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Transition Metal Migration Can Facilitate Ionic Diffusion in Defect Garnet-Based Intercalation Electrodes

  • Nicholas H. Bashian
    Nicholas H. Bashian
    Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States
  • Samantha Abdel-Latif
    Samantha Abdel-Latif
    Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States
  • Mateusz Zuba
    Mateusz Zuba
    Department of Physics, Applied Physics and Astronomy, Binghamton University, Binghamton, New York 13902, United States
    More by Mateusz Zuba
  • Kent J. Griffith
    Kent J. Griffith
    Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom
  • Alex M. Ganose
    Alex M. Ganose
    Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, United Kingdom
  • Joseph W. Stiles
    Joseph W. Stiles
    Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States
  • Shiliang Zhou
    Shiliang Zhou
    Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States
  • David O. Scanlon
    David O. Scanlon
    Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, United Kingdom
    Diamond Light Source Ltd., Diamond House, Harwell Science and Innovation Campus, Didcot, Oxfordshire OX11 0DE, United Kingdom
    Thomas Young Centre, University College London, Gower Street, London WC1E 6BT, United Kingdom
    The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot, United Kingdom
  • Louis F. J. Piper
    Louis F. J. Piper
    Department of Physics, Applied Physics and Astronomy, Binghamton University, Binghamton, New York 13902, United States
    Materials Science & Engineering, Binghamton University, Binghamton, New York 13902, United States
  • , and 
  • Brent C. Melot*
    Brent C. Melot
    Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States
    *Email: [email protected]
Cite this: ACS Energy Lett. 2020, 5, 5, 1448–1455
Publication Date (Web):April 3, 2020
https://doi.org/10.1021/acsenergylett.0c00376
Copyright © 2020 American Chemical Society

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    Abstract

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    The importance of metal migration during multielectron redox activity has been characterized, revealing a competing demand to satisfy bonding requirements and local strains in structures upon alkali intercalation. The local structural evolution required to accommodate intercalation in Y2(MoO4)3 and Al2(MoO4)3 has been contrasted by operando characterization methods, including X-ray absorption spectroscopy and diffraction, along with nuclear magnetic resonance measurements. Computational modeling further rationalized behavioral differences. The local structure of Y2(MoO4)3 was maintained upon lithiation, while the structure of Al2(MoO4)3 underwent substantial local atomic rearrangements as the more ionic character of the bonds in Al2(MoO4)3 allowed Al to mix off its starting octahedral position to accommodate strain during cycling. However, this mixing was prevented in the more covalent Y2(MoO4)3, which accommodated strain through rotational motion of polyhedral subunits. Knowing that an increased ionic character can facilitate the diffusion of redox-inactive metals when cycling multielectron electrodes offers a powerful design principle when identifying next-generation intercalation hosts.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.0c00376.

    • Experimental details, including synthetic methods, materials characterization, solid-state NMR, electrochemical characterization, and computation methodology; additional cyclic voltammetry measurements; additional X-ray diffraction and X-ray absorption spectroscopy results; radial distribution fits of EXAFS data; additional solid-state NMR measurements; additional computational modeling results (PDF)

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    Cited By

    This article is cited by 5 publications.

    1. Parker Schofield, Yuting Luo, Delin Zhang, Wasif Zaheer, David Santos, George Agbeworvi, John D. Ponis, Joseph V. Handy, Justin L. Andrews, Erick J. Braham, Ananya Renuka Balakrishna, Sarbajit Banerjee. Doping-Induced Pre-Transformation to Extend Solid-Solution Regimes in Li-Ion Batteries. ACS Energy Letters 2022, 7 (10) , 3286-3292. https://doi.org/10.1021/acsenergylett.2c01868
    2. Jessica L. Andrews, Michael J. Brady, Eric T. McClure, Brent C. Melot. Impact of Structural Deformations on the Performance of Li-Ion Insertion Hosts. Chemistry of Materials 2022, 34 (11) , 4809-4820. https://doi.org/10.1021/acs.chemmater.2c00331
    3. Joseph V. Handy, Justin L. Andrews, Saul Perez-Beltran, Daniel R. Powell, Ryan Albers, Luisa Whittaker-Brooks, Nattamai Bhuvanesh, Sarbajit Banerjee. A “Li-Eye” View of Diffusion Pathways in a 2D Intercalation Material from Topochemical Single-Crystal Transformation. ACS Energy Letters 2022, 7 (6) , 1960-1962. https://doi.org/10.1021/acsenergylett.2c00739
    4. Rebecca C. Vincent, Yunkai Luo, Jessica L. Andrews, Arava Zohar, Yucheng Zhou, Qizhang Yan, Eve M. Mozur, Molleigh B. Preefer, Johanna Nelson Weker, Anthony K. Cheetham, Jian Luo, Laurent Pilon, Brent C. Melot, Bruce Dunn, Ram Seshadri. High-Rate Lithium Cycling and Structure Evolution in Mo4O11. Chemistry of Materials 2022, 34 (9) , 4122-4133. https://doi.org/10.1021/acs.chemmater.2c00420
    5. V. R. Seymour, J. M. Griffin, B. E. Griffith, S. J. Page, D. Iuga, J. V. Hanna, M. E. Smith. Improved Understanding of Atomic Ordering in Y4SixAl2–xO9–xNx Materials Using a Combined Solid-State NMR and Computational Approach. The Journal of Physical Chemistry C 2020, 124 (43) , 23976-23987. https://doi.org/10.1021/acs.jpcc.0c07281