Diatomic Metal–Organic Framework Cathode Catalysts for Efficient Oxygen Electrocatalysis

ABSTRACT Metal‐air batteries stand as a sustainable energy technology; however, their large‐scale application is impeded by the high overpotential at cathodes, which compromises cycling stability. Recent investigations have demonstrated that dual‐atom catalysts exhibit superior oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performance compared to single‐atom counterparts, highlighting the critical importance of rational design for highly active diatomic metal–organic frameworks (TM 2 ‐MOF). Herein, we systematically explored the ORR/OER behaviors of TM 2 ‐MOF catalysts (TM = Cu, Ag, Au, Ni, Pd, and Pt) via first‐principles calculations. A combination of structural optimization, stability evaluation, charge density distribution analysis, and thermodynamic free energy computations revealed that Au 2 ‐MOF delivers exceptional catalytic activity, with an extremely low overall overpotential of 0.44 V for ORR/OER processes. This structural innovation not only significantly enhances the catalytic efficiency of TM 2 ‐MOF based catalysts but also provides fundamental insights and novel strategies for advanced electrocatalyst development for metal‐air battery.