Efficient and Robust Hydrogen Evolution: Phosphorus Nitride Imide Nanotubes as Supports for Anchoring Single Ruthenium Sites |
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| Authors: | Dr. Jian Yang Dr. Bingxu Chen Dr. Xiaokang Liu Dr. Wei Liu Dr. Zhijun Li Prof. Juncai Dong Dr. Wenxing Chen Prof. Wensheng Yan Prof. Tao Yao Prof. Xuezhi Duan Prof. Yuen Wu Prof. Yadong Li |
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| Affiliation: | 1. Department of Chemistry, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei, China;2. Department of Chemistry, Tsinghua University, Beijing, P.R. China;3. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, China;4. National Synchrotron Radiation Laboratory (NSRL), University of Science and Technology of China, Hefei, Anhui, China;5. Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Application, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, China;6. Institute of High Energy Physics, Beijing, China |
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| Abstract: | Amorphous phosphorus nitride imide nanotubes (HPN) are reported as a novel substrate to stabilize materials containing single‐metal sites. Abundant dangling unsaturated P vacancies play a role in stabilization. Ruthenium single atoms (SAs) are successfully anchored by strong coordination interactions between the d orbitals of Ru and the lone pair electrons of N located in the HPN matrix. The atomic dispersion of Ru atoms can be distinguished by X‐ray absorption fine structure measurements and spherical aberration correction electron microscopy. Importantly, Ru SAs@PN is an excellent electrocatalyst for the hydrogen evolution reaction (HER) in 0.5 m H2SO4, delivering a low overpotential of 24 mV at 10 mA cm?2 and a Tafel slope of 38 mV dec?1. The catalyst exhibits robust stability in a constant current test at a large current density of 162 mA cm?2 for more than 24 hours, and is operative for 5000 cycles in a cyclic voltammetry test. Additionally, Ru SAs@PN presents a turnover frequency (TOF) of 1.67 H2 s?1 at 25 mV, and 4.29 H2 s?1 at 50 mV, in 0.5 m H2SO4 solution, outperforming most of the reported hydrogen evolution catalysts. Density functional theory (DFT) calculations further demonstrate that the Gibbs free energy of adsorbed H* over the Ru SAs on PN is much closer to zero compared with the Ru/C and Ru SAs supported on carbon and C3N4, thus considerably facilitating the overall HER performance. |
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| Keywords: | carbon-free supports hydrogen evolution reaction (HER) phosphorus nitride ruthenium single atoms |
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