“…Particularly, NiFe layered double hydroxides (LDHs) have become one of the most prospective electrocatalytic materials owing to their unique two-dimensional layered structure, tunable interlayer anions, and excellent stability under alkaline conditions. − However, the disadvantages of NiFe double hydroxides, such as poor electrical conductivity and a lack of active sites, have seriously affected their application in electrocatalytic water decomposition. In this regard, in situ etching of NiFe LDH and introducing cationic vacancies into it, which can improve the electrical conductivity and increase the active sites of the material, is considered as a reliable strategy. − The introduction of metal cation vacancies can modulate the surrounding electronic structure and promote hydroxide adsorption during water decomposition, accelerating the slow four-electron kinetic process of OER. − For example, Wang et al successfully introduced nickel vacancies and iron vacancies into NiFe LDH by defect engineering, which modulated the adsorption energy of some intermediates and improved the OER performance of the catalyst …”