Wade, Aaron James Radley; (2024) Optimising tomography protocols for lithium-ion battery electrode imaging. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

Consumption of fossil fuels over the last decade has resulted in rising global temperatures and cities full of carcinogenic particulates. The transportation sector emits 37% of global CO2, and is undergoing an electric revolution, replacing combustion engines with tail-pipe emissionfree electric vehicles. Due to the requirement for high energy-density batteries to enable adequate driving range, lithium-ion batteries (LIBs) are driving this change. However, to enable true global adoption, improvements in energy density must be made. Unfortunately, when improving energy density, the lifetime of the LIB typically suffers, often due to particle cracking, resulting in losses in capacity and lower lifetime performance. Therefore it is critical that characterization of electrode materials is undertaken to understand the causes of failure and if mitigation steps are working. Advanced characterization methods typically involve the use of penetrating radiation (for example X-rays or neutrons), enabling 3D, non-destructive imaging of samples. Due to its relative ease of access (available at lab-scale) X-ray Computed Tomography (X-ray CT) has risen in popularity over the last decade in LIB imaging, probing the electrode microstructure at multiple length-scales. However, despite this, X-ray CT is still an expensive technique, due to the time-consuming nature of imaging, and is typically qualitative rather than quantitative for defect detection. In this thesis, the main areas of focus will be the application of multi-scale imaging of LIB cathodes, and improving the associated workflow. The overall scientific aims of this thesis include: using iterative reconstruction to improve the image quality; applying machine learning segmentation to increase accuracy; comparing novel crack detection methods to quantify intra-particle cracking; and employing the best option on several electrodes with different electrochemical cycling histories and imaging modalities. Overall, this work aims to improve; throughput; cost; useability; and quantification of X-ray CT when applied to LIB materials.

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