Hollandite, α-MnO2, is of interest as a prospective
cathode material for hydrated zinc-ion batteries (ZIBs); however,
the mechanistic understanding of the discharge process remains limited.
Herein, a systematic study on the initial discharge of an α-MnO2 cathode under a hydrated environment was reported using density
functional theory (DFT) in combination with complementary experiments,
where the DFT predictions well described the experimental measurements
on discharge voltages and manganese oxidation states. According to
the DFT calculations, both protons (H+) and zinc ions (Zn2+) contribute to the discharging potentials of α-MnO2 observed experimentally, where the presence of water plays
an essential role during the process. This study provides valuable
insights into the mechanistic understanding of the discharge of α-MnO2 in hydrated ZIBs, emphasizing the crucial interplay among
the H2O molecules, the intercalated Zn2+ or
H+ ions, and the Mn4+ ions on the tunnel wall
to enhance the stability of discharged states and, thus, the electrochemical
performances in hydrated ZIBs.
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