The electrochemical two-electron oxygen reduction reaction (2eORR) for producing hydrogen peroxide (H₂O₂) has attracted significant attention as a potential alternative to the traditional anthraquinone process. In this study, we present a convenient method to regulate the electronic state of carbon sites using oxygenated groups, thereby achieving selective electrocatalytic O₂ reduction to H₂O₂. Oxidized Ketjen Black (KB-Ox) exhibits high oxygen content and good hydrophilicity, improving the accessible surface of the electrolyte. This results in excellent H₂O₂ selectivity (87.5% at an applied potential of 0.55 V vs. RHE) and stability (>80% over 8 h of long-term catalytic testing). Additionally, this convenient and mild method is used to enhance the 2eORR performance of graphene carbon (GC-Ox) and Super P (SP-Ox). Density functional theory (DFT) simulations further reveal that the aldehyde group (–CHO) effectively optimizes the electronic state and coordination environment of the carbon active site, leading to suitable bonding strength towards OOH*, ultimately achieving outstanding 2eORR performance. This work significantly guides the rational design and understanding of the catalytic mechanism of the carbon-based catalyst with high 2eORR activity.

中文翻译：

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通过含氧基团对碳位点进行电子调节，实现电化学氧还原成 H2O2


用于生产过氧化氢（H ₂ O ₂ ）的电化学双电子氧还原反应（2eORR）作为传统蒽醌工艺的潜在替代方案引起了人们的广泛关注。在本研究中，我们提出了一种利用含氧基团调节碳位点电子态的便捷方法，从而实现选择性电催化O ₂还原为H ₂ O ₂ 。氧化科琴黑 (KB-Ox) 具有高氧含量和良好的亲水性，改善了电解质的可接触表面。这导致了出色的 H ₂ O ₂选择性（相对于RHE，在施加 0.55 V 电位时为 87.5%）和稳定性（在 8 小时的长期催化测试中>80%）。此外，这种方便温和的方法还用于增强石墨烯碳（GC-Ox）和Super P（SP-Ox）的2eORR性能。密度泛函理论（DFT）模拟进一步表明，醛基（-CHO）有效优化了碳活性位点的电子态和配位环境，从而使OOH*具有合适的键合强度，最终实现了出色的2eORR性能。这项工作对合理设计和理解具有高2eORR活性的碳基催化剂的催化机理具有重要指导意义。