DOE OSTI · 3024883
Unravelling electro-chemo-mechanical interplay in layered oxide cathode degradation in solid-state batteries
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 LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes from cycled Li x In||Li 6 PS 5 Cl (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 LiNbO 3 (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.
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Zheng, Xueli [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000268002649), Xue, Zhichen [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000315111777), Hao, Hongchang [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Cho, Yukio [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:000000030919692X), Li, Yuanshun [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)] (ORCID:0009000182641287), Kim, Chanho [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Czaja, Pawel [Stanford Univ., CA (United States); Polish Academy of Sciences (PAS), Krakow (Poland)] (ORCID:0000000150119323), Lee, Samuel Sanghyun [Stanford Univ., CA (United States)], Bone, Sharon [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Forschungszentrum Juelich (Germany)] (ORCID:0000000275219627), Spielman-Sun, Eleanor [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000196262969), Jiang, Zhelong [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000300130860), Gu, X. Wendy [Stanford Univ., CA (United States)], Weker, Johanna Nelson [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000168563203), Yang, Guang [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)] (ORCID:0000000305836272), Nanda, Jagjit [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000268750057). 2025-10-08. Unravelling electro-chemo-mechanical interplay in layered oxide cathode degradation in solid-state batteries. https://doi.org/10.1126/sciadv.ady7189
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