Although lithium metal anodes are expected to increase
the energy
density of next-generation batteries, dendrite growth during charge
remains a major bottleneck preventing widespread implementation. Composite
solid electrolytes with ceramic particles embedded in a polymer matrix
have the potential to prevent dendrites owing to the higher mechanical
stiffness while also possessing the flexibility to maintain contact
with the electrode. However, microscopically, the different mechanical
and electrochemical properties of the polymer and ceramic domains
can cause inhomogeneous charge transfer at the Li/electrolyte interface,
which can lead to nonuniform Li deposition and propagation of dendrites.
Here, we computationally examine the coupled electrochemical, transport,
and mechanical processes at the interface to determine the propensity
for dendrite formation and possible approaches to mitigate this issue.
Predictions of two possible microstructures at the interface, namely,
(i) where both the polymer and ceramic come in contact with Li metal
and (ii) when only the polymer comes in contact with Li metal, suggest
that the former has a greater tendency for nonuniform plating. In
addition, predictions suggest that minimizing the interfacial resistance
between polymers and ceramics and incorporating interlayers between
the electrode and electrolyte help mitigate current heterogeneity.
These predictions provide guidance for experimental approaches to
prevent dendrites in composite electrolytes.