posted on 2025-04-07, 15:03authored byTimofey Averianov, Xinle Zhang, Ryan Andris, Daniel Olds, Michael J. Zachman, Ekaterina Pomerantseva
Bilayered vanadium
oxides (BVOs) are promising cathode
materials
for beyond-Li-ion batteries due to their tunable chemistries and high
theoretical capacities. However, the large size of beyond-Li+ ions limits electrochemical cycling and rate capability of BVO electrodes.
Recent reports of MXene-derived BVOs with nanoscale flower-like morphology
have shown improved electrochemical stability at high rates up to
5C in nonaqueous lithium-ion batteries. Here, we report how morphological
stabilization can lead to improved rate capability in potassium-ion
batteries (PIBs) through the synthesis and electrochemical characterization
of MXene-derived K-preintercalated BVOs (MD-KVOs), which were derived
from two V2CTx precursor materials
prepared using two different etching protocols. We show that the etching
conditions affect the surface chemistry of the MXene, which plays
a role in the MXene-to-oxide transformation process. MXene derived
from a milder etchant transformed into a nanoflower MD-KVO with two-dimensional
(2D) nanosheet petals (KVO-DMAE) while a more aggressive etchant produced
a MXene that transformed into a MD-KVO with one-dimensional (1D) nanorod
morphology (KVO-CMAE). Electrochemical cycling of the produced MD-KVOs
after drying at 200 °C under vacuum (KVO-DMAE-200 and KVO-CMAE-200)
in PIBs showed that electrochemical stability of MD-KVO at high rates
improved through the morphological stabilization of 2D particles combined
with the control of interlayer water and K+ ion content.
Structure refinement of KVO-DMAE-200 further corroborates the behavior
observed during K+ ion cycling, connecting structural and
compositional characteristics to the improved rate capability. This
work demonstrates how proper synthetic methodology can cause downstream
effects in the control of structure, chemical composition, and morphology
of nanostructured layered oxide materials, which is necessary for
development of future materials for beyond-Li-ion battery technologies.