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@ARTICLE{Rosen:891795,
author = {Rosen, Melanie and Ye, Ruijie and Lobe, Sandra and
Finsterbusch, Martin and Guillon, Olivier and
Fattakhova-Rohlfing, Dina and Mann, Markus},
title = {{C}ontrolling the lithium proton exchange of {LLZO} to
enable reproducible processing and performance optimization},
journal = {Journal of materials chemistry / A},
volume = {9},
number = {8},
issn = {2050-7496},
address = {London Â[u.a.]Â},
publisher = {RSC},
reportid = {FZJ-2021-01742},
pages = {4831 - 4840},
year = {2021},
abstract = {Ceramic solid state-electrolytes attract significant
attention due to their intrinsic safety and, in the case of
the garnet type Li6.45Al0.05La3Zr1.6Ta0.4O12 (LLZO), the
possibility to use Li-metal anodes to provide high energy
densities on a cell and battery level. However, one of the
major obstacles hindering their wide-spread application is
the translation and optimization of production processes
from laboratory to industrial scale. Even though the
plausibility of manufacturing components and cells via wet
processing routes like tape casting and screen printing has
been shown, the impact of the sensitivity of LLZO to air and
protic solvents due to Li+/H+-exchange is not fully
understood yet. An uncontrolled alteration of the powder
surface results in poorly reproducible processing
characteristics and electrochemical performance of the final
battery components and full cells. This knowledge gap is the
cause of the large performance variations reported across
different research labs worldwide and is unacceptable for
up-scaling to industrial level. To close this gap, the
influence of the Li+/H+-exchange taking place at various
steps in the manufacturing process was systematically
investigated in this study. For the first time, this allowed
a mechanistic understanding of its impact on the
processability itself and on the resulting electrochemical
performance of a free-standing LLZO separator. The
importance of a close control of the pre-treatment and
storage conditions of LLZO, as well as contact time with the
solvent could be extracted for each step of the
manufacturing process. As a result, we were able to optimize
the processing of thin, dense, free standing LLZO separators
and significantly improve the total Li-ion conductivity to
3.90 × 10−4 S cm−1 and the critical current density to
over 300 μA cm−2 without making structural changes to
separator or the starting material. These findings do not
only enable a deeper understanding and control over the
manufacturing process, but also show potential for further
improvement of cell concepts already existing in
literature.},
cin = {IEK-1 / JARA-ENERGY},
ddc = {530},
cid = {I:(DE-Juel1)IEK-1-20101013 / $I:(DE-82)080011_20140620$},
pnm = {122 - Elektrochemische Energiespeicherung (POF4-122)},
pid = {G:(DE-HGF)POF4-122},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000624755900027},
doi = {10.1039/D0TA11096E},
url = {https://juser.fz-juelich.de/record/891795},
}