Identifying Metallic Transition-Metal Dichalcogenides for Hydrogen Evolution through Multilevel High-Throughput Calculations and Machine Learning

Nian Ran; Bo Sun; Wujie Qiu; Erhong Song; Tingwei Chen; Jianjun Liu

doi:10.1021/acs.jpclett.0c03839

Identifying Metallic Transition-Metal Dichalcogenides for Hydrogen Evolution through Multilevel High-Throughput Calculations and Machine Learning

J Phys Chem Lett. 2021 Mar 4;12(8):2102-2111. doi: 10.1021/acs.jpclett.0c03839. Epub 2021 Feb 24.

Authors

Nian Ran^{1

2}, Bo Sun³, Wujie Qiu^{1

2}, Erhong Song^{1

2}, Tingwei Chen³, Jianjun Liu^{1

2}

Affiliations

¹ State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.
³ College of Information, Liaoning University, Shengyang110036, China.

PMID: 33625239
DOI: 10.1021/acs.jpclett.0c03839

Abstract

High-performance electrocatalysts not only exhibit high catalytic activity but also have sufficient thermodynamic stability and electronic conductivity. Although metallic 1T-phase MoS₂ and WS₂ have been successfully identified to have high activity for hydrogen evolution reaction, designing more extensive metallic transition-metal dichalcogenides (TMDs) faces a large challenge because of the lack of a full understanding of electronic and composition attributes related to catalytic activity. In this work, we carried out systematic high-throughput calculation screening for all possible existing two-dimensional TMD (2D-TMD) materials to obtain high-performance hydrogen evolution reaction (HER) electrocatalysts by using a few important criteria, such as zero band gap, highest thermodynamic stability among available phases, low vacancy formation energy, and approximately zero hydrogen adsorption energy. A series of materials-perfect monolayer VS₂ and NiS₂, transition-metal ion vacancy (TM-vacancy) ZrTe₂ and PdTe₂, chalcogenide ion vacancy (X-vacancy) MnS₂, CrSe₂, TiTe₂, and VSe₂-have been identified to have catalytic activity comparable with that of Pt(111). More importantly, electronic structural analysis indicates active electrons induced by defects are mostly delocalized in the nearest-neighbor and next-nearest neighbor range, rather than a single-atom active site. Combined with the machine learning method, the HER-catalytic activity of metallic phase 2D-TMD materials can be described quantitatively with local electronegativity (0.195·LEf + 0.205·LEs) and valence electron number (Vtmx), where the descriptor is ΔG_H* = 0.093 - (0.195·LEf + 0.205·LEs) - 0.15·Vtmx.