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Synthesis and Postprocessing of Single-Crystalline LiNi0.8Co0.15Al0.05O2 for Solid-State Lithium-Ion Batteries with High Capacity and Long Cycling Stability

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    Synthesis and Postprocessing of Single-Crystalline LiNi0.8Co0.15Al0.05O2 for Solid-State Lithium-Ion Batteries with High Capacity and Long Cycling Stability
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    • Roberto Fantin
      Roberto Fantin
      Center for Materials Research and Institute of Physical Chemistry, Justus-Liebig-University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany
      More by Roberto Fantin
    • Enrico Trevisanello
      Enrico Trevisanello
      Center for Materials Research and Institute of Physical Chemistry, Justus-Liebig-University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany
      More by Enrico Trevisanello
    • Raffael Ruess*
      Raffael Ruess
      Center for Materials Research and Institute of Physical Chemistry, Justus-Liebig-University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany
      *(R.R.) Email [email protected]
      More by Raffael Ruess
    • Anuj Pokle
      Anuj Pokle
      Materials Science Center and Department of Physics, Philipps University Marburg, Hans-Meerwein-Straße 6, 35043 Marburg, Germany
      More by Anuj Pokle
      Orcidhttp://orcid.org/0000-0002-7457-8839
    • Gioele Conforto
      Gioele Conforto
      Center for Materials Research and Institute of Physical Chemistry, Justus-Liebig-University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany
      More by Gioele Conforto
    • Felix H. Richter
      Felix H. Richter
      Center for Materials Research and Institute of Physical Chemistry, Justus-Liebig-University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany
      More by Felix H. Richter
    • Kerstin Volz
      Kerstin Volz
      Materials Science Center and Department of Physics, Philipps University Marburg, Hans-Meerwein-Straße 6, 35043 Marburg, Germany
      More by Kerstin Volz
    • Jürgen Janek*
      Jürgen Janek
      Center for Materials Research and Institute of Physical Chemistry, Justus-Liebig-University Giessen, Heinrich-Buff-Ring 17, 35392 Giessen, Germany
      *(J.J.) Email [email protected]
      More by Jürgen Janek
      Orcidhttp://orcid.org/0000-0002-9221-4756
    Other Access OptionsSupporting Information (1)

    Chemistry of Materials

    Cite this: Chem. Mater. 2021, 33, 7, 2624–2634
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    https://doi.org/10.1021/acs.chemmater.1c00471
    Published March 17, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
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    Abstract

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    The application of nickel-rich LiNixCoyAlzO2 (NCA) cathode materials in solid-state lithium-ion batteries (SSBs) promises significant improvements in energy density, stability, and safety over traditional lithium-ion batteries with liquid electrolytes. However, low active mass utilization and strong capacity fading associated with degradation of the cathode often limit SSB applicability. The use of single-crystalline cathode active materials (CAMs) instead of spherical polycrystalline materials optimized for performance in lithium-ion batteries recently emerged as a promising approach in the field of SSBs to overcome this issue. In this work, single-crystalline LiNi0.8Co0.15Al0.05O2 (SC-NCA) is investigated as cathode active material for SSBs. It is shown that appropriate postprocessing of as-synthesized materials, which consists of washing steps with either water or ethanol followed by postannealing at different temperatures, is key to achieve high-performance cathodes. X-ray powder diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, and scanning transmission electron microscopy are employed to characterize the effect of postprocessing on structure and morphology. The postprocessing procedure was tailored to mitigate detrimental side reactions that result in structural damage of the SC-NCA, while retaining the beneficial effects of deagglomeration and control of surface impurities. Washing with ethanol and subsequent postannealing at 750 °C allowed us to obtain SC-NCA materials that perform well in SSB cells with Li6PS5Cl as solid electrolyte, enabling a high initial discharge capacity of 174 mAh g–1, good rate performance, and high capacity retention (94% after 200 cycles) at 25 °C.

    Copyright © 2021 The Authors. Published by American Chemical Society

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.1c00471.

    • SEM images and XRD measurements of pristine and post-treated SC-NCA, FIB-SEM images of SSB cathodes, impedance data of SSB cells, comparison of small and large SC-NCA (PDF)

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    Cited By

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    This article is cited by 46 publications.

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    Chemistry of Materials

    Cite this: Chem. Mater. 2021, 33, 7, 2624–2634
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.1c00471
    Published March 17, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
    Request reuse permissions

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