Algorithm screening to accelerate discovery of 2D metal-free electrocatalysts for hydrogen evolution reaction

Abstract

Hydrogen production by electrocatalytic water splitting is currently the most attractive route, but the development of electrocatalysts with high activity, long durability and low cost is still a big challenge. Here, by combining algorithm screening and density functional theory (DFT) computations, we developed a method to predict two-dimensional (2D) metal-free materials with metallicity as efficient electrocatalysts for the hydrogen evolution reaction (HER). From all metal-free compounds in the Materials Project database, we obtained 18 layered materials without band gaps as candidates for the HER. After being exfoliated into monolayers, a stable metal-free material, a C₃N monolayer, proved to be an efficient HER electrocatalyst according to computations. With this strategy, we can adjust the screening conditions with the target to find promising materials, which overcomes the obstacles of traditional trial-and-error methods and greatly saves computational resource. We hope that this work would inspire the development of a new research paradigm and promote the discovery of more functional materials.