Oxygen‐Bridged Terbium Pairs Anchor the Pt Lattice to Break the Activity‐Stability Trade‐Off in Acidic Oxygen Reduction Reaction

Developing Pt‐based catalysts that simultaneously achieve high activity and durability for the acidic oxygen reduction reaction (ORR) remains a formidable challenge due to the intrinsic trade‐off between lattice stability and surface reactivity. Herein, a “reactive dissolution‐capture” strategy is reported to construct a Pt catalyst incorporated with atomically dispersed Tb species, identified as unique oxygen‐bridged Tb‐O‐Tb “molecular buckles.” Unlike conventional alloys, this configuration leverages the intrinsic oxophilicity of Tb to firmly anchor the dopants into the Pt lattice. Advanced spectroscopy and density functional theory (DFT) calculations reveal that this configuration exerts a dual activation‐stabilization effect: it not only downshifts the Pt d‐band center to optimize intermediate adsorption for accelerated kinetics but also forms robust Pt─O covalent bonds that rigidly immobilize the lattice atoms against dissolution. Consequently, the PtTb/C catalyst delivers an exceptional half‐wave potential of 0.935 V and sustains its performance with negligible decay after 200 000 voltage cycles. This work offers a fresh paradigm for leveraging the intrinsic oxophilicity of rare‐earth elements to engineer highly active and ultra‐stable catalytic interfaces.