Electronic Structure Tuning of CoS2 via N-Heteroatom Doping for Efficient Oxygen Evolution Reaction Application

Abstract

A crucial aspect for developing the catalyst is to overcome the oxygen evolution reaction (OER) bottleneck, which can be achieved through forming conductive network for efficient charge transport across the cocatalyst structure using N-heteroatoms doping and simultaneously accelerating the active catalyst centres. As the nitrogen have the ability to modulated the electronic structure of the host material, owing to its promising electron-withdrawing ability from the neighboring metal-catalyst via donor–acceptor interaction, which results in the optimal electronic structure of the cocatalyst with improved material conductivity and catalytically active sites. In this study, we synthesized cost-effective nitrogen-doped CoS2 (N,CoS2) aggregated nanospheres using a hydrothermal method followed by N-atom doping to enhance catalytic active sites and redox kinetics for efficient OER application. The proposed N,CoS2 exhibits significantly lower overpotential (271 mV) and Tafel slope (63 mV dec⁻1) along with the improved Faradaic efficiency compared to pristine CoS2 (294 and 99 mV dec⁻1), indicating that heteroatom doping enhances OER kinetics. Furthermore, N-CoS2 demonstrated excellent robustness under varied current rates and showed outstanding durability, with long-term stability (75 h) at steady 10, 100, and 500 mA cm⁻2 current densities. Copyright © 2025 Abu Talha Aqueel Ahmed et al. International Journal of Energy Research published by John Wiley & Sons Ltd.