Hierarchical Porous Ni3S4 with Enriched High-Valence Ni Sites as a Robust Electrocatalyst for Efficient Oxygen Evolution Reaction

Electrochemical water splitting is a common way to produce hydrogen gas, but the sluggish kinetics of the oxygen evolution reaction (OER) significantly limits the overall energy conversion efficiency of water splitting. In this work, a highly active and stable, meso-macro hierarchical porous Ni3S4 architecture, enriched in Ni3+ is designed as an advanced electrocatalyst for OER. The obtained Ni3S4 architectures exhibit a relatively low overpotential of 257 mV at 10 mA cm(-2) and 300 mV at 50 mA cm(-2). Additionally, this Ni3S4 catalyst has excellent long-term stability (no degradation after 300 h at 50 mA cm(-2)). The outstanding OER performance is due to the high concentration of Ni3+ and the meso-macro hierarchical porous structure. The presence of Ni3+ enhances the chemisorption of OH-, which facilitates electron transfer to the surface during OER. The hierarchical porosity increases the number of exposed active sites, and facilitates mass transport. A water-splitting electrolyzer using the prepared Ni3S4 as the anode catalyst and Pt/C as the cathode catalyst achieves a low cell voltage of 1.51 V at 10 mA cm(-2). Therefore, this work provides a new strategy for the rational design of highly active OER electrocatalysts with high valence Ni3+ and hierarchical porous architectures.