Dynamically Reconstructed Fe‐CoOOH Semi‐Crystalline Electrocatalyst for Efficient Oxygen Evolution Reaction

Abstract The development of robust and efficient electrocatalysts for the oxygen evolution reaction (OER) has been the main focus of water electrolysis but remains a great challenge. Here, the synthesis of a highly active and ultra‐stable Fe‐CoOOH electrocatalyst is reported by steering raw cobalt foam via an in situ solution combustion method assisted by a galvanic replacement reaction and subsequent electrochemical reconstruction of the CoFeO x pre‐catalyst. In/ ex situ electrochemical analysis and physicochemical characterizations show that the CoFeO x undergoes quick chemical and slow morphological reconstruction to Fe‐CoOOH nanosheets. The Fe‐CoOOH possesses a semi‐crystalline nature with distinct short‐range ordering and outstanding OER activity with overpotentials as low as 271 and 291 mV at current densities of 500 and 1,000 mA cm −2 , respectively. The remarkable stability under 1,000 mA cm −2 for at least 700 h is achieved. Theoretical calculations confirm the crucial role of Fe doping in facilitating surface reconstruction, enhancing OER activity, and improving the stability of the Fe‐CoOOH. Comparative analysis with other transition metals doping reveals the unique ability of Fe to adsorb onto the CoOOH surface, thereby modulating the electronic density and facilitating faster adsorption of reaction intermediates. This work represents valuable insights into the surface reconstruction and doping processes.