Le Houx, James ORCID: https://orcid.org/0000-0002-1576-0673, Mistry, Jamini Jessica, Li, Yaozhu, Lesage, Louis, Staeck, Steffen, Bird, Robert and Spencer-Jolly, Dominic (2026) The topographic origin of chemomechanical failure in high-nickel cathodes revealed by operando darkfield X-ray microscopy. [Working Paper] (doi:10.26434/chemrxiv.15002900/v1)

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Abstract

Mechanical degradation in high-nickel cathodes, driven by anisotropic volume changes, remains a primary bottleneck for the lifetime of high-energy density batteries. Yet, the nanoscale origins of strain and defect initiation within individual primary particles remain unclear. Here, in the first application of operando dark-field X-ray microscopy (DFXM) to a battery system, we directly observe a dislocation wall nucleating from a pre-existing topographical flaw on the surface of a single NMC 811 primary particle. We show that failure is not stochastic, but deterministically driven by surface topography; the flaw creates a local stress concentration of ∼100 MPa, exceeding the material’s yield strength, while the bulk particle remains elastic. This observation establishes a direct physical link between primary particle surface morphology and the onset of irreversible plasticity. These findings prescribe a clear design rule: beyond bulk chemical stability, engineering particles with pristine, defect-free surfaces is essential for mitigating strain localisation and extending battery lifetime.

Item Type:	Working Paper
Uncontrolled Keywords:	Dark-Field X-ray Microscopy (DFXM), chemo-mechanics, strain evolution, single particle analysis, defect nucleation
Subjects:	Q Science > Q Science (General) Q Science > QA Mathematics > QA75 Electronic computers. Computer science T Technology > TP Chemical technology
Faculty / School / Research Centre / Research Group:	Faculty of Engineering & Science Faculty of Engineering & Science > School of Computing & Mathematical Sciences (CMS)
Last Modified:	08 May 2026 14:02
URI:	https://gala.gre.ac.uk/id/eprint/53358

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