Fe-doping and oxygen vacancy achieved by electrochemical activation and precipitation/dissolution equilibrium in...

The poor conductivities and instabilities of accessible nickel oxyhydroxides hinder their use as oxygen evolution reaction (OER) electrocatalysts. Herein, we constructed Fe-NiOOH-O_V-600, an Fe-doped nickel oxide hydroxide with abundant oxygen vacancies supported on nickel foam (NF), using a hydrothermal method and an electrochemical activation strategy involving 600 cycles of cyclic voltammetry, assisted by the precipitation/dissolution equilibrium of ferrous sulfide (FeS) in the electrolyte. This two-step method endows the catalyst with abundant Fe-containing active sites while maintaining the ordered structure of nickel oxide hydroxide (NiOOH). Characterization and density functional theory (DFT) calculations revealed that synergy between trace amounts of the Fe dopant and the oxygen vacancies not only promotes the generation of reconstructed active layers but also optimizes the electronic structure and adsorption capacity of the active sites. Consequently, the as-prepared Fe-NiOOH-O_V-600 delivered large current densities of 100 and 1000 mA cm^-2 for the OER at overpotentials of only 253 and 333 mV in 1 mol/L KOH. Moreover, the catalyst is stable for at least 100 h at 500 mA cm^-2. This work provides insight into the design of efficient transition-metal-based electrocatalysts for the OER.