Enhancing Oxygen Evolution Catalysis of Ni₃Se₂ via Trimetallic Modulation

Abstract

Hydrogen has garnered attention as a promising carbon-free energy carrier capable of addressing escalating energy demands and environmental concerns. However, hydrogen production via alkaline water electrolysis is hindered by the sluggish kinetics of oxygen evolution reaction (OER). Although Ni₃Se₂ has attracted interest as a non-precious metal-based OER catalyst, its performance remains suboptimal. In this work, we present a trimetallic-doped electrocatalyst, CoWCe-Ni₃Se₂, which exhibits outstanding OER performance in alkaline media. The catalyst demonstrates only 204 mV to achieve a current density of 100 mA cm⁻², along with a notably small Tafel slope of 33.59 mV dec⁻¹. Furthermore, it shows exceptional operational durability, maintaining 95% of its initial activity over 90 hours of continuous electrolysis. Mechanistic insights derived from density functional theory (DFT) calculations reveal that the co-doping of W and Ce facilitates the adsorption of critical *OOH intermediates and significantly lowers the energy barrier of the rate-determining step (RDS). The enhanced catalytic performance is attributed to the improved electrical conductivity, increased active surface area, and optimized adsorption/desorption behavior of reaction intermediates. Beyond introducing a highly active and stable OER electrocatalyst, this study provides a fundamental understanding of the synergistic effects of multi-element doping for the rational design of high-performance catalysts.