| Affiliation: | 1. School of Advanced Energy, Sun Yat-sen University (Shenzhen), Shenzhen, 518107 P. R. China
School of Environment and Science, and Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan campus, Brisbane, 4111 Australia;2. School of Materials Science and Engineering, Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, South China University of Technology, Guangzhou, 510641 China;3. Research Center for X-ray Science, Department of Physics, Tamkang University, Tamsui, 25137 China;4. School of Environment and Science, and Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan campus, Brisbane, 4111 Australia;5. Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, 230026 China;6. Department of Applied Chemistry and Zhejiang Moganshan Carbon Neutral Innovation Institute, Zhejiang University of Technology, Hangzhou, 310032 P. R. China;7. School of Advanced Energy, Sun Yat-sen University (Shenzhen), Shenzhen, 518107 P. R. China |
| Abstract: | 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. |
