氧化剂
电催化剂
过氧化氢
共价键
电化学
法拉第效率
化学
密度泛函理论
三嗪
电极
计算化学
高分子化学
有机化学
物理化学
作者
Rahmat Ullah Khan,Jeet Chakraborty,Kuber Singh Rawat,Rino Morent,Nathalie De Geyter,Véronique Van Speybroeck,Pascal Van Der Voort
标识
DOI:10.1002/anie.202313836
摘要
Electrochemical two-electron water oxidation (2e WOR) is gaining surging research traction for sustainable hydrogen peroxide production. However, the strong oxidizing environment and thermodynamically competitive side-reaction (4e WOR) posit as thresholds for the 2e WOR. We herein report a custom-crafted covalent triazine network possessing strong oxidizing properties as a proof-of-concept metal-free functional organic network electrocatalyst for catalyzing 2e WOR. As the first-of-its-kind, the material shows a maximum of 89.9 % Faradaic Efficiency and 1428 μmol/h/cm2 H2 O2 production rate at 3.0 V bias potential (vs reversible hydrogen electrode, RHE), which are either better or comparable to the state-of-the-art electrocatalysts. We have experimentally confirmed a stepwise 2e WOR mechanism which was further computationally endorsed by density functional theory studies.
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