The
electrochemical performances of Ti2CT2 (T =
F, O, and OH) MXenes with different layer structures (monolayer,
bilayer, and pillared structures) as anodes for mono-/multivalent
metal ion (Li+, Na+, Mg2+, and Al3+) batteries (MIBs) were studied via first-principles simulations.
First, metal ions (MIs) adsorbed on Ti2CT2 monolayers
were investigated to reveal the influence of MXene terminated groups
on MIB performance. This indicated that O-terminated MXenes would
be more suitable as electrodes. In particular, the theoretical capacity
of Mg2+ on a Ti2CO2 monolayer could
be more than 1500 mA h g–1. Then, MIs intercalated
into MXene bilayers were considered to better understand the charging/discharging
mechanism. In a Ti2CO2 bilayer with larger interlayer
spacing, monovalent MIs and Mg2+ could form a multilayer
accompanied by drastic expansion/contraction of the electrode, which
still needs to be solved. Finally, imidazolium-based ionic liquids
were used to preintercalate into MXene due to the matching size of
the imidazolium cation, which effectively improved MXene stability
and inhibited the self-stacking of layered MXenes. Our research would
be helpful for theoretically regulating MXene functional groups and
adjusting the interlayer spacing of MXenes via selecting guest molecules
for designing MIBs and other energy storage devices.