A Ceramic Network for Hybrid Solid Electrolyte Lithium Metal Batteries

Advanced Science, vol. 13, pp. e76063

Abstract

ABSTRACT Hybrid solid electrolytes (HSEs) represent a promising material system for lithium metal batteries by combining high ionic conductive and mechanically strong inorganic with soft organic solid electrolytes. However, for HSEs consisting of ceramic fillers, lithium hopping between the polymer and ceramic phases remains unproven, emphasizing the tortuosity inside the polymer phase as a pivotal factor. Herein, we report an in‐plane aligned Li 6.6 La 3 Zr 1.6 Ta 0.4 O 12 (Ta‐LLZO) ceramic fiber network structure for HSEs and compare its morphological nature to typical LLZO‐based fillers. Simulations reveal a high tortuosity inside the polymer phase with a parallel to the electrodes aligned network structure, enabling dendritic structure blocking behavior, but still reaching decent ionic transport (0.44 mS cm −1 , 60°C). Post‐mortem microscopy analyses confirmed the dendrite blocking mechanism of the network, ultimately leading to long cycling lifetime of > 1100 h in symmetric lithium metal cells operated with 0.1 mA cm −2 at 60°C. Overall, the ceramic network HSE represents a superior morphology by combining decent ionic conductivity, low resistance and long cycling life in symmetric and full cells with LiFePO 4 cathodes. The comparison of different filler characteristics with a special focus on tortuosity eventually facilitates the evaluation of these properties for the purpose of optimizing HSEs.

Authors 11

1. Luca Guido Weckelmann corresponding Aachen Institute of Physical Chemistry

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

   Institute of Physical Chemistry RWTH Aachen University Aachen Germany

2. Jeong Seop Yoon

   Argonne National Laboratory

   Affiliation as printed

   Chemical Sciences and Engineering Division Argonne National Laboratory Lemont Illinois USA

3. Jehad Ahmed Aachen Institute of Physical Chemistry

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

   Institute of Physical Chemistry RWTH Aachen University Aachen Germany

4. Krzysztof Dzięcioł

   Forschungszentrum Jülich

   Affiliation as printed

   Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

5. Anna Windmüller

   Forschungszentrum Jülich

   Affiliation as printed

   Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

6. Luc Raijmakers

   Forschungszentrum Jülich

   Affiliation as printed

   Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

7. Sanja Tepavcevic

   Argonne National Laboratory

   Affiliation as printed

   Materials Science Division Argonne National Laboratory Lemont Illinois USA

8. Hans Kungl

   Forschungszentrum Jülich

   Affiliation as printed

   Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

9. Venkat Srinivasan

   Argonne National Laboratory

   Affiliation as printed

   Argonne Collaborative Center For Energy Storage Science Argonne National Laboratory Lemont Illinois USA

10. Chih‐Long Tsai corresponding

    Forschungszentrum Jülich

    Affiliation as printed

    Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

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

    Forschungszentrum Jülich · RWTH Aachen University

    Affiliation as printed

    Institute of Energy Technologies Fundamental Electrochemistry (IET‐1) Forschungszentrum Jülich Jülich Germany

    Institute of Physical Chemistry RWTH Aachen University Aachen Germany