4.6 Article

Mechanistic investigation of redox processes in Zn-MnO2 battery in mild aqueous electrolytes

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 9, Issue 36, Pages 20766-20775

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta05022b

Keywords

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Funding

  1. U.S Department of Energy (DOE) Office of Electricity [70247A]
  2. Pacific Northwest National Laboratory (PNNL), a multiprogram laboratory operated by Battelle Memorial Institute for the DOE [DE-AC05-76RL01830]
  3. Linus Pauling Distinguished Postdoctoral Fellowship program at PNNL

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Zinc-MnO2 based batteries have attracted attention for grid-level applications due to impressive theoretical performance, cost effectiveness, and intrinsic safety. This research elucidates the detailed redox processes at the cathode during battery operation and explores the impact of electrolyte additives, providing insight into the overall electrochemical reaction mechanisms during battery operation.
Zinc-MnO2 based batteries have acquired attention for grid-level applications, due to impressive theoretical performance, cost effectiveness and intrinsic safety. However, there are still many challenges that remain elusive due to the complex and controversial mechanisms of operation that hinder commercialization. In this work, the detailed redox processes that occur at the cathode during Zn-MnO2 battery operation are elucidated. Using a blend of structural and electrochemical techniques, the redox pairs that occur during operation are mechanistically studied while also showcasing the true impact of the electrolyte additive (0.1 M MnSO4) in a 1 M ZnSO4 electrolyte. An electrochemical quartz-crystal microbalance (EQCM) has been leveraged to reveal the effect of zinc hydroxy sulfate salt (Zn4SO4(OH)(6)center dot nH(2)O) and zinc manganese oxide (ZnxMnyOz) dissolution/deposition, which are believed to be major components during discharge and charge conditions. These results provide insight not currently available, allowing a holistic view of the electrochemical reaction mechanisms during battery operation.

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