Xu, Linfeng, Le Houx, James ORCID: https://orcid.org/0000-0002-1576-0673, Manchester, Tristan, Zhang, Jinsong, Wullich, Robin Norbert, Gomez, Victor Alexander, Ihli, Johannes, Banerjee, Sarbajit, Schmidt, Thomas J. and El Kazzi, Mario (2026) Correlative operando X-Ray imaging and diffraction revealing mechanical failure pathways in Lithium metal sulfide-based all-solid-state batteries. [Working Paper]

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Abstract

All-solid-state batteries (ASSBs) employing sulfide solid electrolytes and lithium metal anodes offer a promising pathway toward high energy density and enhanced safety. However, their practical deployment remains limited by strongly coupled electro-chemo-mechanical instabilities at both cathode and anode interfaces, which evolve across multiple length scales and remain insufficiently understood under realistic operating conditions. Here, we present a comprehensive multimodal operando characterization approach combining X-ray computed tomography (XCT), X-ray diffraction (XRD), and stack pressure monitoring to elucidate the dynamic degradation mechanisms in LiNi0.8Co0.1Mn0.1O2 (NCM811) | Li6PS5Cl (LPSC) | Li cells. By directly correlating particle-level morphological evolution with latticescale structural and strain dynamics, this methodology enables a unified, multiscale description of interfacial failure processes. Operando XCT and XRD jointly reveal reversible volume changes of ~6 % in NCM811 particles during (de-)lithiation. Spatially resolved operando XRD further uncovers pronounced heterogeneity in lithiation fronts and depth-dependent electrochemical activity across the cathode thickness. In parallel, a partial release of interfacial microstrain is identified at the NCM811|LPSC interface, associated with oxidative decomposition of LPSC solid electrolyte. At the LPSC|Li interface, operando XCT directly visualizes, at moderate current density (0.45 mA cm-2) but high areal capacity (4.17 mAh cm-2), crack initiation and propagation within the solid electrolyte, driven by the lithium plating-induced stress, followed by lithium infiltration, and progressive interfacial contact loss. These processes ultimately lead to mechanical disconnection and the emergence of short-circuiting at higher current densities. Notably, these mechanically induced degradation phenomena exhibit partial reversibility during lithium stripping. This multimodal operando framework provides critical insight into degradation pathways and establishes design principles for mechanically robust sulfide-based ASSBs.

Item Type:	Working Paper
Additional Information:	The data that support the findings of this study are openly available in Zenodo (DOI: 10.5281/zenodo.19866288).
Uncontrolled Keywords:	all-solid-state battery, mechanical stability, lithium metal, soft short-circuit, operando XCT-XRD, pressure monitoring
Subjects:	Q Science > Q Science (General) T Technology > T Technology (General)
Faculty / School / Research Centre / Research Group:	Faculty of Engineering & Science Faculty of Engineering & Science > School of Computing & Mathematical Sciences (CMS)
Last Modified:	26 Jun 2026 15:26
URI:	https://gala.gre.ac.uk/id/eprint/53846

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