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Orbital-regulated interfacial electronic coupling endows Ni3N with superior catalytic surface for hydrogen evolution reaction

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Abstract

The interstitial structure and weak Ni-N interaction of Ni3N lead to high unoccupied d orbital energy and unsuitable orbital orientation, which consequently results in weak orbital coupling with H2O and slow water dissociation kinetics for alkaline hydrogen evolution catalysis. Herein, we successfully lower the unoccupied d orbital energy of Ni3N to strengthen the interfacial electronic coupling by employing the strong electron pulling capability of oxygen dopants. The prepared O-Ni3N catalyst delivers an overpotential of 55 mV at 10 mA cm−2, very close to the commercial Pt/C. Refined structural characterization indicates the oxygen incorporation can decrease the electron densities around the Ni sites. Moreover, density functional theory calculation further proves the oxygen incorporation can create more unoccupied orbitals with lower energy and superior orientation for water adsorption and dissociation. The concept of orbital-regulated interfacial electronic coupling could offer a unique approach for the rational design of hydrogen evolution catalysts and beyond.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21771169, 51801075, 11722543), the National Key Research and Development Program of China (2017YFA0206703), Anhui Provincial Natural Science Foundation (BJ2060190077), Recruitment Program of Global Expert, and the Fundamental Research Funds for the Central Universities (WK2060190074; WK2060190081, WK2310000066). We also thank the Shanghai Synchrotron Radiation Facility (BL14W1, SSRF) and the Hefei National Synchrotron Radiation Laboratory (BL10B, NSRL) for the characterization of XAFS, UPS and XPS. The computational research in this paper has been done on the supercomputing system in the Supercomputing Center of University of Science and Technology of China.

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science & Technology of China, Hefei, 230026, China

    Yanyan Fang, Da Sun, Shuwen Niu, Jinyan Cai, Yipeng Zang, Yishang Wu, Linqin Zhu, Yufang Xie, Yun Liu, Zixuan Zhu, Amirabbas Mosallanezhad, Di Niu, Zheng Lu, Junjie Shi, Xiaojing Liu, Gongming Wang & Yitai Qian

  2. School of Materials Science and Engineering, Jiangsu University, Zhenjiang, 212013, China

    Dewei Rao

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  1. Yanyan Fang
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Correspondence to Gongming Wang.

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11426_2020_9839_MOESM1_ESM.docx

Orbital-Regulated Interfacial Electronic Coupling Endows Ni3N with Superior Catalytic Surface for Hydrogen Evolution Reaction

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Fang, Y., Sun, D., Niu, S. et al. Orbital-regulated interfacial electronic coupling endows Ni3N with superior catalytic surface for hydrogen evolution reaction. Sci. China Chem. 63, 1563–1569 (2020). https://doi.org/10.1007/s11426-020-9839-y

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