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@INPROCEEDINGS{Arinicheva:877311,
      author       = {Arinicheva, Yulia and Zheng, Hao and Tsai, Chih-Long and
                      Nonemacher, Juliane Franciele and Malzbender, Jürgen and
                      Fattakhova-Rohlfing, Dina and Guillon, Olivier and
                      Finsterbusch, Martin},
      title        = {{I}ntrinsic {I}mprovement of {LLZO} {S}olid-{S}tate
                      {E}lectrolyte to {S}uppress {L}i {D}endrite {G}rowth},
      reportid     = {FZJ-2020-02127},
      year         = {2018},
      abstract     = {AbstractAfter the unexpected discovery of similar metal
                      dendrite issues in dense ceramic electrolytes as in
                      conventional liquid ones, the key factors governing the
                      lithium dendrite growth e.g. in Li7La3Zr2O12 are still not
                      fully understood. Possible factors include lithium ion
                      diffusion kinetics at grain boundaries, influenced by
                      microstructure [1, 2] and density [3], as well as
                      inhomogeneous contact between LLZ solid electrolyte and Li
                      electrodes, leading to high contact resistance. Multiple
                      strategies can be employed to reduce the contact resistance:
                      first, the surface can be treated in order to remove
                      LiOH/Li2CO3-contamination [4], second, the effective contact
                      area can be increased [5], third, surface defects can be
                      reduced [6], and finally, the surface can be coated to
                      increase the wettability [7-9].To elucidate the
                      interdependence of the various possibilities, the present
                      work focuses on the effect of doping, microstructure,
                      surface properties and density of the Li6.6La3Zr1.6Ta0.4O12
                      solid state electrolyte on its electrochemical performance,
                      especially the resistance to dendrite penetration. Al-doped
                      and Al-free LLZ:Ta precursor powders with larger (≈5 μm)
                      and nano-sized particles were synthesized via solid-state
                      synthesis and solution-assisted solid-state synthesis,
                      respectively. LLZ:Ta pellets with high density $(>99\%$ of
                      the theoretical density), high conductivity (8bold dot10-4
                      S/cm ) and various grain sizes were obtained for both
                      precursor powders by hot pressing. The grain size dependence
                      of mechanical properties (fracture toughness, micro
                      hardness, Young's modulus), ionic conductivity, cycling
                      stability, stability in contact with humid air was
                      investigated. The conductivity was separated into grain and
                      grain boundary contributions. Activation energies of
                      conductivity for the samples with larger and smaller grains
                      were determined. Lower interfacial resistances and better
                      cycling behaviour was found for the specimens with smaller
                      grains and attributed to surface quality and mechanical
                      properties of the material.1. Sakamoto, J.; Rangasamy, E.;
                      Kim, H.; Kim, Y.; Wolfenstine, J. Synthesis of nano-scale
                      fast ion conducting cubic Li 7 La 3 Zr 2 O 12 .
                      Nanotechnology, 2013, 24(42), 424005.2. Cheng, L.; Chen, W.;
                      Kunz, M.; Persson, K.; Tamura, N.; Chen, G.; Doeff, M.
                      Effect of surface microstructure on electrochemical
                      performance of garnet solid electrolytes. ACS Appl Mater
                      Interfaces, 2015, 7(3), 2073-2081.3. Ren, Y.; Shen, Y.; Lin,
                      Y.; Nan, C.-W. Direct observation of lithium dendrites
                      inside garnet-type lithium-ion solid electrolyte.
                      Electrochemistry Communications, 2015, 57, 27-30.4. Sharafi,
                      A.; Kazyak, E.; Davis, A. L.; Yu, S.; Thompson, T.; Siegel,
                      D. J.; Dasgupta, N. P.; Sakamoto, J. Surface Chemistry
                      Mechanism of Ultra-Low Interfacial Resistance in the
                      Solid-State Electrolyte Li 7 La 3 Zr 2 O 12 . Chemistry of
                      Materials, 2017.5. Basappa, R.H.; Ito, T.; Yamada, H.
                      Contact between garnet-type solid electrolyte and lithium
                      metal anode: influence on charge transfer resistance and
                      short circuit prevention. Journal of The Electrochemical
                      Society, 2017, 164(4), A666-A671.6. Porz, L.; Swamy, T.;
                      Sheldon, B. W.; Rettenwander, D.; Frömling, T.; Thaman, H.
                      L.; Berendts, S.; Uecker, R.; Carter, W. C.; Chiang, Y.-M.
                      Mechanism of Lithium Metal Penetration through Inorganic
                      Solid Electrolytes. Advanced Energy Materials, 2017,
                      1701003.7. Tsai, C. L.; Roddatis, V.; Chandran, C. V.; Ma,
                      Q.; Uhlenbruck, S.; Bram, M.; Heitjans, P.; Guillon, O. Li 7
                      La 3 Zr 2 O 12 Interface Modification for Li Dendrite
                      Prevention. ACS Appl Mater Interfaces, 2016, 8(16),
                      10617-10626.8. Wang, C.; Gong, Y.; Liu, B.; Fu, K.; Yao, Y.;
                      Hitz, E.; Li, Y.; Dai, J.; Xu, S.; Luo, W.; Wachsman, E. D.;
                      Hu, L. Conformal, Nanoscale ZnO Surface Modification of
                      Garnet-Based Solid-State Electrolyte for Lithium Metal
                      Anodes. Nano Lett, 2017, 17(1), 565-571.9. Han, X.; Gong,
                      Y.; Fu, K. K.; He, X.; Hitz, G. T.; Dai, J.; Pearse, A.;
                      Liu, B.; Wang, H.; Rubloff, G.; Mo, Y.; Thangadurai, V.;
                      Wachsman, E. D.; Hu, L. Negating interfacial impedance in
                      garnet-based solid-state Li metal batteries. Nat Mater,
                      2017. 16(5), 572-579.},
      month         = {May},
      date          = {2018-05-13},
      organization  = {ECS - The Electrochemical Society,
                       Seattle (Vereinigte Staaten), 13 May
                       2018 - 17 May 2018},
      cin          = {IEK-1},
      cid          = {I:(DE-Juel1)IEK-1-20101013},
      pnm          = {131 - Electrochemical Storage (POF3-131)},
      pid          = {G:(DE-HGF)POF3-131},
      typ          = {PUB:(DE-HGF)1},
      url          = {https://juser.fz-juelich.de/record/877311},
}