IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-37313-2.html
   My bibliography  Save this article

Atomic-scale study clarifying the role of space-charge layers in a Li-ion-conducting solid electrolyte

Author

Listed:
  • Zhenqi Gu

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Jiale Ma

    (University of Science and Technology of China)

  • Feng Zhu

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Ting Liu

    (Tsinghua University
    Foshan (Southern China) Institute for New Materials)

  • Kai Wang

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Ce-Wen Nan

    (Tsinghua University)

  • Zhenyu Li

    (University of Science and Technology of China)

  • Cheng Ma

    (University of Science and Technology of China
    University of Science and Technology of China
    National Synchrotron Radiation Laboratory)

Abstract

Space-charge layers are frequently believed responsible for the large resistance of different interfaces in all-solid-state Li batteries. However, such propositions are based on the presumed existence of a Li-deficient space-charge layer with insufficient charge carriers, instead of a comprehensive investigation on the atomic configuration and its ion transport behavior. Consequently, the real influence of space-charge layers remains elusive. Here, we clarify the role of space-charge layers in Li0.33La0.56TiO3, a prototype solid electrolyte with large grain-boundary resistance, through a combined experimental and computational study at the atomic scale. In contrast to previous speculations, we do not observe the Li-deficient space-charge layers commonly believed to result in large resistance. Instead, the actual space-charge layers are Li-excess; accommodating the additional Li+ at the 3c interstitials, such space-charge layers allow for rather efficient ion transport. With the space-charge layers excluded from the potential bottlenecks, we identify the Li-depleted grain-boundary cores as the major cause for the large grain-boundary resistance in Li0.33La0.56TiO3.

Suggested Citation

  • Zhenqi Gu & Jiale Ma & Feng Zhu & Ting Liu & Kai Wang & Ce-Wen Nan & Zhenyu Li & Cheng Ma, 2023. "Atomic-scale study clarifying the role of space-charge layers in a Li-ion-conducting solid electrolyte," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37313-2
    DOI: 10.1038/s41467-023-37313-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-37313-2
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-023-37313-2?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Jürgen Janek & Wolfgang G. Zeier, 2016. "A solid future for battery development," Nature Energy, Nature, vol. 1(9), pages 1-4, September.
    2. Longlong Wang & Ruicong Xie & Bingbing Chen & Xinrun Yu & Jun Ma & Chao Li & Zhiwei Hu & Xingwei Sun & Chengjun Xu & Shanmu Dong & Ting-Shan Chan & Jun Luo & Guanglei Cui & Liquan Chen, 2020. "In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    3. Feng Zhu & Md Shafiqul Islam & Lin Zhou & Zhenqi Gu & Ting Liu & Xinchao Wang & Jun Luo & Ce-Wen Nan & Yifei Mo & Cheng Ma, 2020. "Single-atom-layer traps in a solid electrolyte for lithium batteries," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Lv Hu & Jinzhu Wang & Kai Wang & Zhenqi Gu & Zhiwei Xi & Hui Li & Fang Chen & Youxi Wang & Zhenyu Li & Cheng Ma, 2023. "A cost-effective, ionically conductive and compressible oxychloride solid-state electrolyte for stable all-solid-state lithium-based batteries," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Sebastian Scheld, Walter & Charlotte Hoff, Linda & Vedder, Christian & Stollenwerk, Jochen & Grüner, Daniel & Rosen, Melanie & Lobe, Sandra & Ihrig, Martin & Seok, Ah–Ram & Finsterbusch, Martin & Uhle, 2023. "Enabling metal substrates for garnet-based composite cathodes by laser sintering," Applied Energy, Elsevier, vol. 345(C).
    3. Shuo Wang & Jiamin Fu & Yunsheng Liu & Ramanuja Srinivasan Saravanan & Jing Luo & Sixu Deng & Tsun-Kong Sham & Xueliang Sun & Yifei Mo, 2023. "Design principles for sodium superionic conductors," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Bornmann, Lutz & Haunschild, Robin, 2022. "Empirical analysis of recent temporal dynamics of research fields: Annual publications in chemistry and related areas as an example," Journal of Informetrics, Elsevier, vol. 16(2).
    5. Nian Zhang & Guoxi Ren & Lili Li & Zhi Wang & Pengfei Yu & Xiaobao Li & Jing Zhou & Hui Zhang & Linjuan Zhang & Zhi Liu & Xiaosong Liu, 2024. "Dynamical evolution of CO2 and H2O on garnet electrolyte elucidated by ambient pressure X-ray spectroscopies," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    6. Dong-Su Ko & Sewon Kim & Sangjun Lee & Gabin Yoon & Daeho Kim & ChaeHo Shin & Dongmin Kim & Jaewoo Lee & Soohwan Sul & Dong-Jin Yun & Changhoon Jung, 2025. "Mechanism of stable lithium plating and stripping in a metal-interlayer-inserted anode-less solid-state lithium metal battery," Nature Communications, Nature, vol. 16(1), pages 1-13, December.
    7. Coester, Andreas & Hofkes, Marjan W. & Papyrakis, Elissaios, 2020. "Economic analysis of batteries: Impact on security of electricity supply and renewable energy expansion in Germany," Applied Energy, Elsevier, vol. 275(C).
    8. Xinxin Wang & Jingjing Chen & Dajian Wang & Zhiyong Mao, 2021. "Improving the alkali metal electrode/inorganic solid electrolyte contact via room-temperature ultrasound solid welding," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    9. Bowen Zhang & Botao Yuan & Xin Yan & Xiao Han & Jiawei Zhang & Huifeng Tan & Changuo Wang & Pengfei Yan & Huajian Gao & Yuanpeng Liu, 2025. "Atomic mechanism of lithium dendrite penetration in solid electrolytes," Nature Communications, Nature, vol. 16(1), pages 1-13, 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.
    12. Xiangkun Kong & Run Gu & Zongzi Jin & Lei Zhang & Chi Zhang & Wenyi Xiang & Cui Li & Kang Zhu & Yifan Xu & Huang Huang & Xiaoye Liu & Ranran Peng & Chengwei Wang, 2024. "Maximizing interface stability in all-solid-state lithium batteries through entropy stabilization and fast kinetics," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    13. Mergo Mbeya, Karrick & Damay, Nicolas & Friedrich, Guy & Forgez, Christophe & Juston, Maxime, 2021. "Off-line method to determine the electrode balancing of Li-ion batteries," Mathematics and Computers in Simulation (MATCOM), Elsevier, vol. 183(C), pages 34-47.
    14. Qidi Wang & Yunan Zhou & Xuelong Wang & Hao Guo & Shuiping Gong & Zhenpeng Yao & Fangting Wu & Jianlin Wang & Swapna Ganapathy & Xuedong Bai & Baohua Li & Chenglong Zhao & Jürgen Janek & Marnix Wagema, 2024. "Designing lithium halide solid electrolytes," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    15. In-Gyu Jang & Chung-Seong Lee & Sung-Ho Hwang, 2021. "Energy Optimization of Electric Vehicles by Distributing Driving Power Considering System State Changes," Energies, MDPI, vol. 14(3), pages 1-18, January.
    16. Mouhamad S. Diallo & Tan Shi & Yaqian Zhang & Xinxing Peng & Imtiaz Shozib & Yan Wang & Lincoln J. Miara & Mary C. Scott & Qingsong Howard Tu & Gerbrand Ceder, 2024. "Effect of solid-electrolyte pellet density on failure of solid-state batteries," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    17. Zhimin Chen & Tao Du & N. M. Anoop Krishnan & Yuanzheng Yue & Morten M. Smedskjaer, 2025. "Disorder-induced enhancement of lithium-ion transport in solid-state electrolytes," Nature Communications, Nature, vol. 16(1), pages 1-14, December.
    18. Robert Bock & Morten Onsrud & Håvard Karoliussen & Bruno G. Pollet & Frode Seland & Odne S. Burheim, 2020. "Thermal Gradients with Sintered Solid State Electrolytes in Lithium-Ion Batteries," Energies, MDPI, vol. 13(1), pages 1-13, January.
    19. Shumin Zhang & Feipeng Zhao & Jiatang Chen & Jiamin Fu & Jing Luo & Sandamini H. Alahakoon & Lo-Yueh Chang & Renfei Feng & Mohsen Shakouri & Jianwen Liang & Yang Zhao & Xiaona Li & Le He & Yining Huan, 2023. "A family of oxychloride amorphous solid electrolytes for long-cycling all-solid-state lithium batteries," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    20. Jack Aspinall & Krishnakanth Sada & Hua Guo & Souhardh Kotakadi & Sudarshan Narayanan & Yvonne Chart & Ben Jagger & Emily Milan & Laurence Brassart & David Armstrong & Mauro Pasta, 2024. "The impact of magnesium content on lithium-magnesium alloy electrode performance with argyrodite solid electrolyte," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37313-2. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.