Highly Reversible Cycling of Zn‐MnO2 Batteries Integrated with Acid‐Treated Carbon Supportive Layer

Zn-MnO2 battery with mild-acid electrolytes has been considered as a promising alternative to Li-ion battery for safe and cost-effective energy storage systems (ESSs), and for full electrification. However, the governing mechanism of MnO2 electrochemistry has not been fully elucidated, hindering further advances in highly reversible MnO2 cathodes. Eventual Mn2+ ion dissolution into the electrolyte adversely triggers the irreversible loss of Mn2+ ions and the excessive precipitation of zinc hydroxyl sulfate (Zn4 SO4 (OH)6 ·xH2 O, ZHS), leading to irreversible capacity loss upon prolonged cycling. To overcome these drawbacks, a rationally renovated cell structure is proposed by integrating an acid-treated carbon supportive layer (aCSL) in the MnO2 cathode, which can play multifunctional roles rendering the additional reaction sites for the reversible formation/decomposition of ZHS and re-utilization of the dissolved Mn2+ ions. Furthermore, the improved affinity of the aCSL toward the electrolyte is beneficial for increasing active surface area and facilitating charge transfer at the cathode side. Benefiting from these features, compared to the conventional cell configuration, the aCSL-integrated Zn-MnO2 cell exhibits superior cycling over 3000 cycles with negligible capacity decay (85.6% retention) at a current of 3 A g-1 .