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Balancing hydrogen adsorption/desorption by orbital modulation for efficient hydrogen evolution catalysis
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Journal Article
Balancing hydrogen adsorption/desorption by orbital modulation for efficient hydrogen evolution catalysis
2019
Overview
Hydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction (HER) catalysis. The HER reaction rate is a trade-off between hydrogen adsorption and desorption on the catalyst surface. Herein, we report the rational balancing of hydrogen adsorption/desorption by orbital modulation using introduced environmental electronegative carbon/nitrogen (C/N) atoms. Theoretical calculations reveal that the empty d orbitals of iridium (Ir) sites can be reduced by interactions between the environmental electronegative C/N and Ir atoms. This balances the hydrogen adsorption/desorption around the Ir sites, accelerating the related HER process. Remarkably, by anchoring a small amount of Ir nanoparticles (7.16 wt%) in nitrogenated carbon matrixes, the resulting catalyst exhibits significantly enhanced HER performance. This includs the smallest reported overpotential at 10 mA cm
−2
(4.5 mV), the highest mass activity at 10 mV (1.12 A mg
Ir
−1
) and turnover frequency at 25 mV (4.21 H
2
s
−1
) by far, outperforming Ir nanoparticles and commercial Pt/C.
Hydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction catalysis. Here, the authors demonstrate the rational balancing of hydrogen adsorption/desorption by orbital modulation for significantly enhanced hydrogen evolution performance.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
