Rechargeable-battery chemistry based on lithium oxide growth through nitrate anion redox

Abstract

Next-generation lithium-battery cathodes often involve the growth of lithium-rich phases, which enable specific capacities that are 2−3 times higher than insertion cathode materials, such as lithium cobalt oxide. Here, we investigated battery chemistry previously deemed irreversible in which lithium oxide, a lithium-rich phase, grows through the reduction of the nitrate anion in a lithium nitrate-based molten salt at 150 °C. Using a suite of independent characterization techniques, we demonstrated that a Ni nanoparticle catalyst enables the reversible growth and dissolution of micrometre-sized lithium oxide crystals through the effective catalysis of nitrate reduction and nitrite oxidation, which results in high cathode areal capacities (~12 mAh cm–2). These results enable a rechargeable battery system that has a full-cell theoretical specific energy of 1,579 Wh kg–1, in which a molten nitrate salt serves as both an active material and the electrolyte.