Tudball, Matthew; (2025) Manufacturing Gradients into Battery Electrode Architecture using Ultrasonic Spray Deposition. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

The breadth and impact of lithium batteries has grown rapidly and will continue to increase as energy storage becomes a crucial method of reducing carbon emissions, through electrification of transport and the balancing of renewable electricity generators. Current state-of-the-art transition metal oxide/graphite-based batteries are nearing their theoretical limits, therefore new materials and technologies will be relied on for the necessary increases in performance and safety of future energy storage. Spray deposition encompasses a range of aerosol-based coating techniques which build thin films of material in a layer-by-layer fashion, allowing precise control over the through-thickness structure of the electrode. In this work, a spray deposition-based technique for electrode manufacture is developed with the aim of creating through-thickness gradients within battery materials to solve critical issues which plague these chemistries. This gradient spray technique was applied to three different battery chemistries: lithium sulfur, solid-state and silicon anodes, with the intent to demonstrate the importance of non-homogenous electrode design in optimising the electrochemical performance of a wide-range of materials. Graded electrodes were manufactured, characterised and tested to further understand the influence of the gradient on the intrinsic properties of the battery. Gold catalyst gradients in lithium sulfur cathodes improved capacity retention at high discharge rates when gold content was increased towards the electrode surface. Graded cathode to polymer electrolyte electrodes reduced resistance and improved battery lifetime and performance in solid-state batteries. Finally, grading silicon towards the current collector was shown to extend the lifetime of silicon/graphite anodes. Considerations were made into the commercial viability of spray deposition as a battery manufacture technique, with a focus on reduced manufacture time and cost, through combination with traditional slurry-based methods. The goal of this work was to explore proof-of-concept designs for a commercially viable electrode manufacture method that promoted complex and intricate designs to progress new battery technologies.

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