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Nickel-iron sulfide has shown attractive activity in electrocatalytic oxygen evolution reaction (OER). However, the effects of low valence sulfur (S2−) and metal species on OER in binary nickel-iron sulfide have rarely been systematically studied. Works based on post-catalysis characterization have led to the assumption that the real active species are nickel-iron oxyhydroxide, and that nickel-iron sulfide acts only as a precatalyst. Therefore, to study the role of S, Ni, and Fe for the development of nickel-iron sulfide catalyst is of self-evident importance. Herein, a facile solvothermal method is used to synthesize acetylene black coated with nickel-iron sulfide nanosheets. Electrochemical tests show that the presence of low valence S species makes the catalyst have faster OER kinetics, larger active area, and intermediate active species adsorption area. Therefore, the present study reveals the enhancing effect of low valence sulfur species (S2−) on OER in binary nickel-iron sulfide. In situ Raman spectroscopy shows that the generation of γ-NiOOH intermediate is essential and Fe does not directly participate in the oxygen production. Density functional theory (DFT) calculation shows that Ni-OH deprotonation is a rate-determining step for both binary nickel-iron sulfide and nickel sulfide. The addition of Fe into NiSx lightly increases the charge transfer of Ni atom to O atom, which makes deprotonation easier and thereby improves the OER performance.
This work was supported by the National Natural Science Foundation of China (No. 21901007), and the Natural Science Foundation of Anhui Province (No. 2008085QB83).