Interfacial electronic structure engineering on molybdenum sulfide for robust dual-pH hydrogen evolution

Mingqiang Liu, Jia-Ao Wang, Wantana Klysubun, Gui-Gen Wang (), Suchinda Sattayaporn, Fei Li, Ya-Wei Cai, Fuchun Zhang, Jie Yu and Ya Yang ()
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Mingqiang Liu: Shenzhen Key Laboratory for Advanced Materials, School of Materials Science and Engineering, Harbin Institute of Technology
Jia-Ao Wang: University of Texas at Austin
Wantana Klysubun: Synchrotron Light Research Institute
Gui-Gen Wang: Shenzhen Key Laboratory for Advanced Materials, School of Materials Science and Engineering, Harbin Institute of Technology
Suchinda Sattayaporn: Synchrotron Light Research Institute
Fei Li: Shenzhen Key Laboratory for Advanced Materials, School of Materials Science and Engineering, Harbin Institute of Technology
Ya-Wei Cai: Shenzhen Key Laboratory for Advanced Materials, School of Materials Science and Engineering, Harbin Institute of Technology
Fuchun Zhang: School of Physics and Electronic Information, Yan’an University
Jie Yu: Shenzhen Key Laboratory for Advanced Materials, School of Materials Science and Engineering, Harbin Institute of Technology
Ya Yang: CAS Center for Excellence in Nanoscience, Beijing Key laboratory of Micro-nano Energy and Sensor, Beijing Institute of Nanoenergy and Nanosystems, Chinese Academy of Science

Nature Communications, 2021, vol. 12, issue 1, 1-13

Abstract: Abstract Molybdenum disulfide, as an electronic highly-adjustable catalysts material, tuning its electronic structure is crucial to enhance its intrinsic hydrogen evolution reaction (HER) activity. Nevertheless, there are yet huge challenges to the understanding and regulation of the surface electronic structure of molybdenum disulfide-based catalysts. Here we address these challenges by tuning its electronic structure of phase modulation synergistic with interfacial chemistry and defects from phosphorus or sulfur implantation, and we then successfully design and synthesize electrocatalysts with the multi-heterojunction interfaces (e.g., 1T0.81-MoS2@Ni2P), demonstrating superior HER activities and good stabilities with a small overpotentials of 38.9 and 95 mV at 10 mA/cm2, a low Tafel slopes of 41 and 42 mV/dec in acidic as well as alkaline surroundings, outperforming commercial Pt/C catalyst and other reported Mo-based catalysts. Theoretical calculation verified that the incorporation of metallic-phase and intrinsic HER-active Ni-based materials into molybdenum disulfide could effectively regulate its electronic structure for making the bandgap narrower. Additionally, X-ray absorption spectroscopy indicate that reduced nickel possesses empty orbitals, which is helpful for additional H binding ability. All these factors can decrease Mo-H bond strength, greatly improving the HER catalytic activity of these materials.

Date: 2021
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DOI: 10.1038/s41467-021-25647-8

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