Enhanced Oxygen Evolution Reaction Performance by Dynamic Adsorption of Intermediates on C2N-Supported Single Atom Catalysts

The dynamic adsorption of possible intermediates on single-atom catalysts (SACs) under working condition plays a key role in the electrocatalytic performance by the oxygen evolution reaction (OER), and therefore the performance of the dynamic adsorption should be fully considered in the theoretical screening of potential SACs. Based on density functional theory calculations, the OER performance of 27 types of C2N-supported single transition metal atoms (TM@C2N) is systematically investigated without and with considering the dynamic adsorption of possible intermediates. Without considering dynamic adsorption, only Rh@C2N and Ni@C2N are screened out as good catalysts. However, by further considering the dynamic adsorption configurations of possible intermediates, more promising TM@C2N SACs including Fe(Co, Ni, Ru, Rh, Ir)@C2N toward the OER are screened out. The presence of the intermediates (*HO, *O) on SACs could shift their d band center toward lower energy level, which makes the interaction between the adsorbate and SACs moderate and thus enhances their OER performance. The present work is instructive for further screening and designing of efficient single-atom catalysts for the oxygen evolution reaction.