 to 7 μm, with the predominate mechanism shifting from hydroxyl radical oxidation to direct electron transfer. More interestingly, such an enhancement effect is largely dependent on the molecular structure and its sensitivity to the direct electron transfer process. The spatial distributions of reactant and hydroxyl radicals are visualized via multiphysics simulation, revealing the compressed diffusion layer and restricted hydroxyl radical generation in the microchannels. This study demonstrates that both the reaction kinetics and the electron transfer pathway can be effectively regulated by the spatial confinement effect, which sheds light on the design of cost-effective electrochemical platforms for water purification and chemical synthesis.

Date: 2023
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DOI: 10.1038/s41467-023-42224-3

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