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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},
}