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Revealing the role of electrode potential micro-environments in single Mn atoms for carbon dioxide and oxygen electrolysis

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Abstract

Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention. Herein we construct the well-defined Mn single-atom (MnSA) catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions (CO2RR) and oxygen reduction reactions (ORR). MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90% at −0.9 V for CO2RR and higher H2O2 yield from 0.1 to 0.6 V with excellent ORR activity. Density functional theory (DFT) calculations based on constant potential models were performed to study the mechanism of MnSA on CO2RR. The thermodynamic energy barrier of CO2RR is lowest at −0.9 V vs. reversible hydrogen electrode (RHE). Similar DFT calculations on the H2O2 yield of ORR showed that the H2O2 yield at 0.2 V was higher. This study provides a reasonable explanation for the role of electrode potential micro-environments.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 52073214 and 22075211) and Guangxi Natural Science Fund for Distinguished Young Scholars (No. 2024GXNSFFA010008). This work was supported by the open research fund of the Laboratory of Xinjiang Native Medicinal and Edible Plant Resources Chemistry at Kashi University. This research was supported by the TianHe Qingsuo open research fund of Tianjin Science and Technology Association for Youth Scientists (TSYS) in 2022 and National Supercomputing Center in Tianjin (NSCC-TJ).

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  1. Pengcheng Liu and Yanyi Liu contributed equally to this work.

Authors and Affiliations

  1. Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion, School of Chemistry and Chemical Engineering, Institute of New-Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China

    Pengcheng Liu, Yanyi Liu, Mengmeng Jin, Jingxiu Liu, Tao Qin & Jia He

  2. School of Chemistry and Chemical Engineering and Environmental Engineering, Weifang University, Weifang, 261061, China

    Kaili Wang

  3. Department of Electrical Engineering and Automation, Luoyang Institute of Science and Technology, Luoyang, 471023, China

    Shuai Shi

  4. Institute for Advanced Study, Chengdu University, Chengdu, 610106, China

    Qian Liu

  5. State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, School of Resources, Environment and Materials, Guangxi University, Nanning, 530004, China

    Xijun Liu

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  1. Pengcheng Liu
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Revealing the role of electrode potential micro-environments in single Mn atoms for carbon dioxide and oxygen electrolysis

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Liu, P., Liu, Y., Wang, K. et al. Revealing the role of electrode potential micro-environments in single Mn atoms for carbon dioxide and oxygen electrolysis. Nano Res. (2024). https://doi.org/10.1007/s12274-024-6799-7

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