Balancing hydrogen adsorption/desorption by orbital modulation for efficient hydrogen evolution catalysis
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- Balancing hydrogen adsorption/desorption by orbital modulation for efficient hydrogen evolution catalysis
- Li, Feng; Han, Gao-Feng; Noh, Hyuk-Jun; Jeon, Jong-Pil; Ahmad, Ishfaq; Chen, Shanshan; Yang, Changduk; Bu, Yunfei; Fu, Zhengping; Lu, Yalin; Baek, Jong-Beom
- Issue Date
- NATURE PUBLISHING GROUP
- NATURE COMMUNICATIONS, v.10, pp.4060
- 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 H2 s(-1)) by far, outperforming Ir nanoparticles and commercial Pt/C.
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