Grain Boundary Effects of Hierarchical Ni‐Fe (Oxy)hydroxide Nanosheets in Water Oxidation

Abstract The robust and scalable oxygen evolution electrocatalysts that can deliver high current densities at low applied potential is a great challenge for the large‐scale industrial application in hydrogen production. Here, the preparation of a grain‐boundary‐rich Ni‐Fe (oxy)hydroxide catalyst on Ni foam is reported using a scalable coating approach followed by a chemical precipitating treatment. This facile method effectively assembles the hierarchical Ni‐Fe (oxy)hydroxide nanosheet in the ultrasmall crystalline domains (<4 nm) with rich grain boundaries. The hierarchical nanosheet structure with the grain boundaries provides more accessible catalytic sites, facile charge, and mass transfer. Benefiting from the abundant grain boundaries in the hierarchical nanosheets, the as‐prepared Ni‐Fe (oxy)hydroxide electrodes deliver current densities of 500 and 1000 mA cm −2 at overpotentials of only 278 and 296 mV for the oxygen evolution reaction. The prepared electrode also exhibits long‐term durability at a high current density in alkaline conditions.