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Constructing artificial mimic-enzyme catalysts for carbon dioxide electroreduction

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Abstract

Natural bio-enzyme catalysts usually exhibit unexpected performances for many significant reactions, which are worthy of reference. Here we report artificial metal-sulfur-carbon (M-S-C) mimic-enzyme catalysts based on bionic design. The catalysts combine metal centers and functional ligands, which realize the universal fabrication of phase and adjustable dimension. The synthesized catalysts inherit the highly active and selective feature of bio-enzyme catalysts. When directly used for carbon dioxide electroreduction reaction, the Sn-S-C catalyst exhibits high selectivity for formate (Faradaic efficiency >95%), as well as a continuous stability over 120 h at a high current density of 740 mA cm−2, greatly outperforming the reported catalysts for formate formation. The catalytic sites and pathways are probed with in-situ Fourier transform infrared (FTIR) spectra, in-situ Raman spectra and synchrotron-radiation X-ray photoelectron spectra. These results break the inherent conundrum that it is impossible to simultaneously realize activity and durability under high selectivity. Our findings offer a versatile strategy to inherit from nature and integrate different components, thus designing efficient catalysts for various challenging reactions and energy conversions via a natural sustainable way.

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Acknowledgements

This work was supported by the National Key R&D Program of China (2019YFA0210004, 2017YFA0207301), the Strategic Priority Research Program of Chinese Academy of Sciences (XDB36000000), the National Natural Science Foundation of China (22125503, 21975242, U2032212, 21890754, 2212500041), the Youth Innovation Promotion Association of CAS (CX2340007003), the Major Program of Development Foundation of Hefei Center for Physical Science and Technology (2020HSC-CIP003), the Key Research Program of Frontier Sciences of CAS (QYZDYSSW-SLH011), the Fok Ying-Tong Education Foundation (161012), Users with Excellence Program of Hefei Science Center (2020HSC-UE001), and the University Synergy Innovation Program of Anhui Province (GXXT-2020-001).

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Authors and Affiliations

  1. Hefei National Laboratory for Physical Sciences at Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China

    Li Li, Xiaodong Li, Shumin Wang, Kai Zheng, Ming Zuo, Xiaolong Zu, Yuan Zhao, Wensheng Yan, Junfa Zhu, Yongfu Sun & Yi Xie

  2. Engineering Laboratory for Next Generation Power and Energy Storage Batteries, Tsinghua Shenzhen International Graduate School, Shenzhen, 518055, China

    Qidong Li

  3. Laboratory of Advanced Materials, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China

    Qidong Li

  4. Institute of Energy, Hefei Comprehensive National Science Center, Hefei, 230031, China

    Yongfu Sun & Yi Xie

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  1. Li Li
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  2. Qidong Li
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  3. Xiaodong Li
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  4. Shumin Wang
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  8. Yuan Zhao
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  10. Junfa Zhu
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  11. Yongfu Sun
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  12. Yi Xie
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Correspondence to Yongfu Sun.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Li, L., Li, Q., Li, X. et al. Constructing artificial mimic-enzyme catalysts for carbon dioxide electroreduction. Sci. China Chem. 65, 106–113 (2022). https://doi.org/10.1007/s11426-021-1116-6

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  • DOI: https://doi.org/10.1007/s11426-021-1116-6

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