Partial Sulfidation Strategy to NiFe‐LDH@FeNi2S4 Heterostructure Enable High‐Performance Water/Seawater Oxidation

Abstract The development of a high‐performance electrocatalyst for oxygen evolution reaction (OER) is imperative but challenging. Here, a partial sulfidation route to construct Ni 2 Fe‐LDH/FeNi 2 S 4 heterostructure on nickel foam (Ni 2 Fe‐LDH/FeNi 2 S 4 /NF) by adjusting the hydrothermal duration is reported. The heterostructures afford abundant hydroxide/sulfide interfaces that offer plentiful active sites, rapid charge and mass transfer, favorable adsorption energy to oxygenated species (OH − and OOH) evidenced by the density functional theory calculations, which synergistically boost the alkaline water oxidation. In the 1.0 m KOH solution, Ni 2 Fe‐LDH/FeNi 2 S 4 /NF exhibits an excellent OER catalytic activity with a much smaller overpotential (240 mV) to reach the current density of 100 mA cm −2 than single‐phase Ni 2 Fe‐LDH/NF (279 mV) or FeNi 2 S 4 /NF (271 mV). More impressively, 2000 cycles of cyclic voltammetry scan for water oxidation results in the formation of a sulfate layer over the catalyst. The corresponding post‐catalyst demonstrates better OER activity and durability than the initial one in the alkaline simulated seawater electrolyte. The post‐Ni 2 Fe‐LDH/FeNi 2 S 4 /NF delivers smaller overpotential (250 mV) at 100 mA cm −2 and longer stability time than the original form (260 mV). The post‐formed sulfate passivating layer is responsible for the outstanding corrosion resistance of the salty‐water oxidation anode since it can effectively repel chloride.