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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 ˜[u.a.]œ},
      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},
}