Abstract Electrocatalytic two-electron oxygen reduction reaction (2e− ORR) is a promising strategy to achieve hydrogen peroxide (H2O2) production, which can replace the anthraquinone method in industrial processes. Nitrogen-doped carbon materials are active and selective electrocatalysts for 2e− ORR; however, it remains challenging to develop N-doped carbons for practical H2O2 production and pinpoint the exact role of nitrogen functionalities. Here, we examine covalent organic framework-derived nitrogen-doped carbons with well-defined porous structure and tunable N species for electrocatalytic H2O2 production. Electrochemical studies show their highest ORR activity and H2O2 selectivity of up to 75% in alkaline electrolyte. Notably, chronoamperometric bulk electrolysis achieves an unprecedented carbon-catalyzed H2O2 yield rate of 1286.9 mmol gcatalyst−1 h−1 and a faradaic efficiency of 69.8% at pH 13. X-ray photoelectron spectroscopy analysis combined with control experiments reveals that graphitic N is responsible for H2O2 production from 2e− ORR on N-doped carbons. Our work provides insights into the rational development of heteroatom-doped carbon electrocatalysts for efficient H2O2 generation.

中文翻译：

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氮掺杂碳中的石墨氮促进电催化氧还原合成过氧化氢

摘要 电催化双电子氧还原反应 (2e- ORR) 是实现过氧化氢 (H2O2) 生产的一种有前景的策略，可替代工业过程中的蒽醌法。氮掺杂碳材料是 2e-ORR 的活性和选择性电催化剂；然而，开发用于实际生产 H2O2 的 N 掺杂碳并确定氮官能团的确切作用仍然具有挑战性。在这里，我们研究了共价有机框架衍生的氮掺杂碳，这些碳具有明确的多孔结构和可调节的 N 物种，用于电催化 H2O2 生产。电化学研究表明，它们在碱性电解质中具有最高的 ORR 活性和高达 75% 的 H2O2 选择性。值得注意的是，计时电流法本体电解实现了前所未有的碳催化 H2O2 产率 1286。9 mmol gcatalyst-1 h-1 和在 pH 13 时法拉第效率为 69.8%。结合对照实验的 X 射线光电子能谱分析表明，石墨 N 负责从 N 掺杂碳上的 2e-ORR 产生 H2O2。我们的工作为合理开发杂原子掺杂的碳电催化剂以高效生成 H2O2 提供了见解。