Descriptor-Driven Computational Design of Bifunctional Double-Atom Hydrogen Evolution and Oxidation Reaction Electrocatalysts for Rechargeable Hydrogen Gas Batteries

• Published in: Nano letters Vol. 22; no. 19; pp. 7860 - 7866
• Main Authors: Liu, Zaichun, Yang, Jinlong, Wang, Faxing, Yuan, Yuan, Jiang, Taoli, Zhu, Zhengxin, Li, Ke, Liu, Shuang, Zhang, Kai, Wang, Weiping, Chuai, Mingyan, Sun, Jifei, Wu, Yuping, Chen, Wei
• Format: Journal Article
• Language: English
• Published: American Chemical Society 12-10-2022
• Subjects: rechargeable hydrogen gas batteries; HER/HOR electrochemistry; double-atom catalysts; large-scale energy storage; d-band center theory
• ISSN: 1530-6984; 1530-6992
• DOI: 10.1021/acs.nanolett.2c02569

Rechargeable hydrogen gas batteries (RHGBs) have been attracting much attention as promising all-climate large-scale energy storage devices, which calls for low-cost and high-activity hydrogen evolution/oxidation reaction (HER/HOR) bifunctional electrocatalysts to replace the costly platinum-based catalysts. Based on density functional theory (DFT) computations, herein we report an effective descriptor-driven design principle to govern the HER/HOR electrocatalytic activity of double-atom catalysts (DACs) for RHGBs. We systematically investigate the d-band center variation of DACs and their correlations with HER/HOR free energies. We construct activity maps with the d-band center of DACs as a descriptor, which demonstrate that high HER/HOR electrocatalytic activity can be achieved with an appropriate d-band center of DACs. This work not only broadens the applicability of d-band center theory to the prediction of bifunctional HER/HOR electrocatalysts but also paves the way to fast screening and design of efficient and low-cost DACs to promote practical applications of RHGBs.