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Direct observations of electrochemically induced intergranular cracking in polycrystalline NMC811 particles

Parks, Huw CW; Boyce, Adam M; Wade, Aaron; Heenan, Thomas MM; Tan, Chun; Martínez-Pañeda, Emilio; Shearing, Paul R; ... Jervis, Rhodri; + view all (2023) Direct observations of electrochemically induced intergranular cracking in polycrystalline NMC811 particles. Journal of Materials Chemistry A 10.1039/d3ta03057a. Green open access

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Abstract

Establishing the nature of crack generation, formation, and propagation is paramount to understanding the degradation modes that govern decline in battery performance. Cracking has several possible origins; however, it can be classified in two general cases: mechanically induced, during manufacturing, or electrochemically induced, during operation. Accurate and repeatable tracking of operational cracking to sequentially image the same material as it undergoes cracking is highly challenging; observing these features requires the highest resolutions possible for 3D imaging techniques, necessitating very small sample geometry, while also achieving realistic electrochemical performance. Here, we present a technique in which particle cracking can be completely attributed to electrochemical stimulation via sequential ex situ imaging in a laboratory X-ray nano computed tomography (CT) instrument. This technique preserves the mechanical and electrochemical response of each particle without inducing damage in the particles except for the effects of high voltage. Significant cracking within the core of secondary particles was observed upon the electrochemical delithiation of NMC811, which propagated radially. As X-ray computed tomography allows for imaging of the particle cores, the particles were not required to be modified/milled, guaranteeing any synthesis induced strain in the particles was maintained during the whole technique, resulting in an observation that contrasts crystallographic data, suggesting a significant volume expansion of the secondary particles.

Type: Article
Title: Direct observations of electrochemically induced intergranular cracking in polycrystalline NMC811 particles
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/d3ta03057a
Publisher version: https://doi.org/10.1039/D3TA03057A
Language: English
Additional information: This article is licensed under a Creative Commons Attribution 3.0 Unported Licence
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery-pp.ucl.ac.uk/id/eprint/10177869
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