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Rapid and Tunable Assisted-Microwave Preparation of Glass and Glass-Ceramic Thiophosphate “Li7P3S11” Li-Ion Conductors
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    Research Article

    Rapid and Tunable Assisted-Microwave Preparation of Glass and Glass-Ceramic Thiophosphate “Li7P3S11” Li-Ion Conductors
    Click to copy article linkArticle link copied!

    • Molleigh B. Preefer
      Molleigh B. Preefer
      Department of Chemistry and Biochemistry  and  Materials Research Laboratory, University of California, Santa Barbara, Santa Barbara, California 93106, United States
    • Jason H. Grebenkemper
      Jason H. Grebenkemper
      Materials Research Laboratory, University of California, Santa Barbara, Santa Barbara, California 93106, United States
    • Franziska Schroeder
      Franziska Schroeder
      Materials Research Laboratory, University of California, Santa Barbara, Santa Barbara, California 93106, United States
    • Joshua D. Bocarsly
      Joshua D. Bocarsly
      Materials Research Laboratory  and  Materials Department, University of California, Santa Barbara, Santa Barbara, California 93106, United States
    • Kartik Pilar
      Kartik Pilar
      Materials Research Laboratory, University of California, Santa Barbara, Santa Barbara, California 93106, United States
      More by Kartik Pilar
    • Joya A. Cooley
      Joya A. Cooley
      Materials Research Laboratory, University of California, Santa Barbara, Santa Barbara, California 93106, United States
    • William Zhang
      William Zhang
      Department of Chemistry and Biochemistry, University of California, Santa Barbara, Santa Barbara, California 93106, United States
    • Jerry Hu
      Jerry Hu
      Materials Research Laboratory, University of California, Santa Barbara, Santa Barbara, California 93106, United States
      More by Jerry Hu
    • Sumohan Misra
      Sumohan Misra
      BASF SE, 67056 Ludwigshafen, Germany
    • Fabian Seeler
      Fabian Seeler
      BASF SE, 67056 Ludwigshafen, Germany
    • Kerstin Schierle-Arndt
      Kerstin Schierle-Arndt
      BASF SE, 67056 Ludwigshafen, Germany
    • Ram Seshadri*
      Ram Seshadri
      Department of Chemistry and Biochemistry,  Materials Research Laboratory  and  Materials Department, University of California, Santa Barbara, Santa Barbara, California 93106, United States
      *E-mail: [email protected]
      More by Ram Seshadri
    Other Access OptionsSupporting Information (1)

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2019, 11, 45, 42280–42287
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.9b15688
    Published November 4, 2019
    Copyright © 2019 American Chemical Society

    Abstract

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    Abstract Image

    Glass and glass-ceramic samples of metastable lithium thiophosphates with compositions of 70Li2S-30P2S5 and Li7P3S11 were controllably prepared by using a rapid assisted-microwave procedure in under 30 min. The rapid preparation times and weak coupling of the evacuated silica ampules with microwave radiation ensure minimal reactivity of the reactants and the container. The microwave-prepared samples display comparable conductivity values with more conventionally prepared (melt quenched) glass and glass-ceramic samples, on the order of 0.1 and 1 mS cm–1 at room temperature, respectively. Rietveld analysis of synchrotron X-ray diffraction data acquired with an internal standard quantitatively yields phase amounts of the glassy and amorphous components, establishing the tunable nature of the microwave preparation. X-ray photoelectron spectroscopy and Raman spectroscopy confirm the composition and the appropriate ratios of isolated and corner-sharing tetrahedra in these semicrystalline systems. Solid-state 7Li nuclear magnetic resonance (NMR) spectroscopy resolves the seven crystallographic Li sites in the crystalline compound into three main environments. The diffusion behavior of these Li environments as obtained from pulsed-field gradient NMR methods can be separated into one slow and one fast component. The rapid and tunable approach to the preparation of high quality “Li7P3S11” samples presented here coupled with detailed structural and compositional analysis opens the door to new and promising metastable solid electrolytes.

    Copyright © 2019 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.9b15688.

    • Table of quantified crystallinities from Rietveld refinements for identically prepared glass-ceramic and annealed glass-ceramic samples; laboratory XRD on three identically prepared samples of the glass-ceramic; laboratory XRD comparing the glass, glass-ceramic, and annealed glass-ceramic; Rietveld refinements of glass-ceramic and annealed glass-ceramic with Si added from synchrotron data as well as glass data with added Si; setup to measure electrochemical impedance spectroscopy under pressure and heat described in detail; representative electrochemical impedance spectroscopy equivalent circuit fit used to calculate ionic conductivity values; representative double-exponential fit to pulsed field gradient (PFG) NMR data used to calculate diffusion constants (PDF)

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    Cited By

    Click to copy section linkSection link copied!

    This article is cited by 23 publications.

    1. Molleigh B. Preefer, Jason H. Grebenkemper, Catrina E. Wilson, Margaux Everingham, Joya A. Cooley, Ram Seshadri. Subtle Local Structural Details Influence Ion Transport in Glassy Li+ Thiophosphate Solid Electrolytes. ACS Applied Materials & Interfaces 2021, 13 (48) , 57567-57575. https://doi.org/10.1021/acsami.1c16515
    2. Kazuki Uchida, Takahiro Ohkubo, Futoshi Utsuno, Koji Yazawa. Modified Li7P3S11 Glass-Ceramic Electrolyte and Its Characterization. ACS Applied Materials & Interfaces 2021, 13 (31) , 37071-37081. https://doi.org/10.1021/acsami.1c08507
    3. Rebecca C. Vincent, Pratap Vishnoi, Molleigh B. Preefer, Jimmy-Xuan Shen, Fabian Seeler, Kristin A. Persson, Ram Seshadri. Li5VF4(SO4)2: A Prototype High-Voltage Li-Ion Cathode. ACS Applied Materials & Interfaces 2020, 12 (43) , 48662-48668. https://doi.org/10.1021/acsami.0c14781
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    11. Jianbin Zhou, Ping Chen, Wei Wang, Xin Zhang. Li7P3S11 electrolyte for all-solid-state lithium-ion batteries: structure, synthesis, and applications. Chemical Engineering Journal 2022, 446 , 137041. https://doi.org/10.1016/j.cej.2022.137041
    12. Arya Das, Satyaswini Sahu, Mamata Mohapatra, Sarika Verma, Aninda J. Bhattacharyya, Suddhasatwa Basu. Lithium-ion conductive glass-ceramic electrolytes enable safe and practical Li batteries. Materials Today Energy 2022, 29 , 101118. https://doi.org/10.1016/j.mtener.2022.101118
    13. Shu Zhao, Wei Jiang, Xinxin Zhu, Min Ling, Chengdu Liang. Understanding the synthesis of inorganic solid-state electrolytes for Li ion batteries: Features and progress. Sustainable Materials and Technologies 2022, 33 , e00491. https://doi.org/10.1016/j.susmat.2022.e00491
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    15. Pingping Dong, Qing Jiao, Zengcheng Zhang, Miao Jiang, Changgui Lin, Xianghua Zhang, Hongli Ma, Baochen Ma, Shixun Dai, Tiefeng Xu. Controllable Li 3 PS 4 –Li 4 SnS 4 solid electrolytes with affordable conductor and high conductivity for solid‐state battery. Journal of the American Ceramic Society 2022, 105 (5) , 3252-3260. https://doi.org/10.1111/jace.18287
    16. Jianbin Zhou, Ying Chen, Zhaoxin Yu, Mark Bowden, Quin R. S. Miller, Ping Chen, H. Todd Schaef, Karl T. Mueller, Dongping Lu, Jie Xiao, Jun Liu, Wei Wang, Xin Zhang. Wet-chemical synthesis of Li7P3S11 with tailored particle size for solid state electrolytes. Chemical Engineering Journal 2022, 429 , 132334. https://doi.org/10.1016/j.cej.2021.132334
    17. Shunsuke Ariga, Takahiro Ohkubo, Shingo Urata, Yutaka Imamura, Taketoshi Taniguchi. A new universal force-field for the Li 2 S–P 2 S 5 system. Physical Chemistry Chemical Physics 2022, 24 (4) , 2567-2581. https://doi.org/10.1039/D1CP05393K
    18. C. Vinod Chandran, P. Heitjans. Solid-state NMR studies of lithium ion dynamics across materials classes: Review update. 2022, 1-51. https://doi.org/10.1016/bs.arnmr.2022.04.001
    19. Hirotada Gamo, Atsushi Nagai, Atsunori Matsuda. The effect of solvent on reactivity of the Li2S–P2S5 system in liquid-phase synthesis of Li7P3S11 solid electrolyte. Scientific Reports 2021, 11 (1) https://doi.org/10.1038/s41598-021-00662-3
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2019, 11, 45, 42280–42287
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.9b15688
    Published November 4, 2019
    Copyright © 2019 American Chemical Society

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