Producing hydrogen peroxide (H₂O₂) via a two-electron oxygen reduction reaction (2 e⁻-ORR) is a promising alternative to the conventional anthraquinone process, because of its exceptional low-risk and distributed features. The low yield of H₂O₂ on typical electrocatalysts, usually associated with limited and vulnerable catalytically active sites on their surface, has been the major restriction for improving the practical viability of this technology. Herein, we report an ultrafast microwave-based strategy for constructing distant coordination of Co single-atom sites with secondary fluorene heterodopants on carbon nanotubes, which successfully converts the 2 e⁻-ORR active centers from a single Co atom to multiple surrounding carbon atoms, increasing both the quantity and durability of active sites for 2 e⁻-ORR. Consequently, a high H₂O₂ yield of up to 18.6 mol g⁻¹ L⁻¹ has been achieved, accompanied by a Faraday efficiency of 90%. Besides, an accumulative H₂O₂ concentration of 5.2 g L⁻¹ is obtained after 20 h electrocatalysis, showing the material's high stability and feasibility for practical applications. Density functional theory simulations confirm the optimal adsorption of *OOH on these carbon sites, providing very low kinetic barriers for 2 e⁻-ORR. Thus, this work provides a high-performance electrocatalyst for 2 e⁻-ORR, and more importantly strategy for promoting the performance of single-atom catalysts.

中文翻译：

---

修饰 Co 单原子的氟调控碳纳米管用于多位点电催化双电子氧还原

通过双电子氧还原反应 (2 e ⁻ -ORR)生产过氧化氢 (H ₂ O ₂ ) 是一种很有前途的替代传统蒽醌工艺的方法，因为它具有出色的低风险和分布式特征。典型电催化剂上H ₂ O ₂的低产率，通常与其表面上有限且脆弱的催化活性位点相关，一直是提高该技术实际可行性的主要限制。在此，我们报告了一种基于超快微波的策略，用于构建 Co 单原子位点与碳纳米管上的二次芴杂掺杂剂的远距离配位，成功地将 2 e ^--ORR 活性中心从单个 Co 原子到多个周围的碳原子，增加了 2 e ⁻ -ORR 活性位点的数量和耐久性。因此，实现了高达 18.6 mol g ^-1  L ^-1的高 H ₂ O _{2产率，并伴随着 90% 的法拉第效率。}此外，在电催化20 h后， H ₂ O _{2 的}累积浓度为5.2 g L ^{−1 ，表明该材料具有较高的稳定性和实际应用的可行性。}密度泛函理论模拟证实了 *OOH 在这些碳位点上的最佳吸附，为 2 e 提供了非常低的动力学势垒^--ORR。^{因此，这项工作为 2 e -} -ORR提供了一种高性能电催化剂，更重要的是为提高单原子催化剂的性能提供了策略。