Four charging regimes
from MD simulations. (a) At short times,
the accumulated charge (Q) grows as a square root
of time. (b) At later times, Q saturates exponentially
and enters a superslow regime, during which it saturates exponentially
with a larger decay time constant. The superslow regime is related
to pore overfilling (the inset). Reproduced with permission from ref (113). Copyright 2014 Nature
Publishing Group. (c) In addition to the square-root and exponential
regimes, at very short times, there is a linear regime during which
the charge grows linearly with time (see the inset). This regime is
due to ion migration caused by the applied cell voltage acting on
the ions outside of the pore. (d) Snapshots from MD simulations typical
for various charging regimes. During the short-time linear regime,
the neutral ionic liquids is “compressed” inside the
pore by the adsorbed counterions. The charging proceed by melting
an “interface” between a dense, neutral and a dilute,
charged transient ionic liquid phases. Adapted with permission from
ref (125). Copyright
2018 American Chemical Society.