期刊
ADVANCED MATERIALS
卷 31, 期 16, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201807780
关键词
electrocatalysts; hydrogen evolution reaction; orbital tuning; Pt-Ni nanowires; water dissociation kinetics
类别
资金
- Natural Science Fund of China [21771169, 11804325, 11722543, 11875258, 11505187]
- National Key Research and Development Program of China [2017YFA0206703]
- Anhui Provincial Natural Science Foundation [BJ2060190077]
- USTC
- Recruitment Program of Global Expert
- Fundamental Research Funds for the Central Universities [WK2060190074, WK2060190081, WK2310000066]
Although it is commonly believed that the water-dissociation-related Volmer process is the rate-limiting step for alkaline hydrogen evolution reaction (HER) on Pt-based catalysts, the underlying essence, particularly on the atomic scale, still remains unclear. Herein, it is revealed that the sluggish water-dissociation behavior probably stems from unfavorable orbital orientation and the kinetic issue is successfully resolved via N-induced orbital tuning. Impressively, N modified Pt-Ni nanowires deliver an ultralow overpotential of 13 mV at 10 mA cm(-2), which represents a new benchmark for alkaline HER catalysis. Fine-structural characterization and density functional theory analysis illustrate that the introduced nitrogen can uniquely modulate the electron densities around the Ni sites, and further create empty d(z)(2) orbitals with superior orientation for water adsorption and activation. More importantly, it is demonstrated that N-induced orbital modulation can generally boost the alkaline HER activities of Pt-Co, Pt-Ni, and Pt-Cu, offering a new perspective for the design of HER catalysts and beyond.
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