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Microstructural Evolution of Battery Electrodes During Calendering

Lu, X; Daemi, SR; Bertei, A; Kok, MDR; O'Regan, KB; Rasha, L; Park, J; ... Shearing, PR; + view all (2020) Microstructural Evolution of Battery Electrodes During Calendering. Joule , 4 (12) pp. 2746-2768. 10.1016/j.joule.2020.10.010. Green open access

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Abstract

Calendering is a crucial manufacturing process in the optimization of battery performance and lifetime due to its significant effect on the 3D electrode microstructure. By conducting an in situ calendering experiment on lithium-ion battery cathodes using X-ray nano-computed tomography, here we show that the electrodes composed of large particles with a broad size distribution experience heterogeneous microstructural self-arrangement. At high C-rates, the performance is predominantly restricted by sluggish solid-state diffusion, which is exacerbated by calendering due to the increased microstructural and lithiation heterogeneity, leading to active material underutilization. In contrast, electrodes consisting of small particles are structurally stable with more homogeneous deformation and a lower tortuosity, showing a much higher rated capacity that is less sensitive to calendering densification. Finally, the dependence of performance on the dual variation of both porosity and electrode thickness is investigated to provide new insights into the microstructural optimization for different applications in electrode manufacturing.

Type: Article
Title: Microstructural Evolution of Battery Electrodes During Calendering
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.joule.2020.10.010
Publisher version: https://doi.org/10.1016/j.joule.2020.10.010
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: Calendering, NMC cathodes, 3D microstructure, particle size, solid-state diffusion, heterogeneity, tortuosity, electrode thickness, image-based modelling, rated capacity
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/10119124
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