The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid‐State Lithium Batteries

Author:

Scheld Walter Sebastian12ORCID,Kim Kwangnam3ORCID,Schwab Christian1ORCID,Moy Alexandra C.4ORCID,Jiang Shi‐Kai5ORCID,Mann Markus1ORCID,Dellen Christian1ORCID,Sohn Yoo Jung1ORCID,Lobe Sandra1ORCID,Ihrig Martin1ORCID,Danner Michael Gregory6ORCID,Chang Chia‐Yu5,Uhlenbruck Sven17ORCID,Wachsman Eric D.6ORCID,Hwang Bing Joe58ORCID,Sakamoto Jeff4ORCID,Wan Liwen F.3ORCID,Wood Brandon C.3,Finsterbusch Martin17ORCID,Fattakhova-Rohlfing Dina127ORCID

Affiliation:

1. Institute of Energy and Climate Research: Materials Synthesis and Processing (IEK‐1) Forschungszentrum Jülich GmbH Wilhelm-Johnen-Straße 52425 Jülich Germany

2. Faculty of Engineering and Center for Nanointegration Duisburg‐Essen CENIDE University Duisburg‐Essen Lotharstraße 1 47057 Duisburg Germany

3. Laboratory for Energy Applications for the Future Lawrence Livermore National Laboratory 7000 East Ave Livermore CA 94550 USA

4. Mechanical Engineering University of Michigan 2350 Hayward Ave. Ann Arbor MI 48109 USA

5. Department of Chemical Engineering National Taiwan University of Science and Technology Taipei 106335 Taiwan

6. Maryland Energy Innovation Institute University of Maryland College Park MD 20742 USA

7. Helmholtz Institute Münster: Ionics in Energy Storage (IEK‐12) Corrensstr. 46 48149 Münster Germany

8. National Synchrotron Radiation Research Center (NSRRC) No. 101, Hsin Ann Rd, East District Hsinchu 30076 Taiwan

Abstract

AbstractSolid‐state batteries (SSBs) with a Li7La3Zr2O12 (LLZO) garnet electrolyte are attracting much attention as robust and safe alternative to conventional lithium‐ion batteries. Technical challenges in the practical implementation of garnet SSBs are related to the need for high‐temperature sintering, which often leads to undesirable chemical reactions with the cathode material. While these reactions are well understood for composite cathodes, very little is known about similar processes between cathode and separator during battery fabrication. This work focuses on understanding the processes between the composite LiCoO2‐LLZO cathode and the LLZO separator and how they affect the battery performance. The extensive diffusion of Co‐ions within LLZO, which leads to the often‐observed LLZO darkening, is shown to have a significant impact on ionic conductivity, electronic conductivity, and dendrite stability of the separator. Experimental data coupled with large‐scale molecular dynamics simulations uncover the diffusion mechanism for Co‐ions and identify secondary phases that form during these interactions. In addition to extensive Co‐ion diffusion within the grains, a non‐uniform segregation of Co‐ions at grain boundaries is found leading to the formation of three distinct Co‐containing phases. This work offers a general approach to studying the fundamental ion diffusion processes that occur during the fabrication of oxide SSBs.

Funder

U.S. Department of Energy

Publisher

Wiley

Subject

Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials

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