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Three-dimensional operando optical imaging of particle and electrolyte heterogeneities inside Li-ion batteries

Pandya, R; Valzania, L; Dorchies, F; Xia, F; Mc Hugh, J; Mathieson, A; Tan, HJ; ... Grimaud, A; + view all (2023) Three-dimensional operando optical imaging of particle and electrolyte heterogeneities inside Li-ion batteries. Nature Nanotechnology , 18 pp. 1185-1194. 10.1038/s41565-023-01466-4. Green open access

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Abstract

Understanding (de)lithiation heterogeneities in battery materials is key to ensure optimal electrochemical performance. However, this remains challenging due to the three-dimensional morphology of electrode particles, the involvement of both solid- and liquid-phase reactants and a range of relevant timescales (seconds to hours). Here we overcome this problem and demonstrate the use of confocal microscopy for the simultaneous three-dimensional operando measurement of lithium-ion dynamics in individual agglomerate particles, and the electrolyte in batteries. We examine two technologically important cathode materials: Li xCoO2 and Li xNi0.8Mn0.1Co0.1O2. The surface-to-core transport velocity of Li-phase fronts and volume changes are captured as a function of cycling rate. Additionally, we visualize heterogeneities in the bulk and at agglomerate surfaces during cycling, and image microscopic liquid electrolyte concentration gradients. We discover that surface-limited reactions and intra-agglomerate competing rates control (de)lithiation and structural heterogeneities in agglomerate-based electrodes. Importantly, the conditions under which optical imaging can be performed inside the complex environments of battery electrodes are outlined.

Type: Article
Title: Three-dimensional operando optical imaging of particle and electrolyte heterogeneities inside Li-ion batteries
Location: England
Open access status: An open access version is available from UCL Discovery
DOI: 10.1038/s41565-023-01466-4
Publisher version: https://doi.org/10.1038/s41565-023-01466-4
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: Batteries, Imaging studies, Imaging techniques
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.ucl.ac.uk/id/eprint/10176980
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