Charging a commercial lithium-ion battery intercalates lithium into the
graphite-based anode, creating various lithium carbide structures. Despite their
economic importance, these structures and the dynamics of their
charging-discharging transitions are not well-understood. We have videoed single
microcrystals of high-quality, natural graphite undergoing multiple
lithiation-delithiation cycles. Because the equilibrium lithium-carbide
compounds corresponding to full, half, and one-third charge are gold, red, and
blue respectively, video observations give direct insight into both the
macromolecular structures and the kinematics of charging and discharging. We
find that the transport during the first lithiation is slow and orderly, and
follows the core-shell or shrinking annuli model with phase boundaries moving at
constant velocities (i.e. non-diffusively). Subsequent lithiations are markedly
different, showing transport that is both faster and disorderly, which indicates
that the initially pristine graphite is irreversibly and considerably altered
during the first cycle. In all cases deintercalation is not the time-reverse of
intercalation. These findings both illustrate how lithium enters nearly
defect-free host material, and highlight the differences between the idealized
case and an actual, cycling graphite anode.