期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 2, 页码 461-466出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201808629
关键词
bridge sites; hydrogen evolution; N surface modification; Ni-N catalyst
资金
- Australian Government
- Australian Research Council [LE160100051]
- ARC Discovery Grant [DP160103107]
- Australian Research Council [LE160100051] Funding Source: Australian Research Council
Nickel-heteroatoms bridge sites are important reaction descriptors for many catalytic and electrochemical processes. Herein we report the controllable surface modification of nickel-nitrogen (Ni-N) bridge sites on metallic Ni particles via a simplified vapor-assisted treatment approach. X-ray absorption spectroscopy (XAS) and Operando Raman spectroscopy verifies the interaction between Ni and surface-anchored N, which leads to distorted Ni lattice structure with improved wettability. The Ni-N bridge sites with appropriate N coverage level plays a critical role in the enhanced hydrogen evolution reaction (HER) and the optimized electrode (Ni-N-0.19) has demonstrated superior HER performances with low overpotential merely of 42 mV for achieving a current density of 10 mA cm(-2), as well as favorable reaction kinetics and excellent durability in alkaline electrolyte. DFT calculations revealed that the appropriate N-coverage level can lead to the most favorable Delta G(H*) kinetics for both adsorption of H* and release of H-2, while high N coverage (Ni-N-0.59) results in weaker H* adsorption, thus a decreased HER activity, corresponding well to our experimental observations. Furthermore, this generic synthetic approach can also be applied to prepare S-modified Ni HER catalyst by generating hydrogen sulfide vapor.
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