Complexions at the Electrolyte/Electrode Interface in Solid Oxide Cells

ChemRxiv

Abstract

Rapid deactivation presently limits a wide spread use of high-temperature solid oxide cells (SOCs) as otherwise highly efficient chemical energy converters. With deactivation triggered by the ongoing conversion reactions, an atomic-scale understanding of the active triple-phase boundary (TPB) between electrolyte, electrode and gas phase is essential to increase cell performance. Here we use a multi-method approach comprising transmission electron microscopy and first-principles calculations and molecular simulations to untangle the atomic arrangement of the prototypical SOC interface between a lanthanum strontium manganite (LSM) anode and an yttria-stabilized zirconia (YSZ) electrolyte. We identify an interlayer of self-limited width with partial amorphization and strong compositional gradient, thus exhibiting the characteristics of a complexion that is stabilized by the confinement between two bulk phases. This offers a new perspective to understand the function of SOCs at the atomic scale. Moreover, it opens up a hitherto unrealized design space to tune the conversion efficiency.

Authors 13

1. Hanna Türk

   Fritz Haber Institute of the Max Planck Society · Technical University of Munich

   Affiliation as printed

   Fritz-Haber-Institut der Max-Planck-Gesellschaft, Theory Department, 14195 Berlin, Germany

   Technische Universität München, Department of Chemistry, Chair for Theoretical Chemistry and Catalysis Research Center, 85748 Garching, Germany

2. Thomas Götsch

   Fritz Haber Institute of the Max Planck Society

   Affiliation as printed

   Fritz-Haber-Institut der Max-Planck-Gesellschaft

3. Frank Girgsdies

   Fritz Haber Institute of the Max Planck Society

   Affiliation as printed

   Fritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic Chemistry, 14195 Berlin, Germany

4. Adnan Hammud

   Fritz Haber Institute of the Max Planck Society

   Affiliation as printed

   Fritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic Chemistry, 14195 Berlin, Germany

5. Danail Ivanov

   Fritz Haber Institute of the Max Planck Society

   Affiliation as printed

   Fritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic Chemistry, 14195 Berlin, Germany

6. Izaak C. Vinke

   Forschungszentrum Jülich

   Affiliation as printed

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

7. Lambertus G. J. de Haart
8. Rüdiger‐A. Eichel Aachen Institute of Physical Chemistry

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

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

   RWTH Aachen University, Institute of Physical Chemistry, 52056 Aachen, Germany

9. Karsten Reuter

   Forschungszentrum Jülich · Fritz Haber Institute of the Max Planck Society · Technical University of Munich

   Affiliation as printed

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

   Fritz-Haber-Institut der Max-Planck-Gesellschaft, Theory Department, 14195 Berlin, Germany

   Technische Universität München, Department of Chemistry, Chair for Theoretical Chemistry and Catalysis Research Center, 85748 Garching, Germany

10. Robert Schlögl

    Fritz Haber Institute of the Max Planck Society · Max Planck Institute for Chemical Energy Conversion

    Affiliation as printed

    Fritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic Chemistry, 14195 Berlin, Germany

    Max Planck Institute for Chemical Energy Conversion, Department of Heterogeneous Reactions, 45470 Mülheim an der Ruhr, Germany

11. Axel Knop‐Gericke

    Fritz Haber Institute of the Max Planck Society · Max Planck Institute for Chemical Energy Conversion

    Affiliation as printed

    Fritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic Chemistry, 14195 Berlin, Germany

    Max Planck Institute for Chemical Energy Conversion, Department of Heterogeneous Reactions, 45470 Mülheim an der Ruhr, Germany

12. Christoph Scheurer

    Fritz Haber Institute of the Max Planck Society · Technical University of Munich

    Affiliation as printed

    Fritz-Haber-Institut der Max-Planck-Gesellschaft, Theory Department, 14195 Berlin, Germany

    Technische Universität München, Department of Chemistry, Chair for Theoretical Chemistry and Catalysis Research Center, 85748 Garching, Germany

13. Thomas Lunkenbein

    Fritz Haber Institute of the Max Planck Society

    Affiliation as printed

    Fritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic Chemistry, 14195 Berlin, Germany