journal article·2022-03-09

Study of LiCoO2/Li7La3Zr2O12:Ta Interface Degradation in All-Solid-State Lithium Batteries

Martin Ihrig, Martin Finsterbusch, Alexander M. Laptev, Chia-hao Tu, Ngoc Thanh Thuy Tran, Che-an Lin, Liang-Yin Kuo, Ruijie Ye, Yoo Jung Sohn, Payam Kaghazchi, Shih-kang Lin, Dina Fattakhova-Rohlfing, Olivier Guillon

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Abstract

The garnet-type Li7La3Zr2O12 (LLZO) ceramic solid electrolyte combines high Li-ion conductivity at room temperature with high chemical stability. Several all-solid-state Li batteries featuring the LLZO electrolyte and the LiCoO2 (LCO) or LiCoO2–LLZO composite cathode were demonstrated. However, all batteries exhibit rapid capacity fading during cycling, which is often attributed to the formation of cracks due to volume expansion and the contraction of LCO. Excluding the possibility of mechanical failure due to crack formation between the LiCoO2/LLZO interface, a detailed investigation of the LiCoO2/LLZO interface before and after cycling clearly demonstrated cation diffusion between LiCoO2 and the LLZO. This electrochemically driven cation diffusion during cycling causes the formation of an amorphous secondary phase interlayer with high impedance, leading to the observed capacity fading. Furthermore, thermodynamic analysis using density functional theory confirms the possibility of low- or non-conducting secondary phases forming during cycling and offers an additional explanation for the observed capacity fading. Understanding the presented degradation paves the way to increase the cycling stability of garnet-based all-solid-state Li batteries.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Energy and Climate Research − Materials Synthesis and Processing, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

Institute of Mineral Engineering, RWTH Aachen University, Mauerstraße 5, 52064 Aachen, Germany

Jülich-Aachen Research Alliance: JARA-ENERGY, 52425 Jülich, Germany

Helmholtz Institute Münster: Ionics in Energy Storage, Corrensstraße 46, 48149 Münster, Germany

Hierarchical Green-Energy Materials Research Center, National Cheng Kung University, No. 1, University Road, Tainan City 701, Taiwan

Department of Materials Science and Engineering, National Cheng Kung University, No. 1, University Road, Tainan City 701, Taiwan

Program on Smart and Sustainable Manufacturing, Academy of Innovative Semiconductor and Sustainable Manufacturing, National Cheng Kung University, No. 1, University Road, Tainan City 701, Taiwan

Faculty of Engineering and Center for Nanointegration Duisburg-Essen, University of Duisburg-Essen, Lotharstraße 1, 47057 Duisburg, Germany

Funding

Bundesministerium f?r Bildung und Forschung · Ministry of Science and Technology, Taiwan

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