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Currently, single-atom combo catalysts (SACCs) for carbon dioxide reduction reaction (CO2RR) to the formation of HCOOH are still very limited, especially the lanthanide-based SACCs. In this work, the novel SACCs with atomically dispersed In and Ce active sites were successfully prepared on the nitrogen-doped carbon matrix (InCe/CN). Both aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM) images and the extended X-ray absorption fine structure (EXAFS) spectra proved the well-isolated In and Ce atoms. The as-prepared InCe/CN shows a high Faradaic efficiency (FE) (77%) and current density of HCOOH formation (jHCOOH) at −1.35 V vs. reversible hydrogen electrode (RHE), much higher than the single atom catalysts. Theoretical calculations have indicated that the introduced Ce single atom sites not only significantly promote electron transfer but also optimize the In-5p orbitals towards higher selectivity towards the HCOOH formation. This work innovatively extends the design of SACCs towards the main group and Ln metals for more applications.

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Publication history
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Acknowledgements

Publication history

Received: 30 November 2022
Revised: 06 January 2023
Accepted: 07 January 2023
Published: 22 February 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

We gratefully acknowledge the support from the National Key R&D Program of China (No. 2021YFA1501101), the National Natural Science Foundation of China (No. 21971117), the National Natural Science Foundation of China/Research Grant Council of Hong Kong Joint Research Scheme (No. N_PolyU502/21), Functional Research Funds for the Central Universities, Nankai University (No. 63186005), Tianjin Key Lab for Rare Earth Materials and Applications (No. ZB19500202), 111 Project (No. B18030) from China, the Outstanding Youth Project of Tianjin Natural Science Foundation (No. 20JCJQJC00130), the funding for Projects of Strategic Importance of The Hong Kong Polytechnic University (Project Code: 1-ZE2V), Shenzhen Fundamental Research Scheme-General Program (No. JCYJ20220531090807017), the Key Project of Tianjin Natural Science Foundation (No. 20JCZDJC00650), the National Postdoctoral Program for Innovative Talents (No. BX20220157), Open Foundation of State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures (No. 2022GXYSOF07), Departmental General Research Fund (Project Code: ZVUL) from Department of Applied Biology and Chemical Technology of Hong Kong Polytechnic University, and Haihe Laboratory of Sustainable Chemical Transformations. B.H. also thank the support from Research Centre for Carbon-Strategic Catalysis (RC-CSC), Research Institute for Smart Energy (RISE), and Research Institute for Intelligent Wearable Systems (RI-IWEAR) of the Hong Kong Polytechnic University..

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