Balancing Hydrogen Adsorption/desorption by Orbital Modulation for Efficient Hydrogen Evolution Catalysis

Overview

Journal Nat Commun

Specialty Biology

Date 2019 Sep 8

PMID 31492875

Citations 16

Authors

Feng Li

Gao-Feng Han

Hyuk-Jun Noh

Jong-Pil Jeon

Ishfaq Ahmad

Shanshan Chen

Changduk Yang

Yunfei Bu

Zhengping Fu

Yalin Lu

Jong-Beom Baek

Affiliations

Soon will be listed here.

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 (4.5 mV), the highest mass activity at 10 mV (1.12 A mg) and turnover frequency at 25 mV (4.21 H s) by far, outperforming Ir nanoparticles and commercial Pt/C.

Citing Articles

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