▎ 摘　　要

Rationally designing efficient and robust catalysts for the oxygen evolution reaction (OER) is increasingly vital for energy conversion technologies. Herein, we develop a core-shell electrocatalyst consisting of an amorphous/crystalline heterophase NiFe alloy encapsulated by ultrathin graphene layers (a/c-NiFe-G) via a rapid microwave thermal shock strategy. The amorphous/crystalline heterostructure generates enriched active sites with high intrinsic activity, while the graphene coatings serve as electron transport pathways and protective layers, resulting in dramatically enhanced OER performance in 1 M KOH with an overpotential (eta(10)) of 250 mV at 10 mA cm(-2), a Tafel slope of 36.5 mV dec(-1), a high turnover frequency (TOF) of 0.87 s(-1) that is 24 times as high as that of the crystalline counterpart when evaluated on a glassy carbon electrode. Further, when supported on porous Ni foam, the catalyst exhibited an eta(10) as low as 217 mV, along with excellent durability (136 h). Various characterization methods, including X-ray absorption fine structure analysis and density functional theory calculations, reveal that unsaturated coordination configurations and abundant amorphous/crystalline boundaries in a/c-NiFe-G are responsible for its superior OER performance. This work offers insights for constructing metastable amorphous/crystalline heterophase catalysts toward highly efficient electrocatalysis.