Surface-Reconstructed CdNNi3 Antiperovskite Electrocatalyst: Unlocking Ampere-Level Current Density for Hydrogen Evolution.

Abstract

Developing conductive electrocatalysts is crucial for decreasing the ohmic loss induced by electric resistance of the catalyst layer in the large-current-density hydrogen evolution reaction (HER), which has been overlooked previously. In this study, we screen a highly conductive antiperovskite CdNNi₃ with negligible ohmic loss, as a highly active and durable HER electrocatalyst capable of unlocking ampere-scale current densities. CdNNi₃ exhibits an impressive activity (an overpotential of 235 mV) at 1 A cm^-2 and maintains its performance steadily at an ampere-scale current density (at 1 A cm^-2 over 400 h). Besides, the CdNNi₃-enabled anion-exchange membrane water electrolyzer outperforms that of the benchmark Pt/C, evidenced by a reduced cell voltage of 160 mV at 1 A cm^-2, and presents a favorable stability at 1 A cm^-2. Importantly, this study experimentally discovers the dynamic surface reconstruction phenomena of antiperovskite nitrides during alkaline HER. Theoretical analysis suggests that the presence of Cd in the reconstructed surface effectively adjusts the local electronic configuration of active sites, which promotes the adsorption of OH and reduces the binding strength to H, thereby facilitating the water dissociation step and reducing the energy barrier of the potential-determining step in the HER process.