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Stabilizing high-valent redox couples and exotic electronic statesnecessitate an understanding of the stabilization mechanism. In oxides, whetherthey are being considered for energy storage or computing, highly oxidizedoxide-anion species rehybridize to form short covalent bonds and are related tosignificant local structural distortions. In intercalation oxide electrodes forbatteries, while such reorganization partially stabilizes oxygen redox, it alsogives rise to substantial hysteresis. In this work, we investigate oxygen redoxin layered Na2-XMn3O7, a positive electrode material with ordered Mn vacancies.We show that coulombic interactions between oxidized oxide-anions and theinterlayer Na vacancies can disfavor rehybridization and stabilize holepolarons on oxygen at 4.2 V vs. Na/Na+. These coulombic interactions providethermodynamic energy saving as large as O-O covalent bonding and enable ~ 40 mVvoltage hysteresis over multiple electrochemical cycles with negligible voltagefade. Our results establish a complete picture of redox energetics byhighlighting the role of coulombic interactions across several atomic distancesand suggest avenues to stabilize highly oxidized oxygen for applications inenergy storage and beyond.

Coulombically-stabilized oxygen hole polarons enable fully reversible oxygen redox