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High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

Author

Listed:
  • Fudong Han

    (University of Maryland)

  • Andrew S. Westover

    (Oak Ridge National Laboratory)

  • Jie Yue

    (University of Maryland)

  • Xiulin Fan

    (University of Maryland)

  • Fei Wang

    (University of Maryland)

  • Miaofang Chi

    (Oak Ridge National Laboratory)

  • Donovan N. Leonard

    (Oak Ridge National Laboratory)

  • Nancy J. Dudney

    (Oak Ridge National Laboratory)

  • Howard Wang

    (University of Maryland)

  • Chunsheng Wang

    (University of Maryland)

Abstract

Solid electrolytes (SEs) are widely considered as an ‘enabler’ of lithium anodes for high-energy batteries. However, recent reports demonstrate that the Li dendrite formation in Li7La3Zr2O12 (LLZO) and Li2S–P2S5 is actually much easier than that in liquid electrolytes of lithium batteries, by mechanisms that remain elusive. Here we illustrate the origin of the dendrite formation by monitoring the dynamic evolution of Li concentration profiles in three popular but representative SEs (LiPON, LLZO and amorphous Li3PS4) during lithium plating using time-resolved operando neutron depth profiling. Although no apparent changes in the lithium concentration in LiPON can be observed, we visualize the direct deposition of Li inside the bulk LLZO and Li3PS4. Our findings suggest the high electronic conductivity of LLZO and Li3PS4 is mostly responsible for dendrite formation in these SEs. Lowering the electronic conductivity, rather than further increasing the ionic conductivity of SEs, is therefore critical for the success of all-solid-state Li batteries.

Suggested Citation

  • Fudong Han & Andrew S. Westover & Jie Yue & Xiulin Fan & Fei Wang & Miaofang Chi & Donovan N. Leonard & Nancy J. Dudney & Howard Wang & Chunsheng Wang, 2019. "High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes," Nature Energy, Nature, vol. 4(3), pages 187-196, March.
    • Handle: RePEc:nat:natene:v:4:y:2019:i:3:d:10.1038_s41560-018-0312-z
    DOI: 10.1038/s41560-018-0312-z
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    Cited by:

    1. Sewon Kim & Ju-Sik Kim & Lincoln Miara & Yan Wang & Sung-Kyun Jung & Seong Yong Park & Zhen Song & Hyungsub Kim & Michael Badding & JaeMyung Chang & Victor Roev & Gabin Yoon & Ryounghee Kim & Jung-Hwa, 2022. "High-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    2. Ge Sun & Chenjie Lou & Boqian Yi & Wanqing Jia & Zhixuan Wei & Shiyu Yao & Ziheng Lu & Gang Chen & Zexiang Shen & Mingxue Tang & Fei Du, 2023. "Electrochemically induced crystalline-to-amorphization transformation in sodium samarium silicate solid electrolyte for long-lasting sodium metal batteries," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Chao Zhu & Till Fuchs & Stefan A. L. Weber & Felix. H. Richter & Gunnar Glasser & Franjo Weber & Hans-Jürgen Butt & Jürgen Janek & Rüdiger Berger, 2023. "Understanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    4. Xiaowei Chi & Ye Zhang & Fang Hao & Steven Kmiec & Hui Dong & Rong Xu & Kejie Zhao & Qing Ai & Tanguy Terlier & Liang Wang & Lihong Zhao & Liqun Guo & Jun Lou & Huolin L. Xin & Steve W. Martin & Yan Y, 2022. "An electrochemically stable homogeneous glassy electrolyte formed at room temperature for all-solid-state sodium batteries," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    5. Wesley Chang & Richard May & Michael Wang & Gunnar Thorsteinsson & Jeff Sakamoto & Lauren Marbella & Daniel Steingart, 2021. "Evolving contact mechanics and microstructure formation dynamics of the lithium metal-Li7La3Zr2O12 interface," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    6. Li Huang & Jian Gao & Zhijie Bi & Ning Zhao & Jipeng Wu & Qiu Fang & Xuefeng Wang & Yong Wan & Xiangxin Guo, 2022. "Comparative Study of Stability against Moisture for Solid Garnet Electrolytes with Different Dopants," Energies, MDPI, vol. 15(9), pages 1-9, April.
    7. Han Su & Yu Zhong & Changhong Wang & Yu Liu & Yang Hu & Jingru Li & Minkang Wang & Longan Jiao & Ningning Zhou & Bing Xiao & Xiuli Wang & Xueliang Sun & Jiangping Tu, 2024. "Deciphering the critical role of interstitial volume in glassy sulfide superionic conductors," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    8. Dewu Zeng & Jingming Yao & Long Zhang & Ruonan Xu & Shaojie Wang & Xinlin Yan & Chuang Yu & Lin Wang, 2022. "Promoting favorable interfacial properties in lithium-based batteries using chlorine-rich sulfide inorganic solid-state electrolytes," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    9. V. Reisecker & F. Flatscher & L. Porz & C. Fincher & J. Todt & I. Hanghofer & V. Hennige & M. Linares-Moreau & P. Falcaro & S. Ganschow & S. Wenner & Y.-M. Chiang & J. Keckes & J. Fleig & D. Rettenwan, 2023. "Effect of pulse-current-based protocols on the lithium dendrite formation and evolution in all-solid-state batteries," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    10. Ziteng Liang & Yuxuan Xiang & Kangjun Wang & Jianping Zhu & Yanting Jin & Hongchun Wang & Bizhu Zheng & Zirong Chen & Mingming Tao & Xiangsi Liu & Yuqi Wu & Riqiang Fu & Chunsheng Wang & Martin Winter, 2023. "Understanding the failure process of sulfide-based all-solid-state lithium batteries via operando nuclear magnetic resonance spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    11. Zhenyou Song & Tengrui Wang & Hua Yang & Wang Hay Kan & Yuwei Chen & Qian Yu & Likuo Wang & Yini Zhang & Yiming Dai & Huaican Chen & Wen Yin & Takashi Honda & Maxim Avdeev & Henghui Xu & Jiwei Ma & Yu, 2024. "Promoting high-voltage stability through local lattice distortion of halide solid electrolytes," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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