Although
transitional metal dichalcogenides have been regarded
as appealing electrodes for sodium/potassium-ion batteries (SIBs/PIBs)
owing to their high theoretical capacity, it is a key challenge to
realize dichalcogenide anodes with long-period cycling performance
and high-rate capability because of their poor conductivity and large
volumetric change. Herein, polypyrrole-encapsulated VSe2 nanoplates (VSe2@PPy) were prepared by the selenization
of VOOH hollow nanospheres and subsequent in situ polymerization and coating by pyrrole. Benefiting from the inherent
metallicity of VSe2, the improvement in the conductivity
and the structural protection provided by the PPy layer, the VSe2@PPy nanoplates exhibited enhanced sodium/potassium-storage
performances, delivering a superior rate capability with a capacity
of 260.0 mA h g–1 at 10 A g–1 in
SIBs and 148.6 mA h g–1 at 5 A g–1 in PIBs, as well as revealing an ultrastability in cycling of 324.6
mA h g–1 after 2800 cycles at 4 A g–1 in SIBs. Moreover, the insertion and conversion mechanisms of VSe2@PPy in SIBs with intermediates of Na0.6VSe2, NaVSe2, and VSe were elucidated by in
situ/ex situ X-ray diffraction combined
with ex situ transmission electron microscopy observation
and in situ potentio-electrochemical impedance spectroscopy
during the sodiation and desodiation processes. Density functional
theory calculations show that the strong coupling between VSe2 and PPy not only causes it to have a stronger total density
of states and a built-in electric field, leading to an increased electrical
conductivity, but also effectively decreases the ion diffusion barrier.