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Research Article

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

Xue Bai1Jingyi Han1Xiaodi 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
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Graphical Abstract

Through the co-coordination of nitrogen and sulfur, the d-orbital electronic structure of isolated Mn sites within the asymmetric plane is regulated and the obtained catalyst exhibits low oxygen evolution reaction (OER) energy barrier, high alkaline OER activity (η10 = 280 mV), low Tafel slope (44 mV·dec−1), and excellent stability.

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.

Electronic Supplementary Material (ESM)

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12274_2023_5859_MOESM1_ESM.pdf (1.3 MB)
Nano Research
Pages 10796-10802
Cite this article:
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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Received: 14 April 2023
Revised: 05 May 2023
Accepted: 19 May 2023
Published: 05 July 2023
© Tsinghua University Press 2023
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