“…One strategy to improve intrinsic catalytic activities of transition metal-based OER catalysts is the synthesis of mixed transition metal-based materials, which could outperform their single-component counterparts. − The NiFe-based catalysts are particularly promising since both Ni and Fe are earth-abundant transition metals, and addition of an appropriate amount of Fe into Ni-based catalysts could greatly increase their OER activities. − Recent studies have shown that various NiFe-based compounds, including their oxides and oxyhydroxides, and their hybrids formed by adding other components, can show high OER catalytic activities. − However, their performance still needs significant improvement due to their low conductivity and small catalytically active surface area. The NiFe alloys could be an attractive option to address these challenges in terms of tunable content of Fe and excellent conductivity; in particular, the catalytically active sites of NiFe oxides/(oxy)hydroxides could be derived from their surfaces spontaneously both in the ambient environment and during the anodic oxidation. ,, Until now, there have been only a few studies using NiFe alloys as OER catalysts, and the reported ones still have relatively low activities. ,, Several great challenges exist for significantly improving their OER activities: (1) NiFe alloy NPs with greatly reduced size have significantly increased surface area (researchers are even reducing the size of OER catalysts to the single-atom level to increase the number of exposed active sites), but they easily aggregate to reduce the accessible active sites on them and inhibit the mass diffusion; , (2) the electron transfer/transport between these alloys and the electrode is slow and needs to be greatly accelerated; , (3) both strong reducing agents and large surfactants are required to create the non-noble NiFe alloy NPs, making the synthesis process nonenvironmentally friendly and complicated; , (4) approaches to controllably synthesize NiFe alloy NPs for optimizing their OER activities are still lacking. , …”