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

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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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Acknowledgements

This work was supported by the Anhui Provincial Department of Education (No. KJ2021A1125), the National Natural Science Foundation of China (No. 12374390), Ningbo 3315 Innovative Teams Program (No. 2019A-14-C), and the member of Youth Innovation Promotion Association Foundation of CAS, China (No. 2023310). The authors thank the BL14W1 in the Shanghai Synchrotron Radiation Facility (SSRF), BL10B and BL12B in the National Synchrotron Radiation Laboratory (NSRL) for help with characterizations.

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Authors and Affiliations

  1. Anhui Provincial Engineering Laboratory of Silicon-based Materials, Bengbu University, Bengbu, 233030, China

    Yan Gao & Jinlong Ge

  2. State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China

    Jingqiao Zhang, Ting Cao & Zheng Liu

  3. SEPA Key Laboratory of Eco-Industry, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China

    Jingqiao Zhang, Ting Cao & Zheng Liu

  4. Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Science, Ningbo, 315201, China

    Jie Lin

  5. Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China

    Zhiyi Sun & Wenxing Chen

  6. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China

    Wensheng Yan

  7. Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, 201204, China

    Yu Wang

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  1. Yan Gao
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  2. Jinlong Ge
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Correspondence to Yan Gao, Jie Lin or Zheng Liu.

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Gao, Y., Ge, J., Zhang, J. et al. Asymmetrically coordinated main group atomic In-S1N3 interface sites for promoting electrochemical CO2 reduction. Nano Res. 17, 5011–5021 (2024). https://doi.org/10.1007/s12274-024-6513-9

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