Sb2S3-templated synthesis of sulfur-doped Sb-N-C with hierarchical architecture and high metal loading for H2O2 electrosynthesis

Minmin Yan, Zengxi Wei, Zhichao Gong, Bernt Johannessen, Gonglan Ye (), Guanchao He, Jingjing Liu, Shuangliang Zhao (), Chunyu Cui () and Huilong Fei ()
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Minmin Yan: Hunan University
Zengxi Wei: Guangxi University
Zhichao Gong: Hunan University
Bernt Johannessen: Australian Synchrotron
Gonglan Ye: Hunan University
Guanchao He: Hunan University
Jingjing Liu: Hunan University
Shuangliang Zhao: Guangxi University
Chunyu Cui: Hunan University
Huilong Fei: Hunan University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Selective two-electron (2e−) oxygen reduction reaction (ORR) offers great opportunities for hydrogen peroxide (H2O2) 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 Sb2S3 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 gcatalyst−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-N4 moieties.

Date: 2023
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DOI: 10.1038/s41467-023-36078-y

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