Highly Active and Durable Double-Layered Hydroxide Electrocatalysts by Tungsten and Sulfur Modification for Oxygen Evolution Reaction

Highly active and durable oxygen evolution reaction (OER) electrocatalysts are necessary for the development of an anion exchange membrane water electrolyzer (AEMWE). In this study, tungsten (W) and sulfur (S) are successfully introduced into NiFe-layered double hydroxide (defined as NiS2@Ni3FeWS/NF) to improve its activity and durability. The AEMWE equipped with NiS2@Ni3FeWS/NF as the anodic catalyst demonstrates a current density of 5 A cm–2 at a remarkably low voltage of 2.06 V. Furthermore, it achieves long-term durability with no noticeable degradation at 1 A cm–2 for 600 h. Experimental and theoretical calculations demonstrate that the synergistic effects of W and S codoping significantly enhance the OER performance by modulating the electronic structure, facilitating surface reconstruction, and inducing the adsorbate evolution mechanism and lattice oxygen oxidation mechanism compatible mechanism. This work articulates the profound significance of rationally designing the mechanism of the OER in enhancing the performance of electrocatalysts and promoting efficient hydrogen production.