Xu, Linfeng, Le Houx, James ORCID: https://orcid.org/0000-0002-1576-0673, Kachkanov, Vyacheslav, Zhang, Jinsong, Norbert Wullich, Robin, Fankhauser, Matthias, Löffel, Kaspar, Schmidt, Thomas J. and El Kazzi, Mario (2026) Operando X‐Ray computed tomography reveals the role of interfacial nucleation nanolayers in suppressing mechanical failure in zero‐excess lithium all‐solid‐state batteries. Small:e12284. ISSN 1613-6810 (Print), 1613-6829 (Online) (doi:10.1002/smll.202512284)

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Abstract

Lithium metal (LM) and zero-excess lithium (ZE) anodes offer pathways to increase the energy density of all-solid-state batteries (ASSBs). We employ operando X-ray computed tomography combined with an image subtraction method to visualize lithium plating/stripping morphology, stack mechanical failure, and quantify the lithium reversibility in asymmetric Li6PS5Cl (LPSC)-based ASSBs. Lithium metal counter electrode (CE) and copper (Cu) working electrode (WE) emulate LM and ZE interface configurations, respectively. We compare bare Cu and silver-coated Cu (Ag/Cu) WEs under varying current densities. At 0.25 mA cm−2(WE), bare Cu shows edge-localized and non-uniform lithium deposition, while Ag/Cu facilitates more uniform lithium spreading, but results in higher first-cycle irreversibility and lower Coulombic efficiency. Above 0.5 mA cm−2(WE), failure in Li|LPSC|Cu cells initiate at the LPSC|Cu interface via spallation cracks. In contrast, Ag preserves interface integrity at the WE despite lithium initially plates at discrete nucleation spots. However, failure shifts to the Li|LPSC interface, where non-uniform lithium depletion at the CE exposes the underlying Cu, leading to spallation cracks upon subsequent plating. Mechanical finite element simulations support these observations and underscore the critical role of the nucleation layers in mitigating mechanical failure. This study highlights interface engineering as a key strategy to address electro-chemo-mechanical degradation in LM- and ZE-ASSBs.

Swiss Nanoscience Institute
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung. Grant Number: Sinergia CRSII5_202296
Rutherford Appleton Laboratory
Faraday Institution

Item Type:	Article
Additional Information:	Open access publishing facilitated by ETH-Bereich Forschungsanstalten, as part of the Wiley - ETH-Bereich Forschungsanstalten agreement via the Consortium Of Swiss Academic Libraries.
Uncontrolled Keywords:	Swiss Nanoscience Institute Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung. Grant Number: Sinergia CRSII5_202296 Rutherford Appleton Laboratory Faraday Institution alloy interlayer | all-solid-state battery | image subtraction method | Li metal | operando XCT | zero-excess lithium anode
Subjects:	Q Science > Q Science (General) Q Science > QA Mathematics > QA75 Electronic computers. Computer science 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:	12 Jan 2026 10:20
URI:	https://gala.gre.ac.uk/id/eprint/52269

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