期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 277, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119236
关键词
Hydrogen evolution reaction; Ruthenium single atoms; Molybdenum carbide; Nitrogen doping; Anti-Ostwald ripening
资金
- Taishan Scholars Project Special Funds [tsqn201812083]
- Natural Science Foundation of Shandong Province [ZR2019YQ20, 2019JMRH0410]
- Tip-top Scientific and Technical Innovative Youth Talents of Guangdong Special Support Program [2016TQ03N541]
- Guangdong Natural Science Funds for Distinguished Young Scholar [2017B030306001]
- National Natural Science Foundation of China [51972147]
The irreversible sintering of supported ruthenium (Ru) catalyst in the preparation process has seriously affected its hydrogen evolution reaction (HER) activity and stability. Herein, ultrathin nitrogen-doped molybdenum carbide nanosheets (N-Mo2C NSs) is used as a versatile support to stabilize Ru single atoms (SAs) sites via the anti-Ostwald ripening. Ru SAs are dispersed into the N-Mo2C NSs matrix via the strong bonding between the Ru atoms and Mo2C NSs regulated by N doping. The atomic isolated Ru SAs are confirmed by spherical aberration correction transmission electron microscopy (AC HAADF-STEM) and X-ray absorption fine structure (XAFS) measurements. Ru SAs/N-Mo2C NSs exhibits outstanding HER performance, with a small overpotential of 43 mV at 10 mA/cm(2), and robust catalytic stability in 1.0 M KOH. Importantly, Ru SAs/N-Mo2C NSs possesses a higher mass activity of 6.44 A/mg(Ru) than that of 20 wt% PVC (0.91 A/mg(Pt)) at the overpotential of 100 mV. Theoretical calculations further reveal that the high HER activity of Ru SAs/N-Mo2C NSs is derived from the synergistically accelerated the dissociation of H2O and the optimized H adsorption strength in Mo-Ru interface. This result provides a new direction for the rational designing monatomic electrocatalysts for HER via support interaction effect.
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