Transformations
at interfaces between solid-state electrolytes
(SSEs) and lithium metal electrodes can lead to high impedance and
capacity decay during cycling of solid-state batteries, but the links
between structural/chemical/mechanical evolution of interfaces and
electrochemistry are not well understood. Here, we use in situ X-ray
computed tomography to reveal the evolution of mechanical damage within
a Li1+x
Al
x
Ge2–x
(PO4)3 (LAGP) SSE caused by interphase growth during electrochemical cycling.
The growth of an interphase with expanded volume drives fracture in
this material, and the extent of fracture during cycling is found
to be the primary factor causing the impedance increase, as opposed
to the resistance of the interphase itself. Cracks are observed to
initiate near the edge of the lithium/LAGP interface, which agrees
with simulations. The chemomechanical effects of interphase growth
studied here are expected to play a role in a variety of SSE materials,
and this work is a step toward designing durable interfaces.
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