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Improved Lithium-Ion Transport Within the LiNi0.8Co0.15Al0.05O2 Secondary Cathode Particles Through a Template-Assisted Synthesis Route

  • Buse Bulut Kopuklu
    Buse Bulut Kopuklu
    Faculty of Engineering and Natural Sciences (FENS), Sabancı University, Üniversite Caddesi 27, 34956 Istanbul, Turkey
  • Aurora Gomez-Martin*
    Aurora Gomez-Martin
    MEET Battery Research Center, Institute of Physical Chemistry, University of Münster, Corrensstraße 46, 48149 Münster, Germany
    *Email: [email protected]. Phone:+49 251 83-36754.
  • Martin Winter
    Martin Winter
    MEET Battery Research Center, Institute of Physical Chemistry, University of Münster, Corrensstraße 46, 48149 Münster, Germany
    Helmholtz Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
  • Tobias Placke
    Tobias Placke
    MEET Battery Research Center, Institute of Physical Chemistry, University of Münster, Corrensstraße 46, 48149 Münster, Germany
  • Richard Schmuch
    Richard Schmuch
    MEET Battery Research Center, Institute of Physical Chemistry, University of Münster, Corrensstraße 46, 48149 Münster, Germany
  • Selmiye Alkan Gursel
    Selmiye Alkan Gursel
    Faculty of Engineering and Natural Sciences (FENS), Sabancı University, Üniversite Caddesi 27, 34956 Istanbul, Turkey
    Sabancı University SUNUM Nanotechnology Research Centre, Üniversite Caddesi 27, 34956 Istanbul, Turkey
  • , and 
  • Alp Yurum*
    Alp Yurum
    Sabancı University SUNUM Nanotechnology Research Centre, Üniversite Caddesi 27, 34956 Istanbul, Turkey
    *Email: [email protected]. Phone: +90(216) 483 90 00-2404.
    More by Alp Yurum
Cite this: ACS Sustainable Chem. Eng. 2021, 9, 37, 12560–12574
Publication Date (Web):September 3, 2021
https://doi.org/10.1021/acssuschemeng.1c03179
Copyright © 2021 American Chemical Society

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    Abstract

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    Herein, we report a sacrificial carbon fiber (CF) template-assisted synthesis of LiNi0.8Co0.15Al0.05O2 (C-NCA) by the Pechini method. An anisotropic primary particle morphology with an interconnected microstructure is obtained, originating from local overheating and oxygen-deficient zones induced by combustion of the CFs during high-temperature lithiation. Moreover, the particles assembled around the CFs demonstrated denser packing compared to the reference bare NCA (B-NCA) synthetized in the absence of the CF template. The anisotropic surfaces facilitate ion transport and stabilize the structure for high voltage and temperature operation. C-NCA||Li metal cells exhibit a reversible capacity of 106 mA h g–1 at 10 C and are able to retain 96% of their initial capacity as the C-rate is reverted to 0.1 C. The state of health of C-NCA||graphite full cells remains at 70% after 200 cycles at 0.33 C within 2.8–4.3 V. The results outperform the B-NCA cell, exhibiting a significant loss over 66 cycles while delivering only 50% of its initial capacity. The synthesis method allows for a straightforward route for tailoring the particle size, shape, and crystallinity, enabling the development of stable nickel-rich cathode materials, even at an upper cutoff voltage of 4.5 V or an operating temperature of 60 °C.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.1c03179.

    • XRD patterns of the pre-calcined NCA precursors; relative intensities of the XRD reflections of the NCA powder samples; XPS Ni2p3/2 fitting spectra of the NCA powder samples; detailed O 1s and C 1s XPS graphs; comparison of the deliverable specific capacities of the NCA||Li metal cells; N2 adsorption–desorption isotherms and calculated BJH pore size distributions of NCA powders; GITT curves; detailed electrochemical results at 60 °C; and post mortem SEM/EDX of the graphite electrodes (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Buse Bulut Kopuklu, Ekin Esen, Aurora Gomez-Martin, Martin Winter, Tobias Placke, Richard Schmuch, Selmiye Alkan Gursel, Alp Yurum. Practical Implementation of Magnetite-Based Conversion-Type Negative Electrodes via Electrochemical Prelithiation. ACS Applied Materials & Interfaces 2022, 14 (30) , 34665-34677. https://doi.org/10.1021/acsami.2c06328
    2. Sweta Mariam George, S. Sampath, Aninda J. Bhattacharyya. A Self‐Standing Flexible Gel Polymer Electrolyte for Dendrite‐Free Lithium‐Metal Batteries. Batteries & Supercaps 2022, 5 (11) https://doi.org/10.1002/batt.202200252

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