IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v16y2025i1d10.1038_s41467-025-56662-8.html
   My bibliography  Save this article

Non-local interactions determine local structure and lithium diffusion in solid electrolytes

Author

Listed:
  • Swastika Banerjee

    (Indian Institute of Technology
    University of Luxembourg)

  • Alexandre Tkatchenko

    (University of Luxembourg)

Abstract

Solid-state batteries, in which solid electrolytes (SEs) replace their liquid alternatives, promise high energy density and safety. However, understanding the relation between SE composition and properties, stemming from intricate interactions among constituent sublattices that involve non-local electronic and nuclear dynamics, remains a critical and unsolved challenge. Here, we evaluate electronic structure methods and demonstrate that a density-functional approach incorporating non-local and many-body effects in exchange-correlation interactions provides predictive results for the local structure and diffusion properties of SEs. Focusing on argyrodite SEs (Li6±xM1±yS5±zXn, LMSX; M = P, Ge, Si, Sn; X = Cl, Br, I), we explore their compositional landscape as a test case. The employed HSE06+MBDNL method unveils how the S/X site disorder dictates the diffusion of lithium by controlling the number and length of the diffusion pathways. Additionally, non-local exchange and van der Waals interactions precisely modulate the coupling between the framework lattice and mobile lithium ions, thereby influencing the migration barrier. Consequently, the interplay of non-local electronic interactions in the predictive design of Li-solid electrolytes – and likely many other functional materials – is emphasized.

Suggested Citation

  • Swastika Banerjee & Alexandre Tkatchenko, 2025. "Non-local interactions determine local structure and lithium diffusion in solid electrolytes," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-56662-8
    DOI: 10.1038/s41467-025-56662-8
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-025-56662-8
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-025-56662-8?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. M. Armand & J.-M. Tarascon, 2008. "Building better batteries," Nature, Nature, vol. 451(7179), pages 652-657, February.
    2. Ying Zhang & Xingfeng He & Zhiqian Chen & Qiang Bai & Adelaide M. Nolan & Charles A. Roberts & Debasish Banerjee & Tomoya Matsunaga & Yifei Mo & Chen Ling, 2019. "Unsupervised discovery of solid-state lithium ion conductors," Nature Communications, Nature, vol. 10(1), pages 1-7, 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. Li, Qun & Yin, Longwei & Ma, Jingyun & Li, Zhaoqiang & Zhang, Zhiwei & Chen, Ailian & Li, Caixia, 2015. "Mesoporous silicon/carbon hybrids with ordered pore channel retention and tunable carbon incorporated content as high performance anode materials for lithium-ion batteries," Energy, Elsevier, vol. 85(C), pages 159-166.
    2. Chen, Dongfang & Pan, Lyuming & Pei, Pucheng & Huang, Shangwei & Ren, Peng & Song, Xin, 2021. "Carbon-coated oxygen vacancies-rich Co3O4 nanoarrays grow on nickel foam as efficient bifunctional electrocatalysts for rechargeable zinc-air batteries," Energy, Elsevier, vol. 224(C).
    3. Zhi Chang & Huijun Yang & Xingyu Zhu & Ping He & Haoshen Zhou, 2022. "A stable quasi-solid electrolyte improves the safe operation of highly efficient lithium-metal pouch cells in harsh environments," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    4. Entwistle, Jake & Ge, Ruihuan & Pardikar, Kunal & Smith, Rachel & Cumming, Denis, 2022. "Carbon binder domain networks and electrical conductivity in lithium-ion battery electrodes: A critical review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 166(C).
    5. Yohwan Choi & Hongseok Kim, 2016. "Optimal Scheduling of Energy Storage System for Self-Sustainable Base Station Operation Considering Battery Wear-Out Cost," Energies, MDPI, vol. 9(6), pages 1-19, June.
    6. Lili Zhang & Ning Zhang & Huishan Shang & Zhiyi Sun & Zihao Wei & Jingtao Wang & Yuanting Lei & Xiaochen Wang & Dan Wang & Yafei Zhao & Zhongti Sun & Fang Zhang & Xu Xiang & Bing Zhang & Wenxing Chen, 2024. "High-density asymmetric iron dual-atom sites for efficient and stable electrochemical water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    7. Chao Wang & Ming Liu & Michel Thijs & Frans G. B. Ooms & Swapna Ganapathy & Marnix Wagemaker, 2021. "High dielectric barium titanate porous scaffold for efficient Li metal cycling in anode-free cells," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    8. Navaratnarajah Kuganathan & Efstratia N. Sgourou & Yerassimos Panayiotatos & Alexander Chroneos, 2019. "Defect Process, Dopant Behaviour and Li Ion Mobility in the Li 2 MnO 3 Cathode Material," Energies, MDPI, vol. 12(7), pages 1-11, April.
    9. Jiang, Yunfeng & Xia, Bing & Zhao, Xin & Nguyen, Truong & Mi, Chris & de Callafon, Raymond A., 2017. "Data-based fractional differential models for non-linear dynamic modeling of a lithium-ion battery," Energy, Elsevier, vol. 135(C), pages 171-181.
    10. Lu Zhang & Xiaohua Zhang & Guiying Tian & Qinghua Zhang & Michael Knapp & Helmut Ehrenberg & Gang Chen & Zexiang Shen & Guochun Yang & Lin Gu & Fei Du, 2020. "Lithium lanthanum titanate perovskite as an anode for lithium ion batteries," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    11. Runlin Wang & Haozhe Zhang & Qiyu Liu & Fu Liu & Xile Han & Xiaoqing Liu & Kaiwei Li & Gaozhi Xiao & Jacques Albert & Xihong Lu & Tuan Guo, 2022. "Operando monitoring of ion activities in aqueous batteries with plasmonic fiber-optic sensors," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    12. Wu, Xiaoyu & Li, Songmei & Wang, Bo & Liu, Jianhua & Yu, Mei, 2020. "Free-standing 3D network-like cathode based on biomass-derived N-doped carbon/graphene/g-C3N4 hybrid ultrathin sheets as sulfur host for high-rate Li-S battery," Renewable Energy, Elsevier, vol. 158(C), pages 509-519.
    13. 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.
    14. Siwu Li & Haolin Zhu & Yuan Liu & Zhilong Han & Linfeng Peng & Shuping Li & Chuang Yu & Shijie Cheng & Jia Xie, 2022. "Codoped porous carbon nanofibres as a potassium metal host for nonaqueous K-ion batteries," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    15. Odoom-Wubah, Tareque & Rubio, Saúl & Tirado, José L. & Ortiz, Gregorio F. & Akoi, Bior James & Huang, Jiale & Li, Qingbiao, 2020. "Waste Pd/Fish-Collagen as anode for energy storage," Renewable and Sustainable Energy Reviews, Elsevier, vol. 131(C).
    16. Arjun K. Thapa & Abhinav C. Nouduri & Mohammed Mohiuddin & Hari Prasad Reddy Kannapu & Lihui Bai & Hui Wang & Mahendra K. Sunkara, 2024. "Recycling and Reuse of Mn-Based Spinel Electrode from Spent Lithium-Ion Batteries," Energies, MDPI, vol. 17(16), pages 1-13, August.
    17. Min Xu & Jinjun Qu & Mai Li, 2022. "National Policies, Recent Research Hotspots, and Application of Sustainable Energy: Case of China, USA, and European Countries," Sustainability, MDPI, vol. 14(16), pages 1-30, August.
    18. Freitas Gomes, Icaro Silvestre & Perez, Yannick & Suomalainen, Emilia, 2020. "Coupling small batteries and PV generation: A review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 126(C).
    19. Zhi Chang & Huijun Yang & Anqiang Pan & Ping He & Haoshen Zhou, 2022. "An improved 9 micron thick separator for a 350 Wh/kg lithium metal rechargeable pouch cell," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    20. Tao Cheng & Zhongtao Ma & Run Gu & Riming Chen & Yingchun Lyu & Anmin Nie & Bingkun Guo, 2018. "Cracks Formation in Lithium-Rich Cathode Materials for Lithium-Ion Batteries during the Electrochemical Process," Energies, MDPI, vol. 11(10), pages 1-10, October.

    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:16:y:2025:i:1:d:10.1038_s41467-025-56662-8. 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.