Research and Development of Zinc-based Rechargeable Batteries in RISING3 (Supporting Information)

It is important to develop a rechargeable battery that is safe and free from resource risk to replace the current lithium–ion battery in various application fields. We have been conducting research and development of aqueous electrolyte batteries with zinc as the negative electrode (anode) through national programs, Research and Development Initiative for Scientific Innovation of New Generation Batteries (RISING, RISING2 and RISING3), commissioned by the New Energy and Industrial Technology Development Organization (NEDO). In RISING2, we demonstrated a full cell that can achieve a target specific energy of 500 Wh kg−1 for a zinc–air system through advancements in elemental technology and full-cell engineering. RISING3 aims to develop a sealed zinc-anode rechargeable battery by developing positive electrode (cathode) materials to replace air electrodes. A notable achievement of this study is proving that the manganese dioxide (MnO2) prepared through electrolysis (EMD) has good rechargeability in alkaline electrolyte systems, in which the amount of structural water in the oxide determines the discharge capacity for the first one-electron reduction. We also found that the newly developed MnO2 from the chemical reduction of permanganate (PMD) enables a reversible two-electron reaction even in the electrolyte containing zinc species, in which hetaerolite (ZnMn2O4) generally forms to inhibit further electrochemical reactions.