TY  - JOUR
AU  - Finsterbusch, Martin
AU  - Danner, Timo
AU  - Tsai, Chih-Long
AU  - Uhlenbruck, Sven
AU  - Latz, Arnulf
AU  - Guillon, Olivier
TI  - High Capacity Garnet-Based All-Solid-State Lithium Batteries: Fabrication and 3D-Microstructure Resolved Modeling
JO  - ACS applied materials & interfaces
VL  - 10
IS  - 26
SN  - 1944-8252
CY  - Washington, DC
PB  - Soc.
M1  - FZJ-2021-01944
SP  - 22329 - 22339
PY  - 2018
AB  - The 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.
LB  - PUB:(DE-HGF)16
C6  - 29888903
UR  - <Go to ISI:>//WOS:000438179000061
DO  - DOI:10.1021/acsami.8b06705
UR  - https://juser.fz-juelich.de/record/892108
ER  -