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Medium-Range Ordering in the Ionic Glass Electrolytes LiPON and LiSiPON

  • Andrew S. Westover*
    Andrew S. Westover
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *Email: [email protected]
  • Mordechai Kornbluth
    Mordechai Kornbluth
    Robert Bosch Research and Technology Center, Cambridge, Massachusetts 02139, United States
  • Takeshi Egami
    Takeshi Egami
    Department of Materials Science and Engineering, and Department of Physics and Astronomy, University of Tennessee, Knoxville, Tennessee 37996, United States
    Materials Sciences and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Jue Liu
    Jue Liu
    Neutron Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Jue Liu
  • Sergiy Kalnaus
    Sergiy Kalnaus
    Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831-6164, United States
  • Dong Ma
    Dong Ma
    Neutron Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    Neutron Science Platform, Songshan Lake Materials Laboratory, Dongguan, Guangdong 532800, China
    More by Dong Ma
  • Andrew K. Kercher
    Andrew K. Kercher
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Joerg C. Neuefeind
    Joerg C. Neuefeind
    Neutron Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Michelle Everett
    Michelle Everett
    Neutron Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Victor Torres
    Victor Torres
    Department of Materials Science and Engineering, Iowa State University, Ames, Iowa 50011, United States
  • Steve W. Martin
    Steve W. Martin
    Department of Materials Science and Engineering, Iowa State University, Ames, Iowa 50011, United States
  • Boris Kozinsky
    Boris Kozinsky
    John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States
    Robert Bosch Research and Technology Center, Cambridge, Massachusetts 02139, United States
  • , and 
  • Nancy J. Dudney
    Nancy J. Dudney
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
Cite this: Chem. Mater. 2023, 35, 7, 2730–2739
Publication Date (Web):March 27, 2023
https://doi.org/10.1021/acs.chemmater.2c02380
Copyright © 2023 American Chemical Society

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    Abstract

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    Here, we provide an in-depth structural characterization of the amorphous ionic glasses LiPON and LiSiPON with high Li content. Based on ab initio molecular dynamics simulations, the structure of these materials is an inverted structure with either isolated polyanion tetrahedra or polyanion dimers in a Li+ matrix. Based on neutron scattering data, this type of inverted structure leads to a significant amount of medium-range ordering in the structure, as demonstrated by two sharp diffraction peaks and a periodic structural oscillation in the density function G(r). While this medium-range ordering is commonly observed in liquids and metallic glasses, it has not previously been observed in oxides. On a local scale, adding N and Si increases the number of anion bridges and polyanion dimer structures, leading to higher ionic conductivity. In the medium-range ordering, the addition of Si leads to more disorder in the polyanion substructure but a significant increase in the ordering of the O substructure. Finally, we demonstrate that this inverted structure with medium-range ordering results in a glassy material that is both mechanically stiff and ductile on the nanoscale.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.2c02380.

    • Comparison of the simulated and experimental PDF for LiPO3 from 1–6 Å, simulated partial PDF data of Li2.7Si0.7P0.3O3.17N0.22, simulated X-ray PDF of Li2.7PO3.52N0.22, a comparison of LiSiPON scattering data with and without air exposure, unweighted PDF data g(r) for all three compositions, and fitting of the mid-range ordering of the three key compositions (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Antranik Jonderian, Sarish Rehman, Malcolm Card Gormley, Shipeng Jia, Sang Bok Ma, Giyun Kwon, Eric McCalla. Pioneering Combinatorial Investigation to Unlock the Potential of Lithium Borosilicate Glasses as Solid Electrolytes. ACS Applied Energy Materials 2024, Article ASAP.

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