Abstract
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 mgIr−1) and turnover frequency at 25 mV (4.21 H2 s−1) by far, outperforming Ir nanoparticles and commercial Pt/C.
Highlights
Hydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction (HER) catalysis
Because of its potential value in efficient and scalable hydrogen production, water splitting via the electrochemical hydrogen evolution reaction (HER) has attracted considerable attention from industrial and scientific communities[1,2]. Even though they are the heart of hydrogen evolution catalysis, catalysts with satisfactory performance are still rare, despite the tremendous effort that has been devoted to improving HER catalysts[3,4,5,6,7,8,9,10,11]
In summary, we report the rational design of an efficient catalyst for hydrogen evolution, by balancing hydrogen adsorption/desorption via orbital modulation
Summary
Hydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction (HER) catalysis. Because of its potential value in efficient and scalable hydrogen production, water splitting via the electrochemical hydrogen evolution reaction (HER) has attracted considerable attention from industrial and scientific communities[1,2]. Hydrogen adsorption/desorption on such catalysts can be tailored by tuning the d orbitals of the transition metals With their small atomic radius and high electronegativity, the p orbitals of carbon and nitrogen are able to efficiently interact with the d orbitals of the transition metals[15]. This provides an important opportunity to enhance the catalytic activity of catalysts toward HER via orbital manipulation
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