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

Mingqiang Liu,Suchinda Sattayaporn,Ya-Wei Cai,Fuchun Zhang,Fei Li,Jie Yu,Jia-Ao Wang,Gui-Gen Wang,Ya Yang,Wantana Klysubun

doi:10.1038/s41467-021-25647-8

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.

Highlights

Molybdenum disulfide, as an electronic highly-adjustable catalysts material, tuning its electronic structure is crucial to enhance its intrinsic hydrogen evolution reaction (HER) activity
The electrocatalytic activity of MoS2 is closely associated with its surface electric structure[26,27,28,29,30,31,32,33,34,35,36], many researchers have focused on adjusting the electronic structure of the MoS2 surface to promote electrocatalytic activity, such as surface engineering[26], doping[27], single-atom anchoring[28], phase structure[29,30,31,32,33], interface active site[34,35], and defect[36]
1T0.41MoS2 nanospheres were obtained on carbon cloth (CC) by acidinduced hydrothermal approach at 200 °C for 12 h

Summary

Introduction

Molybdenum disulfide, as an electronic highly-adjustable catalysts material, tuning its electronic structure is crucial to enhance its intrinsic hydrogen evolution reaction (HER) activity. The heterojunction-phase catalyst synthesized by the above-mentioned approach further improves the HER activity and good stability, the understanding and regulation of the surface electronic structure on the MoS2 interface are still huge challenges, and it is very necessary to develop an efficient synthesis approach to obtain stable multiheterogeneous interface catalyst We address these challenges by tuning its electronic structure through phase modulation synergistic with interfacial chemistry and defects of phosphorus or sulfur implantation, and we successfully design and prepare a series of heterojunction-phase-interface electrocatalysts (denoted 1T0.81MoS2@Ni2P and 1T0.72-MoS2@NiS2) with an outstanding HER activity and are stable in dual-pH surroundings.

Methods

Results

Conclusion