IrO2 as benchmark electrocatalyst for acidic oxygen evolution reaction (OER) suffers from its low activity and poor stability. Modulating the coordination environment of IrO2 by chemical doping is a methodology to suppress Ir dissolution and tailor adsorption behavior of active oxygen intermediates on interfacial Ir sites. Herein, the Re‐doped IrO2 with low crystallinity is rationally designed as highly active and robust electrocatalysts for acidic OER. Theoretical calculations suggest that the similar ionic sizes of Ir and Re impart large spontaneous substitution energy and successfully incorporate Re into the IrO2 lattice. Re‐doped IrO2 exhibits a much larger migration energy from IrO2 surface (0.96 eV) than other dopants (Ni, Cu, and Zn), indicating strong confinement of Re within the IrO2 lattice for suppressing Ir dissolution. The optimal catalysts (Re: 10 at%) exhibit a low overpotential of 255 mV at 10 mA cm−2 and a high stability of 170 h for acidic OER. The comprehensive mechanism investigations demonstrate that the unique structural arrangement of the Ir active sites with Re‐dopant imparts high performance of catalysts by minimizing Ir dissolution, facilitating *OH adsorption and *OOH deprotonation, and lowering kinetic barrier during OER. This study provides a methodology for designing highly‐performed catalysts for energy conversion.

The tunable oxygen vacancies of LaNiO3 (LNO-Vo) is realized by the theoretical prediction and NaBH4-reduction approach. The LNO2.7 catalyst exhibits superior catalytic activity and long-time stability for water oxidation. A...

One-dimensional nanotube heterostructures with IrO2-stabilized La2IrO6 is obtained by an electrospinning approach. The La2IrO6/IrO2 catalyst exhibits superior catalytic activity and strong stability for oxygen evolution reaction. The synergistic cooperation between...

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