电合成
锰
催化作用
过氧化氢
化学
氢原子
Atom(片上系统)
无机化学
电化学
有机化学
电极
物理化学
计算机科学
烷基
嵌入式系统
作者
Yuan Zeng,Xin Tan,Zewen Zhuang,Chen Chen,Qing Peng
标识
DOI:10.1002/anie.202416715
摘要
The two‐electron oxygen reduction reaction (2e− ORR) is a pivotal pathway for the distributed production of hydrogen peroxide (H2O2). In nature, enzymes containing manganese (Mn) centers can convert reactive oxygen species into H2O2. However, Mn‐based heterogeneous catalysts for 2e− ORR are scarcely reported. Herein, we developed a nature‐inspired single‐atom electrocatalyst comprising N, O co‐coordinated Mn sites, utilizing carbon dots as the modulation platform (Mn CD/C). As‐synthesized Mn CD/C exhibited exceptional 2e− ORR activity with an onset potential of 0.786 V and a maximum H2O2 selectivity of 95.8%. Impressively, Mn CD/C continuously produced 0.1 M H2O2 solution at 200 mA/cm2 for 50 h in the flow cell, with negligible loss in activity and H2O2 faradaic efficiency, demonstrating practical application potential. The enhanced activity was attributed to the incorporation of Mn atomic sites into the carbon dots. Theoretical calculations revealed that the N, O co‐coordinated structure, combined with abundant oxygen‐containing functional groups on the carbon dots, optimized the binding strength of intermediate *OOH at the Mn sites to the apex of the catalytic activity volcano. This work illustrates that carbon dots can serve as a versatile platform for modulating the microenvironment of single‐atom catalysts and for the rational design of nature‐inspired catalysts.
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