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

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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.

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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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Authors and Affiliations

  1. Institute of Physical Chemistry, College of Chemistry, Jilin University, 2519 Jiefang Road, Changchun, 130021, China

    Xue Bai, Jingyi Han & Jingqi Guan

  2. College of Food Science and Engineering, Jilin University, Changchun, 130062, China

    Xiaodi Niu

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  1. Xue Bai
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Correspondence to Xiaodi Niu or Jingqi Guan.

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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 Res. 16, 10796–10802 (2023). https://doi.org/10.1007/s12274-023-5859-8

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