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Research Article

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

Pengcheng Liu1,§, Yanyi Liu1,§, Kaili Wang2( ), Shuai Shi3, Mengmeng Jin1, Jingxiu Liu1, Tao Qin1, Qian Liu4, Xijun Liu5( ), Jia He1( )
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
School of Chemistry and Chemical Engineering and Environmental Engineering, Weifang University, Weifang 261061, China
Department of Electrical Engineering and Automation, Luoyang Institute of Science and Technology, Luoyang 471023, China
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
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

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

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Graphical Abstract

Mn single-atom dual functional catalysts with low oxidation state were developed for carbon dioxide and oxygen electroreductions. Changes in electrode potential will affect the adsorption behavior of Mn single-atom and the electronic structure of intermediates during the electroreduction.

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.

Keywords

electrode potential micro-environmentsMn single-atom catalystcarbon dioxide reduction reactionoxygen reduction reactionconstant potential models

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Nano Research
Volume 17 Issue 9,
September 2024
Pages 7957-7966
DOI: 10.1007/s12274-024-6799-7
Cite this article:
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 Research, 2024, 17(9): 7957-7966. https://doi.org/10.1007/s12274-024-6799-7
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Electrocatalysis

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Received: 13 April 2024
Revised: 24 May 2024
Accepted: 29 May 2024
Published: 01 July 2024
© Tsinghua University Press 2024
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