Impact of dual-layer solid-electrolyte interphase inhomogeneities on early-stage defect formation in Si electrodes

Nature Communications, vol. 11, pp. 3283

Abstract

Abstract While intensive efforts have been devoted to studying the nature of the solid-electrolyte interphase (SEI), little attention has been paid to understanding its role in the mechanical failures of electrodes. Here we unveil the impact of SEI inhomogeneities on early-stage defect formation in Si electrodes. Buried under the SEI, these early-stage defects are inaccessible by most surface-probing techniques. With operando full field diffraction X-ray microscopy, we observe the formation of these defects in real time and connect their origin to a heterogeneous degree of lithiation. This heterogeneous lithiation is further correlated to inhomogeneities in topography and lithium-ion mobility in both the inner- and outer-SEI, thanks to a combination of operando atomic force microscopy, electrochemical strain microscopy and sputter-etched X-ray photoelectron spectroscopy. Our multi-modal study bridges observations across the multi-level interfaces (Si/LixSi/inner-SEI/outer-SEI), thus offering novel insights into the impact of SEI homogeneities on the structural stability of Si-based lithium-ion batteries.

Authors 12

1. Chunguang Chen corresponding

   Forschungszentrum Jülich · Eindhoven University of Technology

   Affiliation as printed

   Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands. c.chen@fz-juelich.de

   IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany. c.chen@fz-juelich.de

   Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands

   IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany

2. Tao Zhou

   Argonne National Laboratory

   Affiliation as printed

   ID01 ESRF, CS 40220, F-38043, Grenoble Cedex 9, France

   Nanoscience and Technology Division, Argonne National Laboratory, Chicago, 60439, IL, USA

3. Dmitri L. Danilov

   Forschungszentrum Jülich · Eindhoven University of Technology

   Affiliation as printed

   Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands

   IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany

4. Lu Gao

   Eindhoven University of Technology

   Affiliation as printed

   Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands

5. Svenja Benning Aachen

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany

   RWTH Aachen University, D-52074, Aachen, Germany

6. Nino Schön Aachen

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany

   RWTH Aachen University, D-52074, Aachen, Germany

7. Samuel Tardif

   Commissariat à l'Énergie Atomique et aux Énergies Alternatives · CEA Grenoble · Institut de Recherche Interdisciplinaire de Grenoble

   Affiliation as printed

   Univ. Grenoble Alpes, CEA, IRIG-MEM, Grenoble, 38000, France

8. Hugh Simons

   Technical University of Denmark

   Affiliation as printed

   Department of Physics, Technical University of Denmark, 2800, Kongens Lyngby, Denmark

9. Florian Hausen Aachen

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany

   RWTH Aachen University, D-52074, Aachen, Germany

10. Tobias Urs Schülli
    Affiliation as printed

    ID01 ESRF, CS 40220, F-38043, Grenoble Cedex 9, France

11. Rüdiger‐A. Eichel Aachen

    Forschungszentrum Jülich · RWTH Aachen University

    Affiliation as printed

    IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany

    RWTH Aachen University, D-52074, Aachen, Germany

12. Peter H. L. Notten corresponding

    University of Technology Sydney · Forschungszentrum Jülich · Eindhoven University of Technology

    Affiliation as printed

    Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven, The Netherlands. p.h.l.notten@tue.nl

    IEK-9, Forschungszentrum Jülich, D-52425, Jülich, Germany. p.h.l.notten@tue.nl

    University of Technology Sydney, Broadway, Sydney, NSW, 2007, Australia. p.h.l.notten@tue.nl

    University of Technology Sydney, Broadway, Sydney, NSW, 2007, Australia