Self‐Reconstruction of Sulfate‐Containing High Entropy Sulfide for Exceptionally High‐Performance Oxygen Evolution Reaction Electrocatalyst

Abstract Novel earth‐abundant metal sulfate‐containing high entropy sulfides, FeNiCoCrXS 2 (where X = Mn, Cu, Zn, or Al), are synthesized via a two‐step solvothermal method. It is shown that sulfate‐containing FeNiCoCrMnS 2 exhibits superior oxygen evolution reaction (OER) activity with an exceptionally low overpotential of 199, 246, 285, and 308 mV at current densities of 10, 100, 500, and 1000 mA cm –2 , respectively, and surpassing its unary‐, binary‐, ternary‐, and quaternary‐metal counterparts. The electrocatalyst yields exceptional stability after 12 000 cycles and 55 h of durability even at a high current density of 500 mA cm –2 . Various in situ and ex situ analyses are used to investigate the self‐reconstruction of the sulfides during the OER for the first time. The resulting metal (oxy)hydroxide is believed to be the true active center for OER. The remaining sulfate also contributes to the catalytic activity. Density function theory calculation is in good agreement with the experimental result. The extraordinary OER performance of the high entropy sulfide brings a great opportunity for desirable catalyst design for practical applications.