Operando Transmission Electron Microscopy Study of All-Solid-State Battery Interface: Redistribution of Lithium among Interconnected Particles

ACS Applied Energy Materials, vol. 3, pp. 5101–5106

Abstract

Abstract With operando transmission electron microscopy visualizing the solid–solid electrode–electrolyte interface of silicon active particles and lithium oxide solid electrolyte as a model system, we show that (de)lithiation (battery cycling) does not require all particles to be in direct contact with electrolytes across length scales of a few hundred nanometers. A facile lithium redistribution that occurs between interconnected active particles indicates that lithium does not necessarily become isolated in individual particles due to loss of a direct contact. Our results have implications for the design of all-solid-state battery electrodes with improved capacity retention and cyclability.

Authors 17

1. Shibabrata Basak corresponding

   Forschungszentrum Jülich · Delft University of Technology

   Affiliation as printed

   Delft University of Technology , , Mekelweg 15 , ,

   Forschungszentrum Jülich GmbH , , ,

   Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, Delft 2629JB, Netherlands

   Institute of Energy and Climate Research, Fundamental Electrochemistry (IEK-9), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

2. Vadim Migunov

   Forschungszentrum Jülich · Ernst Ruska Centre

   Affiliation as printed

   Forschungszentrum Jülich GmbH , , ,

   Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

3. Amir Hossein Tavabi

   Forschungszentrum Jülich · Ernst Ruska Centre

   Affiliation as printed

   Forschungszentrum Jülich GmbH , , ,

   Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

4. Chandramohan George

   Imperial College London

   Affiliation as printed

   Imperial College London , , ,

   Dyson School of Design Engineering, Imperial College London, SW7 2AZ London, United Kingdom

5. Qing Lee

   Delft University of Technology

   Affiliation as printed

   Delft University of Technology , , Mekelweg 15 , ,

   Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, Delft 2629JB, Netherlands

6. Paolo Rosi

   University of Modena and Reggio Emilia

   Affiliation as printed

   University of Modena and Reggio Emilia , , ,

   Department of Physics, University of Modena and Reggio Emilia, Modena 41125, Italy

7. Violetta A. Arszelewska

   Delft University of Technology

   Affiliation as printed

   Delft University of Technology , , Mekelweg 15 , ,

   Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, Delft 2629JB, Netherlands

8. Swapna Ganapathy

   Delft University of Technology

   Affiliation as printed

   Delft University of Technology , , Mekelweg 15 , ,

   Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, Delft 2629JB, Netherlands

9. Frans G. B. Ooms

   Delft University of Technology

   Affiliation as printed

   Delft University of Technology , , Mekelweg 15 , ,

   Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, Delft 2629JB, Netherlands

10. Roland Schierholz

    Forschungszentrum Jülich

    Affiliation as printed

    Forschungszentrum Jülich GmbH , , ,

    Institute of Energy and Climate Research, Fundamental Electrochemistry (IEK-9), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

11. Hermann Tempel

    Forschungszentrum Jülich

    Affiliation as printed

    Forschungszentrum Jülich GmbH , , ,

    Institute of Energy and Climate Research, Fundamental Electrochemistry (IEK-9), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

12. Hans Kungl

    Forschungszentrum Jülich

    Affiliation as printed

    Forschungszentrum Jülich GmbH , , ,

    Institute of Energy and Climate Research, Fundamental Electrochemistry (IEK-9), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

13. Joachim Mayer Aachen Central Facility for Electron Microscopy GFE

    Forschungszentrum Jülich · Ernst Ruska Centre · RWTH Aachen University

    Affiliation as printed

    Forschungszentrum Jülich GmbH , , ,

    RWTH Aachen University , , ,

    Central Facility for Electron Microscopy GFE, RWTH Aachen University, 52074 Aachen, Germany

    Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

14. Rafal E. Dunin‐Borkowski

    Forschungszentrum Jülich · Ernst Ruska Centre

    Affiliation as printed

    Forschungszentrum Jülich GmbH , , ,

    Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

15. Rüdiger‐A. Eichel Aachen Institute of Physical Chemistry

    Forschungszentrum Jülich · RWTH Aachen University

    Affiliation as printed

    Forschungszentrum Jülich GmbH , , ,

    RWTH Aachen University , , ,

    Institute of Energy and Climate Research, Fundamental Electrochemistry (IEK-9), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

    Institute of Physical Chemistry, RWTH Aachen University, 52074 Aachen, Germany

16. Marnix Wagemaker

    Delft University of Technology

    Affiliation as printed

    Delft University of Technology , , Mekelweg 15 , ,

    Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, Delft 2629JB, Netherlands

17. Erik M. Kelder

    Delft University of Technology

    Affiliation as printed

    Delft University of Technology , , Mekelweg 15 , ,

    Department of Radiation Science and Technology, Delft University of Technology, Mekelweg 15, Delft 2629JB, Netherlands