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Nano Research 2023, 16(8): 10796-10802 https://doi.org/10.1007/s12274-023-5859-8
Research Article | Issue | Published: 05 July 2023

The d-orbital regulation of isolated manganese sites for enhanced oxygen evolution

Show Author's Information Xue Bai1,  Jingyi Han1,  Xiaodi Niu2( ),  Jingqi Guan1( )
Institute of Physical Chemistry, College of Chemistry, Jilin University, 2519 Jiefang Road, Changchun 130021, China
College of Food Science and Engineering, Jilin University, Changchun 130062, China
Keywords:
theoretical calculation, single-atom catalyst, oxygen evolution reaction (OER), dual-heteroatom coordination, Mn1-N2S2Cx
Topics:
CalculationsDensity functional theoryElectrocatalysis ElectrocatalystsElectrolysis Free energy GrapheneNanocatalystsOxygen evolution reactionX-ray absorptionX-ray absorption spectroscopy
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Bai X, Han J, Niu X, et al. The d-orbital regulation of isolated manganese sites for enhanced oxygen evolution. Nano Research, 2023, 16(8): 10796-10802. https://doi.org/10.1007/s12274-023-5859-8
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Abstract Full text Electronic supplementary material About this article

Developing transition metal-nitrogen-carbon materials (M-N-C) as electrocatalysts for the oxygen evolution reaction (OER) is significant for low-cost energy conversion systems. Further d-orbital adjustment of M center in M-N-C is beneficial to the improvement of OER performance. Herein, we synthesize a single-Mn-atom catalyst based on carbon skeleton (Mn1-N2S2Cx) with isolated Mn-N2S2 sites, which exhibits high alkaline OER activity (η10 = 280 mV), low Tafel slope (44 mV·dec−1), and excellent stability. Theoretical calculations reveal the pivotal function of isolated Mn-N2S2 sites in promoting OER, including the adsorption kinetics of intermediates and activation mechanism of active sites. The doping of S causes the increase in both charge density and work function of active Mn center, and ortho-Mn1-N2S2Cx expresses the fastest OER kinetics due to the asymmetric plane.


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About this article

The d-orbital regulation of isolated manganese sites for enhanced oxygen evolution

Show Author's information Xue Bai1, Jingyi Han1, Xiaodi Niu2( ), Jingqi Guan1( )
Institute of Physical Chemistry, College of Chemistry, Jilin University, 2519 Jiefang Road, Changchun 130021, China
College of Food Science and Engineering, Jilin University, Changchun 130062, China

Abstract

Developing transition metal-nitrogen-carbon materials (M-N-C) as electrocatalysts for the oxygen evolution reaction (OER) is significant for low-cost energy conversion systems. Further d-orbital adjustment of M center in M-N-C is beneficial to the improvement of OER performance. Herein, we synthesize a single-Mn-atom catalyst based on carbon skeleton (Mn1-N2S2Cx) with isolated Mn-N2S2 sites, which exhibits high alkaline OER activity (η10 = 280 mV), low Tafel slope (44 mV·dec−1), and excellent stability. Theoretical calculations reveal the pivotal function of isolated Mn-N2S2 sites in promoting OER, including the adsorption kinetics of intermediates and activation mechanism of active sites. The doping of S causes the increase in both charge density and work function of active Mn center, and ortho-Mn1-N2S2Cx expresses the fastest OER kinetics due to the asymmetric plane.

Keywords: theoretical calculation, single-atom catalyst, oxygen evolution reaction (OER), dual-heteroatom coordination, Mn1-N2S2Cx

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Publication history
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Acknowledgements

Publication history

Received: 14 April 2023
Revised: 05 May 2023
Accepted: 19 May 2023
Published: 05 July 2023
Issue date: August 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 22075099), the Natural Science Foundation of Jilin Province (No. 20220101051JC), and the Education Department of Jilin Province (No. JJKH20220967KJ)

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