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; Huilong Fei

doi:10.1038/s41467-023-36078-y

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

Nat Commun. 2023 Jan 23;14(1):368. doi: 10.1038/s41467-023-36078-y.

Authors

Minmin Yan^#¹, Zengxi Wei^#², Zhichao Gong¹, Bernt Johannessen³, Gonglan Ye⁴, Guanchao He¹, Jingjing Liu¹, Shuangliang Zhao⁵, Chunyu Cui⁶, Huilong Fei^{7

8}

Affiliations

¹ State Key Laboratory for Chemo/Biosensing and Chemometrics, and College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China.
² Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology and School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, China.
³ Australian Synchrotron, Clayton, Victoria, 3168, Australia.
⁴ State Key Laboratory for Chemo/Biosensing and Chemometrics, and College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China. glye@hnu.edu.cn.
⁵ Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology and School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, China. szhao@gxu.edu.cn.
⁶ State Key Laboratory for Chemo/Biosensing and Chemometrics, and College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China. cycui@hnu.edu.cn.
⁷ State Key Laboratory for Chemo/Biosensing and Chemometrics, and College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China. hlfei@hnu.edu.cn.
⁸ Advanced Catalytic Engineering Research Center of the Ministry of Education, Hunan University, Changsha, 410082, China. hlfei@hnu.edu.cn.

^# Contributed equally.

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 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-N₄ moieties.

Abstract

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