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

Research output: Contribution to journalArticlepeer-review

32 Citations (Scopus)


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.

Original languageEnglish
Pages (from-to)11288-11299
Number of pages12
JournalACS Applied Materials and Interfaces
Issue number9
Publication statusPublished - 2022 Mar 9

All Science Journal Classification (ASJC) codes

  • General Materials Science


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