Data-driven pursuit of electrochemically stable 2D materials with basal plane activity toward oxygen electrocatalysis

Abstract

In silico design of efficient electrocatalysts for the oxygen reduction/evolution reaction (ORR/OER) is vital for developing the hydrogen economy. However, practical design principles are still lacking due to the difficulty of evaluating materials’ catalytic performance (e.g., activity and stability) under electrochemical conditions. Herein, based on the 2D materials database of 2DMatPedia containing over 6300 materials, we develop a data-driven framework for discovering potential 2D materials with intrinsic basal plane activity and electrochemical stability toward oxygen electrocatalysis. Through a systematic evaluation of synthesizability, conductivity, and catalytic performance, we identified 1411 candidates that can be exfoliated from their layered bulk phase, 338 of which exhibit suitable electric conductivity and hold great promise for electrochemical applications, and 47 materials show superior activity for the ORR/OER approaching or beyond the activity benchmark of Pt/IrO₂. Further examinations via grand canonical density functional theory computations and molecular dynamics simulations unveiled possible dissolution and oxidation of the active materials under reaction conditions. These efforts screened out 24 ORR catalysts and two OER catalysts with remarkable superiority to tackle the activity–stability trade-off in oxygen electrocatalysis. Generally, this work proposes a universal framework to discover new materials and elucidates the possible degradation mechanism of electrocatalysts under positive electrode potentials, thus paving the way for designing high-performance electrocatalysts for practical applications.