1. N coupling with S-coordinated Ru nanoclusters for highly efficient hydrogen evolution in alkaline media
- Author
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Haibo Tang, Ling-Jie Xie, Cheng-Fei Li, Yu Wang, Jia-Wei Zhao, Gao-Ren Li, and Lirong Zheng
- Subjects
Materials science ,Renewable Energy, Sustainability and the Environment ,chemistry.chemical_element ,02 engineering and technology ,General Chemistry ,Overpotential ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Photochemistry ,Persulfate ,01 natural sciences ,0104 chemical sciences ,Nanoclusters ,Ruthenium ,Catalysis ,Metal ,X-ray photoelectron spectroscopy ,chemistry ,visual_art ,visual_art.visual_art_medium ,General Materials Science ,0210 nano-technology ,Spectroscopy - Abstract
Optimizing the coordination/surrounding environments of active metal nanoclusters to promote the catalytic performance during hydrogen evolution reaction (HER) in alkaline media is highly important but extremely challenging. Here, we demonstrate that novel S-coordinated ruthenium (Ru) nanoclusters anchored on N/S-codoped carbon nanosheets (Ru–S/N–C) can be successfully synthesized via the space-confinement pyrolysis of Ru complexes in the framework of polyaniline–ammonia persulfate supermolecules. X-ray absorption fine structure spectroscopy and X-ray photoelectron spectroscopy studies reveal the local coordination structure of Ru–S bonds, the surrounding N/S/C environments of Ru, and the synergistic electronic interactions among N, S, C and Ru atoms. Theoretical calculations further confirm that the coordination/surrounding environments could optimize the adsorption energies of intermediates on Ru through interfacial charge transfer and, thus, accelerate the reaction kinetics of hydrogen evolution. The fabricated Ru–S/N–C exhibits an ultra-small overpotential of 10 mV at 10 mA cm−2 and an extremely high turnover frequency (TOF) of 2.3 H2 s−1 at an overpotential of 50 mV for the HER, as well as a mass catalytic activity about 10 times higher than that of a commercial Pt/C catalyst.
- Published
- 2021