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High Capacity Garnet-Based All-Solid-State Lithium Batteries: Fabrication and 3D-Microstructure Resolved Modeling
journal contribution
posted on 2018-06-11, 00:00 authored by Martin Finsterbusch, Timo Danner, Chih-Long Tsai, Sven Uhlenbruck, Arnulf Latz, Olivier GuillonThe
development of high-capacity, high-performance all-solid-state batteries
requires the specific design and optimization of its components, especially
on the positive electrode side. For the first time, we were able to
produce a completely inorganic mixed positive electrode consisting
only of LiCoO2 and Ta-substituted Li7La3Zr2O12 (LLZ:Ta) without the use of additional
sintering aids or conducting additives, which has a high theoretical
capacity density of 1 mAh/cm2. A true all-solid-state cell
composed of a Li metal negative electrode, a LLZ:Ta garnet electrolyte,
and a 25 μm thick LLZ:Ta + LiCoO2 mixed positive
electrode was manufactured and characterized. The cell shows 81% utilization
of theoretical capacity upon discharging at elevated temperatures
and rather high discharge rates of 0.1 mA (0.1 C). However, even though
the room temperature performance is also among the highest reported
so far for similar cells, it still falls far short of the theoretical
values. Therefore, a 3D reconstruction of the manufactured mixed positive
electrode was used for the first time as input for microstructure-resolved
continuum simulations. The simulations are able to reproduce the electrochemical
behavior at elevated temperature favorably, however fail completely
to predict the performance loss at room temperature. Extensive parameter
studies were performed to identify the limiting processes, and as
a result, interface phenomena occurring at the cathode active material/solid–electrolyte
interface were found to be the most probable cause for the low performance
at room temperature. Furthermore, the simulations are used for a sound
estimation of the optimization potential that can be realized with
this type of cell, which provides important guidelines for future
oxide based all-solid-state battery research and fabrication.
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3 D reconstructionHigh Capacity Garnet-Based All-Solid-State Lithium Batteriesall-solid-state battery research25 μ melectrodeLLZLiCoO 2capacitymicrostructure-resolved continuum simulationsExtensive parameter studiesinterfaceoptimizationTa-substituted Li 7 La 3 Zr 2 O 12room temperature performanceroom temperature
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