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Oxide-Based Solid-State Batteries: A Perspective on Composite Cathode Architecture
Authors:Yaoyu Ren  Timo Danner  Alexandra Moy  Martin Finsterbusch  Tanner Hamann  Jan Dippell  Till Fuchs  Marius Müller  Ricky Hoft  André Weber  Larry A. Curtiss  Peter Zapol  Matthew Klenk  Anh T. Ngo  Pallab Barai  Brandon C. Wood  Rongpei Shi  Liwen F. Wan  Tae Wook Heo  Martin Engels  Jagjit Nanda  Felix H. Richter  Arnulf Latz  Venkat Srinivasan  Jürgen Janek  Jeff Sakamoto  Eric D. Wachsman  Dina Fattakhova-Rohlfing
Affiliation:1. Maryland Energy Innovation Institute (MEI2), University of Maryland (UMD), College Park, MD, 20742 USA;2. Deutsches Zentrum für Luft- und Raumfahrt (DLR) – Helmholtz-Institut Ulm (HIU), Helmholtzstraße 11, 89081 Ulm, Germany;3. Mechanical Engineering, University of Michigan (UofM), 2350 Hayward Ave., Ann Arbor, MI, 48109 USA;4. Forschungszentrum Jülich (FZJ), Institute of Energy and Climate Research (IEK-1), Wilhelm-Johnen-Straße, 52425 Jülich, Germany;5. Institute of Physical Chemistry, Justus-Liebig University Giessen (JLU), Heinrich-Buff-Ring 17, 35392 Giessen, Germany;6. Karlsruher Institut für Technologie (KIT), Institute for Applied Materials – Electrochemical Technologies (IAM-ET), Adenauerring 20b, 76131 Karlsruhe, Germany;7. Argonne National Laboratory (ANL), Lemont, IL, 60439 USA;8. Laboratory for Energy Applications for the Future (LEAF), Lawrence Livermore National Laboratory, Livermore, CA, 94550 USA;9. Oak Ridge National Laboratory (ORNL), Energy Storage and Conversion Group, Chemical Sciences Division, Oak Ridge, TN, 37830 USA
Abstract:The garnet-type phase Li7La3Zr2O12 (LLZO) attracts significant attention as an oxide solid electrolyte to enable safe and robust solid-state batteries (SSBs) with potentially high energy density. However, while significant progress has been made in demonstrating compatibility with Li metal, integrating LLZO into composite cathodes remains a challenge. The current perspective focuses on the critical issues that need to be addressed to achieve the ultimate goal of an all-solid-state LLZO-based battery that delivers safety, durability, and pack-level performance characteristics that are unobtainable with state-of-the-art Li-ion batteries. This perspective complements existing reviews of solid/solid interfaces with more emphasis on understanding numerous homo- and heteroionic interfaces in a pure oxide-based SSB and the various phenomena that accompany the evolution of the chemical, electrochemical, structural, morphological, and mechanical properties of those interfaces during processing and operation. Finally, the insights gained from a comprehensive literature survey of LLZO–cathode interfaces are used to guide efforts for the development of LLZO-based SSBs.
Keywords:ceramic cathode/electrolyte interface  grain boundaries  oxide solid electrolyte  solid state battery
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