Atomic-Scale
Influence of Grain Boundaries on Li-Ion
Conduction in Solid Electrolytes for All-Solid-State Batteries
James A. Dawson
Pieremanuele Canepa
Theodosios Famprikis
Christian Masquelier
M. Saiful Islam
10.1021/jacs.7b10593.s001
https://acs.figshare.com/articles/journal_contribution/Atomic-Scale_Influence_of_Grain_Boundaries_on_Li-Ion_Conduction_in_Solid_Electrolytes_for_All-Solid-State_Batteries/5734971
Solid electrolytes
are generating considerable interest for all-solid-state
Li-ion batteries to address safety and performance issues. Grain boundaries
have a significant influence on solid electrolytes and are key hurdles
that must be overcome for their successful application. However, grain
boundary effects on ionic transport are not fully understood, especially
at the atomic scale. The Li-rich anti-perovskite Li<sub>3</sub>OCl
is a promising solid electrolyte, although there is debate concerning
the precise Li-ion migration barriers and conductivity. Using Li<sub>3</sub>OCl as a model polycrystalline electrolyte, we apply large-scale
molecular dynamics simulations to analyze the ionic transport at stable
grain boundaries. Our results predict high concentrations of grain
boundaries and clearly show that Li-ion conductivity is severely hindered
through the grain boundaries. The activation energies for Li-ion conduction
traversing the grain boundaries are consistently higher than that
of the bulk crystal, confirming the high grain boundary resistance
in this material. Using our results, we propose a polycrystalline
model to quantify the impact of grain boundaries on conductivity as
a function of grain size. Such insights provide valuable fundamental
understanding of the role of grain boundaries and how tailoring the
microstructure can lead to the optimization of new high-performance
solid electrolytes.
2017-12-10 00:00:00
grain boundary effects
electrolyte
Li 3 OCl
Li-rich anti-perovskite Li 3 OCl
all-solid-state Li-ion batteries
Li-ion migration barriers
grain boundary resistance
grain boundaries