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

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.