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Enhancing H 2 O 2 Electrosynthesis at Industrial-Relevant Current in Acidic Media on Diatomic Cobalt Sites.

Helai HuangMingze SunShuwei LiShengbo ZhangYiyang LeeZhengwen LiJinjie FangChengjin ChenYu-Xiao ZhangYanfen WuYizhen CheShuairen QianWei ZhuCheng TangZhongbin ZhuangLiang ZhangZhiqiang Niu
Published in: Journal of the American Chemical Society (2024)
Electrocatalytic synthesis of hydrogen peroxide (H 2 O 2 ) in acidic media is an efficient and eco-friendly approach to produce inherently stable H 2 O 2 , but limited by the lack of selective and stable catalysts under industrial-relevant current densities. Herein, we report a diatomic cobalt catalyst for two-electron oxygen reduction to efficiently produce H 2 O 2 at 50-400 mA cm -2 in acid. Electrode kinetics study shows a >95% selectivity for two-electron oxygen reduction on the diatomic cobalt sites. In a flow cell device, a record-high production rate of 11.72 mol g cat -1 h -1 and exceptional long-term stability (100 h) are realized under high current densities. In situ spectroscopic studies and theoretical calculations reveal that introducing a second metal into the coordination sphere of the cobalt site can optimize the binding strength of key H 2 O 2 intermediates due to the downshifted d-band center of cobalt. We also demonstrate the feasibility of processing municipal plastic wastes through decentralized H 2 O 2 production.
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