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Yan, Minmin; Wei, Zengxi; Gong, Zhichao; Johannessen, Bernt; Ye, Gonglan; He, Guanchao; Liu, Jingjing; Zhao, Shuangliang; Cui, Chunyu; Fei, Huilong
Nature communications, 01/2023, Volume: 14, Issue: 1Journal Article
Abstract Selective two-electron (2e − ) oxygen reduction reaction (ORR) offers great opportunities for hydrogen peroxide (H 2 O 2 ) electrosynthesis and its widespread employment depends on identifying cost-effective catalysts with high activity and selectivity. Main-group metal and nitrogen coordinated carbons (M-N-Cs) are promising but remain largely underexplored due to the low metal-atom density and the lack of understanding in the structure-property correlation. Here, we report using a nanoarchitectured Sb 2 S 3 template to synthesize high-density (10.32 wt%) antimony (Sb) single atoms on nitrogen- and sulfur-codoped carbon nanofibers (Sb-NSCF), which exhibits both high selectivity (97.2%) and mass activity (114.9 A g −1 at 0.65 V) toward the 2e − ORR in alkaline electrolyte. Further, when evaluated with a practical flow cell, Sb-NSCF shows a high production rate of 7.46 mol g catalyst −1 h −1 with negligible loss in activity and selectivity in a 75-h continuous electrolysis. Density functional theory calculations demonstrate that the coordination configuration and the S dopants synergistically contribute to the enhanced 2e − ORR activity and selectivity of the Sb-N 4 moieties.
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