Self‐Regulated Surface Reconstruction of Fe Modified Nickel Tellurium Oxides Enabling Highly Efficient and Durable Oxygen Evolution

Improving the efficiency and stability of oxygen evolution electrocatalysts remains essential for advancing water splitting technologies. Although in situ surface reconstruction into active phases is desirable, it often leads to uncontrolled structural degradation. Herein, we demonstrate that lattice doping of Fe into Ni 2 Te 3 O 8 (NTO) pre‐catalysts triggers a self‐terminating surface reconstruction during OER. The deliberate incorporation of Fe introduced a higher density of unsaturated surface coordination sites and weakened the local surface crystallinity, which collectively accelerated the oxidative transformation of the NTO into an oxyhydroxide‐rich active layer during electrocatalysis. During the reconstructive process, soluble tellurium species released from the host framework spontaneously adsorbed onto the evolving surface and subsequently served as stabilizing anionic units, contributing to the structural integrity of the metastable oxyhydroxide phase. Benefiting from this self‐terminating mechanism, the optimized Fe‐NTO catalyst exhibited remarkable oxygen evolution activity, requiring only 220 mV of overpotential to deliver a current density of 50 mA cm −2 , along with exceptional operational durability exceeding 200 h at the same current. This work highlights the critical role of doping and anionic regulation in controlling reconstruction dynamics and establishes a novel paradigm for designing durable, high‐performance electrocatalysts.