过氧化氢
钴
电化学
硅酸盐
沸石
化学
无机化学
催化作用
有机化学
电极
物理化学
作者
Jiong Wang,Guanghua Yu,Yingying Jin,Ye Zhou,Jing Xia,Xiangmin Meng,Guoliang Dai
标识
DOI:10.1002/anie.202506390
摘要
Electrochemical synthesis of hydrogen peroxide (H2O2) via metal-catalyzed two-electron oxygen reduction reaction (2e- ORR) emerges as a sustainable alternative to the traditional anthraquinone method. However, metal catalysts are commonly supported by graphitic carbon that are susceptible to be oxidized by reactive oxygen species generated in ORR and have limited oxygen capacities. Here, we report a silica based electrocatalyst embedding cobalt (Co) sites into silicate-1 (S-1) zeolite, which exhibited exceptional 2e- ORR performance. The aligned microporosity of S-1 zeolite highly isolated Co sites to derive a specific tri-coordination unit of Co(OSi)3 moiety. The nanochannels of S-1 zeolite further provide robust and substantial reaction spaces, where the Co(OSi)3 moiety facilitates O2 chemisorption and holds moderate bonding with *OOH intermediates to reduce the barrier of H2O2 formation. It achieved high Faradaic efficiency over 96% and a steady yield of 11.56 mol gcat-1 h-1 in a gas diffusion electrode setup. This work provides a novel insight into 2e- ORR on Co sites and highlights the potential of zeolite-based materials for electrochemical applications.
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