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X-ray Nanoimaging of Crystal Defects in Single Grains of Solid-State Electrolyte Li7–3xAlxLa3Zr2O12

Cite this: Nano Lett. 2021, 21, 11, 4570–4576
Publication Date (Web):April 29, 2021
Copyright © 2021 American Chemical Society

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    Abstract Image

    All-solid-state lithium batteries promise significant improvements in energy density and safety over traditional liquid electrolyte batteries. The Al-doped Li7La3Zr2O12 (LLZO) solid-state electrolyte shows excellent potential given its high ionic conductivity and good thermal, chemical, and electrochemical stability. Nevertheless, further improvements on electrochemical and mechanical properties of LLZO call for an in-depth understanding of its local microstructure. Here, we employ Bragg coherent diffractive imaging to investigate the atomic displacements inside single grains of LLZO with various Al-doping concentrations, resulting in cubic, tetragonal, and cubic–tetragonal mixed structures. We observe coexisting domains of different crystallographic orientations in the tetragonal structure. We further show that Al doping leads to crystal defects such as dislocations and phase boundaries in the mixed- and cubic-phase grain. This study addresses the effect of Al doping on the nanoscale structure within individual grains of LLZO, which is informative for the future development of solid-state batteries.

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    Supporting Information

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    The Supporting Information is available free of charge at

    • SEM images, Ewald sphere, tetragonal peaks, histograms of Bragg angles and peak widths, diffraction patterns, reconstructed amplitude, single reconstructed displacement and strain fields of the particles in the three structural phases, cross sections of averaged displacement field, additional side views of the cross sections of the strain fields (PDF)

    • Movie S1: Reconstructed 3D displacement field in the cubic structure (AVI)

    • Movie S2: Reconstructed 3D strain field in the cubic structure (AVI)

    • Movie S3: Reconstructed 3D displacement field in the mixed structure (AVI)

    • Movie S4: Reconstructed 3D strain field in the mixed structure (AVI)

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    Cited By

    This article is cited by 11 publications.

    1. Zhenjiang Yu, Hongmei Shan, Yunlei Zhong, Xia Zhang, Guo Hong. Leveraging Advanced X-ray Imaging for Sustainable Battery Design. ACS Energy Letters 2022, 7 (9) , 3151-3176.
    2. C. Hyun Ryu, Hyein Lee, Heekwon Lee, Hang Ren. Learning from the Heterogeneity at Electrochemical Interfaces. The Journal of Physical Chemistry Letters 2022, 13 (33) , 7838-7846.
    3. Chao Zhu, Till Fuchs, Stefan A. L. Weber, Felix. H. Richter, Gunnar Glasser, Franjo Weber, Hans-Jürgen Butt, Jürgen Janek, Rüdiger Berger. Understanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques. Nature Communications 2023, 14 (1)
    4. Hyejeong Hyun, Daseul Ham, Su Yong Lee, Jongwoo Lim. Annealing‐Induced Dynamic Strain Evolution in Cycled High‐Ni Layered Oxides Revealing Latent Lattice Imperfections. Advanced Energy Materials 2023, 13 (36)
    5. Qing-Song Liu, Han-Wen An, Xu-Feng Wang, Fan-Peng Kong, Ye-Cai Sun, Yu-Xin Gong, Shuai-Feng Lou, Yi-Fan Shi, Nan Sun, Biao Deng, Jian Wang, Jia-Jun Wang. Effective transport network driven by tortuosity gradient enables high-electrochem-active solid-state batteries. National Science Review 2023, 10 (3)
    6. Yali Luo, Dingqian Dong, Jiacheng Zhou, Yuanjun Wang, Zihan Xue, Xue Jiang. Solid-state lithium-sulfur battery chemistries achieving excellent room-temperature cycle performance by high-quality Li7La3Zr2O12-based electrolyte. Journal of Alloys and Compounds 2023, 935 , 168112.
    7. Ji-Hwan Kim, Deok-Hye Park, Jae-Sung Jang, Jae-Hoon Shin, Min-Cheol Kim, Sung-Beom Kim, Sang-Hyun Moon, Seong-Nam Lee, Kyung-Won Park. High-performance free-standing hybrid solid electrolyte membrane combined with Li6.28Al0.24La3Zr2O12 and hexagonal-BN for all-solid-state lithium-based batteries. Chemical Engineering Journal 2022, 446 , 137035.
    8. Nan Sun, Yajie Song, Qingsong Liu, Wei Zhao, Fang Zhang, Liping Ren, Ming Chen, Zinan Zhou, Zihan Xu, Shuaifeng Lou, Fanpeng Kong, Jian Wang, Yujin Tong, Jiajun Wang. Surface‐to‐Bulk Synergistic Modification of Single Crystal Cathode Enables Stable Cycling of Sulfide‐Based All‐Solid‐State Batteries at 4.4 V. Advanced Energy Materials 2022, 12 (29)
    9. Chixia Tian, Feng Lin. Synchrotron X ‐ray Spectroscopy and Imaging for Metal Oxide Intercalation Cathode Chemistry. 2022, 343-373.
    10. Oleg Gorobtsov, Andrej Singer. Shear displacement gradient in X-ray Bragg coherent diffractive imaging. Journal of Synchrotron Radiation 2022, 29 (3) , 866-870.
    11. Jizhou Li, Yanshuai Hong, Hanfei Yan, Yong S. Chu, Piero Pianetta, Hong Li, Daniel Ratner, Xiaojing Huang, Xiqian Yu, Yijin Liu. Probing lattice defects in crystalline battery cathode using hard X-ray nanoprobe with data-driven modeling. Energy Storage Materials 2022, 45 , 647-655.

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