【摘 要】
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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 dispe
【机 构】
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School of Chemistry and Materials Science,Hefei National Laboratory for Physical Sciences at the Mic
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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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