Boosting Water Dissociation Kinetics on Pt-Ni Nanowires by N-Induced Orbital Tuning

Advanced Materials
Yufang XieYitai Qian

Abstract

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 dz2 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.

References

Dec 18, 2008·Chemical Society Reviews·Akihiko Kudo, Yugo Miseki
Apr 18, 2015·Chemical Society Reviews·Xiaoxin Zou, Yu Zhang
Feb 14, 2017·Nature Nanotechnology·Javeed MahmoodJong-Beom Baek

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Citations

Jan 21, 2020·Advanced Materials·Nasir UddinZongyou Yin
Feb 13, 2021·Nano Convergence·Shan WangChuan-Jian Zhong
Mar 19, 2021·Chemistry, an Asian Journal·Ling ShenXiao-Yu Yang
Jul 15, 2021·Chemical Science·Carsten WalterMatthias Driess

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