Simultaneous diffusion of cation and anion to access N,S cocoordinated Bi-sites for enhanced CO_(2) electroreduction  

作　　者：Zhiyuan Wang Chun Wang Yidong Hu Shuai Yang Jia Yang Wenxing Chen Huang Zhou Fangyao Zhou Lingxiao Wang Junyi Du Yafei Li Yuen Wu 

机构地区：[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

出　　处：《Nano Research》2021年第8期2790-2796,共7页纳米研究（英文版）

基　　金：supported by the National Key R&D Program of China(Nos.2017YFA0208300 and 2017YFA0700104);the National Natural Science Foundation of China(Nos.21522107 and 21671180);the DNL Cooperation Fund,CAS(No.NDL201918).

摘　　要：Developing highly active single-atom sites catalysts for electrochemical reduction of CO_(2) 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 CO_(2) 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-N_(3)S/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 FE_(CO)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-N_(4)C 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.

关 键 词：S N-co-doped carbon nanotube single bismuth sites electronic structure modulation electrochemical CO_(2)reduction 

分 类 号：O64[理学—物理化学]