Facile and Scalable Mechanochemical Synthesis of Defective MoS2 with Ru Single Atoms Toward High-Current-Density Hydrogen Evolution
作者:Lang, CG (Lang, Chengguang) [1] , [2] , [3] ; Jiang, WB (Jiang, Wenbin) [4] ; Yang, CJ (Yang, Cheng-Jie) [5] ; Zhong, H (Zhong, Hao) [4] ; Chen, PR (Chen, Peirong) [4] ; Wu, QL (Wu, Qilong) [2] , [3] ; Yan, XC (Yan, Xuecheng) [2] , [3] ; Dong, CL (Dong, Chung-Li) [5] ; Lin, Y (Lin, Yue) [6] ; Ouyang, LZ (Ouyang, Liuzhang) [4] ;
DOI10.1002/smll.202300807
在线发表APR 2023
已索引2023-05-03
文献类型Article; Early Access
摘要
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 (Ru-1@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 Ru-1@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 Ru-1@D-MoS2. Our strategy provides a promising and practical way towards large-scale preparation of advanced HER catalysts for commercial applications.
关键词
作者关键词asymmetrical electronic distributionatomic metal specieshigh-current-density hydrogen evolutionmass productionvacancy defects
Keywords PlusEFFICIENTELECTROCATALYSTS
作者信息
通讯作者地址
Yao, Xiangdong
(通讯作者)
Sun Yat Sen Univ Shenzhen, Sch Adv Energy, Shenzhen 518107, Peoples R China
地址
1 Sun Yat Sen Univ Shenzhen, Sch Adv Energy, Shenzhen 518107, Peoples R China
2 Griffith Univ, Sch Environm & Sci, Nathan Campus, Brisbane, Qld 4111, Australia
3 Griffith Univ, Queensland Microand Nanotechnol Ctr, Nathan Campus, Brisbane, Qld 4111, Australia
4 South China Univ Technol, Sch Mat Sci & Engn, Guangdong Prov Key Lab Adv Energy Storage Mat, Guangzhou 510641, Peoples R China
5 Tamkang Univ, Res Ctr X Ray Sci, Dept Phys, Tamsui 25137, Peoples R China
电子邮件地址x.yao@griffith.edu.au
类别/分类
研究方向ChemistryScience & Technology - Other TopicsMaterials SciencePhysics
Web of Science 类别Chemistry, MultidisciplinaryChemistry, PhysicalNanoscience & NanotechnologyMaterials Science, MultidisciplinaryPhysics, AppliedPhysics,