Unlocking Anion Reduction of Lithium Perchlorate via Electrochemically Coupled Oxygen Atom Transfer

Abstract

Abstract The growing demand for high energy density electrochemical energy storage necessitates energy vectors that maximize the number of electrons transferred per formula unit of active material. Herein, we introduce electrochemically coupled oxygen atom transfer (OAT) as a new paradigm to harness the energy of p-block oxoanions in a Li–metal solid-state battery. Using carbon-supported Fe nanoparticles in a dual role of OAT catalyst and conversion-type cathode active material, we demonstrate the eight-electron anion reduction of ClO4– at >50% conversion, delivering a capacity of 1150 mA h g–1 and an energy density of 1950 W h kg–1. We further demonstrate strategies to enhance the energy density at the electrode level, establishing a foundation for oxoanion-based anion redox in battery systems.