Date of Award
Doctor of Philosophy (PhD)
Renewable energy sources offer a viable solution to the growing energy demand while mitigating concerns for greenhouse gas emissions and climate change. This has led to a tremendous momentum towards solar and wind-based energy harvesting technologies driving efficiencies higher and costs lower. However, the intermittent nature of these energy sources necessitates energy storage technologies, which remain the Achilles heel in meeting the renewable energy goals. This dissertation focusses on two approaches for addressing the needs of energy storage: first, targeting direct solar to fuel conversion via photoelectrochemical water-splitting and second, improving the performance of current rechargeable batteries by developing new electrode architectures and synthesis processes.
The aerosol chemical vapor deposition (ACVD) process has emerged as a promising single-step approach for nanostructured thin film synthesis directly on substrates. The relationship between the morphology and the operating parameters in the process is complex. In this work, a simulation based approach has been developed to understand the relationship and acquire the ability of predicting the morphology. These controlled nanostructured morphologies of TiO2, compounded with gold nanoparticles of various shapes, are used for solar water-splitting applications. Tuning of light absorption in the visible-light range along with reduced electron-hole recombination in the composite structures has been demonstrated.
The ACVD process is further extended to a novel single-step synthesis of nanostructured TiO2 electrodes directly on the current collector for applications as anodes in lithium-ion batteries, mainly for electric vehicles and hybrid electric vehicles. The effect of morphology of the nanostructures has been investigated via experimental studies and electrochemical transport modelling. Results demonstrate the exceptional performance of the single crystal one-dimensional nanostructures over granular structures, due to a combination of high surface area, improved lithium diffusivity and electronic conductivity. The model developed allows for the prediction of optimized nanostructure geometry depending on the end-use application.
Increasing demand for lithium-ion batteries, posing concerns for lithium supply and costs in future, have motivated research in sodium-ion batteries as alternatives. In this work, the nanostructured TiO2 electrodes have been studied as anodes for sodium ion batteries. To improve the performance, a new multi-component ACVD process has been developed to achieve single-step synthesis of doped nanostructured thin films. One-dimensional niobium doped TiO2 thin films have been synthesized and characterized as a novel anode material for sodium-ion batteries. The doped nanostructured thin films deliver significant improvements on capacity over their undoped counterparts and demonstrate feasibility of sodium-ion batteries. In summary, the studies conducted in this dissertation develop a detailed understanding of the ACVD process and demonstrate its ability to synthesize superior nanostructured thin films for energy storage applications, thereby motivating process scalability for commercial applications.
Richard L. Axelbaum, Parag Banerjee, Palaghat Ramachandran, Elijah Thimsen, Srikanth Kommu