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Simultaneous diffusion of cation and anion to access N, S cocoordinated Bi-sites for enhanced CO2 electroreduction

Zhiyuan Wang1, Chun Wang2, Yidong Hu1, Shuai Yang4, Jia Yang1,6, Wenxing Chen5, Huang Zhou1, Fangyao Zhou1, Lingxiao Wang1, Junyi Du1, Yafei Li2 (✉), and Yuen Wu1,3 (✉)

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1 School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China
2 Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China
3 Dalian National Laboratory for Clean Energy, Dalian 116023, China
4 Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201210, China
5 Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
6 Institutes of Physical Science and Information Technology, Key Laboratory of Structure and Functional Regulation of Hybrid Materials, Ministry of Education, Anhui Graphene Engineering Laboratory, Anhui University, Hefei 230601, China

Keywords: S, N-co-doped carbon nanotube, single bismuth sites, electronic structure modulation, electrochemical CO2 reduction
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Developing highly active single-atom sites catalysts for electrochemical reduction of CO2 is an effective and environmental-friendly strategy to promote carbon-neutral energy cycle and ameliorate global climate issues. Herein, we develop an atomically dispersed N, S co-coordinated bismuth atom sites catalyst (Bi-SAs-NS/C) via a cation and anion simultaneous diffusion strategy for electrocatalytic CO2 reduction. In this strategy, the bonded Bi cation and S anion are simultaneously diffused into the nitrogen-doped carbon layer in the form of Bi2S3. Then Bi is captured by the abundant N-rich vacancies and S is bonded with carbons support at high temperature, formed the N, S co-coordinated Bi sites. Benefiting from the simultaneous diffusion of Bi and S, different electronegative N and S can be effectively co-coordinated with Bi, forming the uniform Bi-N3S/C sites. The synthesized Bi-SAs-NS/C exhibits a high selectivity towards CO with over 88% Faradaic efficiency in a wide potential range, and achieves a maximum FECO of 98.3% at −0.8 V vs. RHE with a current density of 10.24 mA·cm−2, which can keep constant with negligible degradation in 24 h continuous electrolysis. Experimental results and theoretical calculations reveal that the significantly improved catalytic performance of Bi-SAs-NS/C than Bi-SAs-N/C is ascribed to the replacement of one coordinated-N with low electronegative S in Bi-N4C center, which can greatly reduce the energy barrier of the intermediate formation in rate-limiting step and increase the reaction kinetics. This work provides an effective strategy for rationally designing highly active single-atom sites catalysts for efficient electrocatalysis with optimized electronic structure.
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Simultaneous diffusion of cation and anion to access N, S cocoordinated Bi-sites for enhanced CO2 electroreduction. Nano Res.

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