Unravelling electro-chemo- mechanical interplay in layered oxide cathode degradation in solid-state batteries

  • Xueli Zheng
  • , Zhichen Xue
  • , Hongchang Hao
  • , Yukio Cho
  • , Yuanshun Li
  • , Chanho Kim
  • , Pawel Czaja
  • , Samuel Sanghyun Lee
  • , Sharon Bone
  • , Eleanor Spielman-Sun
  • , Zhelong Jiang
  • , X. Wendy Gu
  • , Johanna Nelson Weker
  • , Guang Yang
  • , Jagjit Nanda

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

Solid-state batteries (SSBs) hold notable promise for advancing energy storage technologies. However, their commercial viability is limited by the poor cycle stability and complex degradation mechanism. This study underscores the pivotal role of electro-chemo- mechanical interactions in driving the failure of SSBs. Leveraging advanced x-ray imaging and spectroscopy techniques, we analyzed LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes from cycled LixIn||Li6PS5Cl (LPSC)||NMC811 SSBs, uncovering the interplay between microstructure, chemical heterogeneity, mechanical characteristics, and electrochemical performance. Our results show that revealing electro-chemo- mechanical interactions is essential to develop strategies to suppress the degradation of SSBs. Particularly, we revisit a LiNbO3 (LNO) coating layer to mitigate electrochemical degradation. The LNO@NMC811 cathode retains 116 milliampere-hours per gram after 200 cycles, showing excellent stability, while the uncoated NMC811 cathode keeps degrading over time, with suppressed chemical heterogeneity and mechanical failure. This work highlights the importance of synergizing advanced material design with coating techniques, ensuring uniform lithium flux and improving mechanical properties to achieve stable, high-performance SSBs.

Original languageEnglish
Article numbeready7189
JournalScience Advances
Volume11
Issue number41
DOIs
StatePublished - 2025

Funding

Acknowledgments Funding: this research is supported by the Office of energy efficiency and Renewable energy (eeRe) in the vehicle technologies Office (vtO) through the Advanced Battery Materials Research (BMR) Program, managed by S. thompson and t. duong. We acknowledge the use and support of the Stanford nano Shared Facilities and the Stanford nanofabrication Facility. Use of the SSRl, SlAc national Accelerator laboratory, is supported by the US department of energy, Office of Science, Office of Basic energy Sciences under contract no. de-Ac02-76SF00515. Author contributions: conceptualization: X.Z., Z.X., G.Y., and J.n. Methodology: P.c., S.B., e.S.-S., X.W.G., J.n.W., and G.Y. investigation: X.Z., Z.X., h.h., Y.c., Y.l., P.c., S.S.l., c.K., and Z.J. visualization: X.Z., Z.X., h.h., and S.S.l. Supervision: Z.X., G.Y., and J.n. Writing—original draft: Z.X. and X.Z. Writing—review and editing: G.Y. and J.n. Competing interests: the authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. This research is supported by the Office of Energy Efficiency and Renewable Energy (EERE) in the Vehicle Technologies Office (VT O) through the Advanced Battery Materials Research (BMR) Program, managed by S. Thompson and T. Duong. We acknowledge the use and support of the Stanford Nano Shared Facilities and the Stanford Nanofabrication Facility. Use of the SSRL, SLAC National Accelerator Laboratory, is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02- 76SF00515.

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