Tracking Battery Swelling in Uncompressed Li-Ion Cells Via in-Operando X-Ray Radiography and Micro-Tomography

Li-ion battery swelling during cycling is known to be a major cause of battery electrode degradation and can contribute significantly to cell failure [1,2]. The main cause of battery swelling is due to the intercalation of Li into the carbon and LiCoO2 electrodes. This swelling is known to occur anisotropically due to the electric field and Li salt distributions in the electrode [3]. We have used x-ray radiography and µCT to map this swelling, in-operando under charge and discharge conditions, in the layers of an uncompressed Li-ion battery. This study gives insight into the relationship between the battery state of charge and the electrode swelling. The change in swelling due to the electrode geometry is also investigated. Li-ion pouch cells were cycled at 0.5, 1 and 2 C while undergoing x-ray radiography and tomography at the BMIT beamline of the Canadian Light Source. Synchrotron radiography allowed the tracking of the electrode swelling in two dimensions with high temporal (10 s/frame) and spatial resolution (3 µm/pixel). µCT measurements of Li-ion cells were carried out under the same battery cycling conditions and scans were taken at 0, 25, 75 and 100 % state of charge (3 µm/pixel, 225 s/scan). Reconstruction and segmentation of the collected images allowed for the measurement of each electrode volume. From these results it appears that electrode swelling depends on a number of factors, including electrode geometry, charge/discharge rate and battery age. There is also a noticeable degree of irreversibility in the swelling of the electrode, which may be a possible metric for battery degradation. The quantification of the carbon electrode swelling corresponds closely with the theoretical value for lithium intercalation to LiC6, although there is a discrepancy between the swelling value obtained for the LiCoO2 electrode and theory. These results give a valuable insight into the mechanical dynamics of Li-ion batteries under in-operando conditions and will provide validation to, and data for, battery models including stress-strain and degradation models. References Bond, T., Zhou, J., & Cutler, J. (2017). Electrode Stack Geometry Changes during Gas Evolution in Pouch-Cell-Type Lithium Ion Batteries. Journal of The Electrochemical Society, 164(1), A6158–A6162. Chen, C., Wei, Y., Zhao, Z., Zou, Y., & Luo, D. (2019). Investigation of the swelling failure of lithium-ion battery packs at low temperatures using 2D/3D X-ray computed tomography. Electrochimica Acta, 305, 65–71. Zhang, N., & Tang, H. (2012). Dissecting anode swelling in commercial lithium-ion batteries. Journal of Power Sources, 218, 52–55. Figure 1 (a) 2D x-ray radiography of a Li-ion pouch cell and (b) 3D reconstruction of a µCT of a Li-ion pouch cell section. Figure 1

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