Facile and Scalable Mechanochemical Synthesis of Defective MoS2 with Ru Single Atoms Toward High‐Current‐Density Hydrogen Evolution

• Published in: Small (Weinheim an der Bergstrasse, Germany) Vol. 19; no. 32; pp. e2300807 - n/a
• Main Authors: Lang, Chengguang, Jiang, Wenbin, Yang, Cheng‐Jie, Zhong, Hao, Chen, Peirong, Wu, Qilong, Yan, Xuecheng, Dong, Chung‐Li, Lin, Yue, Ouyang, Liuzhang, Jia, Yi, Yao, Xiangdong
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 09.08.2023
• Subjects: Adsorption; asymmetrical electronic distribution; atomic metal species; Atomic properties; Ball milling; Catalysts; Density functional theory; high‐current‐density hydrogen evolution; Hydrogen evolution; Hydrogen production; Mass production; Molybdenum disulfide; Nanotechnology; Skewed distributions; Stability tests; vacancy defects
• ISSN: 1613-6810; 1613-6829
• DOI: 10.1002/smll.202300807

Designing a facile strategy to prepare catalysts with highly active sites are challenging for large‐scale implementation of electrochemical hydrogen production. Herein, a straightforward and eco‐friendly method by high‐energy mechanochemical ball milling for mass production of atomic Ru dispersive in defective MoS2 catalysts (Ru1@D‐MoS2) is developed. It is found that single atomic Ru doping induces the generation of S vacancies, which can break the electronic neutrality around Ru atoms, leading to an asymmetrical distribution of electrons. It is also demonstrated that the Ru1@D‐MoS2 exhibits superb alkaline hydrogen evolution enhancement, possibly attributing to this electronic asymmetry. The overpotential required to deliver a current density of 10 mA cm−2 is as low as 107 mV, which is much lower than that of commercial MoS2 (C‐MoS2, 364 mV). Further density functional theory (DFT) calculations also support that the vacancy‐coupled single Ru enables much higher electronic distribution asymmetry degree, which could regulate the adsorption energy of intermediates, favoring the water dissociation and the adsorption/desorption of H*. Besides, the long‐term stability test under 500 mA cm−2 further confirms the robust performance of Ru1@D‐MoS2. Our strategy provides a promising and practical way towards large‐scale preparation of advanced HER catalysts for commercial applications. The high‐energy mechanochemical ball milling strategy is adopted for the massive preparation of atomic Ru‐doped defective molybdenum disulfide (MoS2). The as‐obtained Ru1@D‐MoS2 catalyst with a unique coordination configuration of atomic Ru provides the necessary driving force to accelerate water dissociation and alter the adsorption/desorption of H* by optimizing intermediates binding, leading to a superb alkaline hydrogen evolution performance. This strategy provides a promising and practical way toward large‐scale preparation of advanced HER catalysts for commercial application.