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Research Article

Asymmetrically coordinated main group atomic In-S1N3 interface sites for promoting electrochemical CO2 reduction

Yan Gao1( )Jinlong Ge1Jingqiao Zhang2,3Ting Cao2,3Zhiyi Sun5Wensheng Yan6Yu Wang7Jie Lin4( )Wenxing Chen5Zheng Liu2,3( )
Anhui Provincial Engineering Laboratory of Silicon-based Materials, Bengbu University, Bengbu 233030, China
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
SEPA Key Laboratory of Eco-Industry, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Science, Ningbo 315201, China
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai 201204, China
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Graphical Abstract

Outstandingly, the engineered In-S1N3 demonstrated a maximum formate Faradaic efficiency (FEHCOO) of 94.3% at −0.8 V vs. reversible hydrogen electrode (RHE), exceeding the In-S2N2 and In-N4 catalysts. Furthermore, at a potential of −1.10 V vs. RHE, In-S1N3 achieves an impressive FE of 93.7% in flow cell. In-situ X-ray absorption fine structure (XAFS) and density functional theory (DFT) reveal the boosted catalytic performance of In-S1N3 sites. The contributions of In-S1N3 interfaces are deeply analysed by DFT calculations.

Abstract

Designing catalysts with highly active, selectivity, and stability for electrocatalytic CO2 to formate is currently a severe challenge. Herein, we developed an electronic structure engineering on carbon nano frameworks embedded with nitrogen and sulfur asymmetrically dual-coordinated indium active sites toward the efficient electrocatalytic CO2 reduction reaction. As expected, atomically dispersed In-based catalysts with In-S1N3 atomic interface with asymmetrically coordinated exhibited high efficiency for CO2 reduction reaction (CO2RR) to formate. It achieved a maximum Faradaic efficiency (FE) of 94.3% towards formate generation at −0.8 V vs. reversible hydrogen electrode (RHE), outperforming that of catalysts with In-S2N2 and In-N4 atomic interface. And at a potential of −1.10 V vs. RHE, In-S1N3 achieves an impressive Faradaic efficiency of 93.7% in flow cell. The catalytic performance of In-S1N3 sites was confirmed to be enhanced through in-situ X-ray absorption near-edge structure (XANES) measurements under electrochemical conditions. Our discovery provides the guidance for performance regulation of main group metal catalysts toward CO2RR at atomic scale.

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Nano Research
Pages 5011-5021
Cite this article:
Gao Y, Ge J, Zhang J, et al. Asymmetrically coordinated main group atomic In-S1N3 interface sites for promoting electrochemical CO2 reduction. Nano Research, 2024, 17(6): 5011-5021. https://doi.org/10.1007/s12274-024-6513-9
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Received: 29 November 2023
Revised: 20 January 2024
Accepted: 23 January 2024
Published: 07 March 2024
© Tsinghua University Press 2024
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