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Coordinating the Edge Defects of Bismuth with Sulfur for Enhanced CO2 Electroreduction to Formate |
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| Authors: | Lei Lv Ruihu Lu Jiexin Zhu Ruohan Yu Dr Wei Zhang Enhui Cui Xingbao Chen Yuhang Dai Lianmeng Cui Dr Jiong Li Prof Liang Zhou Prof Wei Chen Dr Ziyun Wang Prof Liqiang Mai |
| Institution: | 1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070 Wuhan, Hubei, P.?R. China
These authors contributed equally to this work.;2. School of Chemical Sciences, The University of Auckland, 1010 Auckland, New Zealand These authors contributed equally to this work.;3. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070 Wuhan, Hubei, P.?R. China;4. Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, P.?R. China;5. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070 Wuhan, Hubei, P.?R. China Hubei Longzhong Laboratory, Wuhan University of Technology (Xiangyang Demonstration Zone), 441000 Xiangyang, Hubei, P.?R. China;6. School of Chemical Sciences, The University of Auckland, 1010 Auckland, New Zealand |
| Abstract: | Bismuth-based materials have been recognized as promising catalysts for the electrocatalytic CO2 reduction reaction (ECO2RR). However, they show poor selectivity due to competing hydrogen evolution reaction (HER). In this study, we have developed an edge defect modulation strategy for Bi by coordinating the edge defects of bismuth (Bi) with sulfur, to promote ECO2RR selectivity and inhibit the competing HER. The prepared catalysts demonstrate excellent product selectivity, with a high HCOO? Faraday efficiency of ≈95 % and an HCOO? partial current of ≈250 mA cm?2 under alkaline electrolytes. Density function theory calculations reveal that sulfur tends to bind to the Bi edge defects, reducing the coordination-unsaturated Bi sites (*H adsorption sites), and regulating the charge states of neighboring Bi sites to improve *OCHO adsorption. This work deepens our understanding of ECO2RR mechanism on bismuth-based catalysts, guiding for the design of advanced ECO2RR catalysts. |
| Keywords: | Carbon Dioxide Reduction Electrocatalysis Electrochemical Reconstruction S-Doping |