SMALL, ss.1-14, 2024 (SCI-Expanded)
Herein, P2-type layered manganese and ruthenium oxide is synthesized as
an outstanding intercalation cathode material for high-energy density Na-ion
batteries (NIBs). P2-type sodium deficient transition metal oxide structure,
Na0.67Mn1-xRuxO2 cathodes where x varied between 0.05 and 0.5 are
fabricated. The partially substituted main phase where x = 0.4 exhibits the best
electrochemical performance with a discharge capacity of ≈170 mAh g−1. The
in situ X-ray Absorption Spectroscopy (XAS) and time-resolved X-ray Diffraction
(TR-XRD) measurements are performed to elucidate the neighborhood of
the local structure and lattice parameters during cycling. X-ray photoelectron
spectroscopy (XPS) revealed the oxygen-rich structure when Ru is introduced.
Density of States (DOS) calculations revealed the Fermi-Level bandgap
increases when Ru is doped, which enhances the electronic conductivity of the
cathode. Furthermore, magnetization calculations revealed the presence of
stronger Ru─O bonds and the stabilizing effect of Ru-doping onMnO6 octahedra.
The results of Time-of-flight secondary-ion mass spectroscopy (TOF-SIMS)
revealed that the Ru-doped sample has more sodium and oxygenated-based
species on the surface, while the inner layers mainly contain Ru–O and Mn–O
species. The full cell study demonstrated the outstanding capacity retention
where the cell maintained 70% of its initial capacity at 1 C-rate after 500 cycles.