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Stabilizing the Cathode/Electrolyte Interface Using a Dry-Processed Lithium Titanate Coating for All-Solid-State Batteries
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    Stabilizing the Cathode/Electrolyte Interface Using a Dry-Processed Lithium Titanate Coating for All-Solid-State Batteries
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    • Rajendra S. Negi
      Rajendra S. Negi
      Center for Materials Research (LaMa) Justus Liebig University Giessen, Heinrich-Buff-Ring 16, D-35392 Giessen, Germany
    • Philip Minnmann
      Philip Minnmann
      Institute of Physical Chemistry, Justus Liebig University Giessen, Heinrich-Buff-Ring 17, D-35392 Giessen, Germany
    • Ruijun Pan
      Ruijun Pan
      Institute of Physical Chemistry, Justus Liebig University Giessen, Heinrich-Buff-Ring 17, D-35392 Giessen, Germany
      More by Ruijun Pan
    • Shamail Ahmed
      Shamail Ahmed
      Materials Science Centre and Faculty of Physics, Philipps University Marburg, Hans-Meerwein-Strasse 6, 35043 Marburg, Germany
    • Marcel J. Herzog
      Marcel J. Herzog
      Evonik Operations GmbH, Rodenbacher Chaussee 4, 63457 Hanau, Germany
    • Kerstin Volz
      Kerstin Volz
      Materials Science Centre and Faculty of Physics, Philipps University Marburg, Hans-Meerwein-Strasse 6, 35043 Marburg, Germany
      More by Kerstin Volz
    • Ryo Takata
      Ryo Takata
      Evonik Operations GmbH, Rodenbacher Chaussee 4, 63457 Hanau, Germany
      More by Ryo Takata
    • Franz Schmidt
      Franz Schmidt
      Evonik Operations GmbH, Rodenbacher Chaussee 4, 63457 Hanau, Germany
    • Jürgen Janek
      Jürgen Janek
      Center for Materials Research (LaMa) Justus Liebig University Giessen, Heinrich-Buff-Ring 16, D-35392 Giessen, Germany
      Institute of Physical Chemistry, Justus Liebig University Giessen, Heinrich-Buff-Ring 17, D-35392 Giessen, Germany
    • Matthias T. Elm*
      Matthias T. Elm
      Center for Materials Research (LaMa) Justus Liebig University Giessen, Heinrich-Buff-Ring 16, D-35392 Giessen, Germany
      Institute of Physical Chemistry, Justus Liebig University Giessen, Heinrich-Buff-Ring 17, D-35392 Giessen, Germany
      Institute of Experimental Physics I, Justus Liebig University Giessen, Heinrich-Buff-Ring 16, D-35392 Giessen, Germany
      *Email: [email protected]
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    Chemistry of Materials

    Cite this: Chem. Mater. 2021, 33, 17, 6713–6723
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.1c01123
    Published August 20, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society

    Abstract

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    Considering the high theoretical energy density and improved safety, thiophosphate-based all-solid-state batteries (ASSBs) have become one of the most promising candidates for next-generation energy storage systems. However, the intrinsic electrochemical instability of thiophosphate-based solid electrolytes in contact with oxide-based cathodes results in rapid capacity fading and has driven the need of protective cathode coatings. In this work, for the first time, a fumed lithium titanate (LTO) powder-based coating has been applied to Ni-rich oxide-based cathode active material (CAM) using a newly developed dry-coating process. The LTO cathode coating has been tested in thiophosphate-based ASSBs. It exhibits a significantly improved C-rate performance along with superior long-term cycling stability. The improved electrochemical performance is attributed to a reduced interfacial resistance between coated cathode and solid electrolyte as deduced from in-depth electrochemical impedance spectroscopy analysis. These results open up a new, facile dry-coating route to fabricate effective protective CAM coatings to enable long-life ASSBs. This nondestructive coating process with no post-heat-treatment approach is expected to simplify the coating process for a wide range of coatings and cathode materials, resulting in much improved cathode/electrolyte interfacial stability and electrochemical performance of ASSBs.

    Copyright © 2021 The Authors. Published by American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.1c01123.

    • SEM image and XRD pattern of the fumed LTO coating, SPED virtual dark-field (VDF) image of an NCM primary particle, Coulombic efficiency (CE) plot at 0.25C and first-cycle charge/discharge voltage profile of P-NCM- and LTO-2 wt %-based cells, equivalent circuit used for fitting, table of obtained fitting parameters, and Bode plots after the 1st and 100th cycles of P-NCM and LTO-2 wt % (PDF)

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    Cited By

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    This article is cited by 13 publications.

    1. Miguel Wiche, Yuriy Yusim, Kilian Vettori, Raffael Ruess, Anja Henss, Matthias T. Elm. State of Charge-Dependent Impedance Spectroscopy as a Helpful Tool to Identify Reasons for Fast Capacity Fading in All-Solid-State Batteries. ACS Applied Materials & Interfaces 2024, 16 (3) , 3253-3259. https://doi.org/10.1021/acsami.3c13160
    2. Subhajit Sarkar, Venkataraman Thangadurai. Critical Current Densities for High-Performance All-Solid-State Li-Metal Batteries: Fundamentals, Mechanisms, Interfaces, Materials, and Applications. ACS Energy Letters 2022, 7 (4) , 1492-1527. https://doi.org/10.1021/acsenergylett.2c00003
    3. Alexander Kraytsberg, Yair Ein-Eli. Recent Developments in the Field of Sulfide Ceramic Solid‐State Electrolytes. Energy Technology 2023, 26 , 2201291. https://doi.org/10.1002/ente.202201291
    4. Jeongheon Kim, Min Ji Kim, Jaeik Kim, Jin Woong Lee, Joonhyeok Park, Sung Eun Wang, Seungwoo Lee, Yun Chan Kang, Ungyu Paik, Dae Soo Jung, Taeseup Song. High‐Performance All‐Solid‐State Batteries Enabled by Intimate Interfacial Contact Between the Cathode and Sulfide‐Based Solid Electrolytes. Advanced Functional Materials 2023, 33 (12) , 2211355. https://doi.org/10.1002/adfm.202211355
    5. Zhen Zeng, Jun Cheng, Yuanyuan Li, Hongqiang Zhang, Deping Li, Hongbin Liu, Fengjun Ji, Qing Sun, Lijie Ci. Composite cathode for all-solid-state lithium batteries: Progress and perspective. Materials Today Physics 2023, 32 , 101009. https://doi.org/10.1016/j.mtphys.2023.101009
    6. Theodoor A. Hendriks, Martin A. Lange, Ellen M. Kiens, Christoph Baeumer, Wolfgang G. Zeier. Balancing Partial Ionic and Electronic Transport for Optimized Cathode Utilization of High‐Voltage LiMn 2 O 4 /Li 3 InCl 6 Solid‐State Batteries. Batteries & Supercaps 2023, 7 https://doi.org/10.1002/batt.202200544
    7. Jun Chen, Hongyi Chen, Yu Mei, Shu Zhang, Lianshan Ni, Xu Gao, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji. Polarly modulated solvent strategy for high-voltage cathode materials. Chemical Engineering Journal 2022, 450 , 138318. https://doi.org/10.1016/j.cej.2022.138318
    8. Matthias T. Elm. Surface engineering of oxide nanostructures for efficient energy technologies. 2022, 1-4. https://doi.org/10.1109/IMFEDK56875.2022.9975419
    9. Jie Shi, Zhihui Ma, Kun Han, Qi Wan, Di Wu, Xuanhui Qu, Ping Li. Coupling novel Li 7 TaO 6 surface buffering with bulk Ta-doping to achieve long-life sulfide-based all-solid-state lithium batteries. Journal of Materials Chemistry A 2022, 10 (40) , 21336-21348. https://doi.org/10.1039/D2TA06703J
    10. Philip Minnmann, Florian Strauss, Anja Bielefeld, Raffael Ruess, Philipp Adelhelm, Simon Burkhardt, Sören L. Dreyer, Enrico Trevisanello, Helmut Ehrenberg, Torsten Brezesinski, Felix H. Richter, Jürgen Janek. Designing Cathodes and Cathode Active Materials for Solid‐State Batteries. Advanced Energy Materials 2022, 12 (35) , 2201425. https://doi.org/10.1002/aenm.202201425
    11. Sahin Cangaz, Felix Hippauf, Ryo Takata, Franz Schmidt, Susanne Dörfler, Stefan Kaskel. Surface Functionalization of LiNi 7.0 Co 0.15 Mn 0.15 O 2 with Fumed Li 2 ZrO 3 via a Cost‐Effective Dry‐Coating Process for Enhanced Performance in Solid‐State Batteries. Batteries & Supercaps 2022, 5 (9) https://doi.org/10.1002/batt.202200100
    12. Heyang Jiang, Xiaowei Mu, Hui Pan, Menghang Zhang, Ping He, Haoshen Zhou. Insights into interfacial chemistry of Ni-rich cathodes and sulphide-based electrolytes in all-solid-state lithium batteries. Chemical Communications 2022, 58 (40) , 5924-5947. https://doi.org/10.1039/D2CC01220K
    13. Rajendra S. Negi, Yuriy Yusim, Ruijun Pan, Shamail Ahmed, Kerstin Volz, Ryo Takata, Franz Schmidt, Anja Henss, Matthias T. Elm. A Dry‐Processed Al 2 O 3 /LiAlO 2 Coating for Stabilizing the Cathode/Electrolyte Interface in High‐Ni NCM‐Based All‐Solid‐State Batteries. Advanced Materials Interfaces 2022, 9 (8) , 2101428. https://doi.org/10.1002/admi.202101428

    Chemistry of Materials

    Cite this: Chem. Mater. 2021, 33, 17, 6713–6723
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.1c01123
    Published August 20, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society

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