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(2021)ThesisImprovements in liquid lithium-ion battery electrolytes using of metal organic frameworks (MOFs) as a functional decoration on polymer membrane separators were investigated using a combination of experimental and theoretical methods. Zirconium-based MOF UiO-66 was introduced to the polymer support using the mixed matrix membrane (MMM) method. The method allowed the one-step manufacture of a robust, mechanically pliable polymer-MOF membrane composite of high MOF loading. MOF-MMMs imparted improved electrochemical behaviours such as a widened potential operating window, near-unity transference number, and increased presence of solid electrolyte interphase (SEI) components crucial to battery performance. Density functional theory (DFT) calculations were also performed to provide insights regarding electrolyte solvation in the presence of MOF. A simple dip-coating technique was utilised to modify the surface of the MOF-MMMs with polydopamine (PDA) for further improvement of the electrochemical properties. Increased transference numbers, as well as stability during rate cycling, were observed with the resulting PDA-MMM owing to the improved electrode/electrolyte interface. However, surface analyses using x-ray photoelectron spectroscopy (XPS) showed that there are reduced amounts vital SEI components compared to the original MOF-MMM support. The last section further explores the versatility of UiO-66 and tackled the preparation of gel polymer electrolytes (GPEs) decorated with UiO-66 via phase inversion technique. Using the phase inversion method, the fabricated GPE contained pores from both polymer substrate and the intrinsic pores of the 3D nanomaterial for improvement of electrochemical properties. It was demonstrated in this work that the MOF GPE is equally inert and suitable in ether or carbonate-based electrolytes. Overall, this study demonstrated the versatility of UiO-66 metal organic frameworks for use as a functional nanofiller for electrolyte membranes. With the use of inexpensive membrane fabrication methods, the composites obtained are viable for lithium-metal battery applications. Similarly, insights drawn can provide a springboard towards future study of MOF-based electrolytes.
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(2022)ThesisThis thesis focuses on the development and applications of magnetic resonance electrical properties tomography (MREPT), which is an emerging imaging modality to noninvasively obtain the electrical properties of tissues, such as conductivity and permittivity. Chapter 2 describes the general information about human research ethics, MRI scanner, MR sequence and the method of phase-based MREPT implemented in this thesis. Chapter 3 examines the repeatability of phase-based MREPT in the brain conductivity measurement using balanced fast field echo (bFFE) and turbo spin echo (TSE) sequences, and investigate the effects of compressed SENSE, whole-head B_1 shimming and video watching during scan on the measurement precision. Chapter 4 investigates the conductivity signal in response to short-duration visual stimulus, compares the signal and functional activation pathway with that of BOLD, and tests the consistency of functional conductivity imaging (funCI) with visual stimulation across participants. Chapter 5 extends the use of functional conductivity imaging to somatosensory stimulation and trigeminal nerve stimulation to evaluate the consistency of functional conductivity activation across different types of stimuli. In addition, visual adaptation experiment is performed to test if the repetition suppression effect can be observed using funCI. Chapter 6 explores if resting state conductivity networks can be reliably constructed using resting state funCI, evaluates the consistency of persistent homology architectures, and compares the links between nodes in the whole brain. Chapter 7 investigates the feasibility of prostate conductivity imaging using MREPT, and distinctive features in the conductivity distribution between healthy participants and participants with suspected abnormalities.
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(2022)ThesisTwo-dimensional transition metal dichalcogenide (TMD) nanocrystals (NCs) exhibit unique optical and electrocatalytic properties. However, the growth of uniform and high-quality NCs of monolayer TMD remains a challenge. Until now, most of them are synthesized via solution-based hydrothermal process or ultrasonic exfoliation method, in which the capping ligands introduced from organic solution often quench the optical and electrocatalytic properties of TMD NCs. Moreover, it is difficult to homogeneously disperse the solution-based TMD NCs on a substrate for device fabrication since the dispersed NCs can easily aggregate. Here, we put forward a novel CVD method to grow closely-spaced TMD NCs and explored the growth mechanism and attempts on the size control. Their applications acting as electrocatalysts and adhesion layer for Au film deposition have been also well displayed. Through the whole chapters of this thesis, the following aspects are highlighted: 1. MoS2 and other TMD nanocrystals have been grown on the c-plane sapphire. The surface oxygen vacancies determine the density of TMD nanocrystals. The MoS2 nanocrystals demonstrate excellent hydrogen evolution reaction and surface-enhanced Raman scattering performance owing to the abundant edges. 2. Deep insights into the growth of MoS2 nanograins have been explored. The surface step edges and lattice structures of the underlying sapphire substrates have a significant influence on the growth behaviors. The step edges could modulate the aggregation of MoS2 nanograins to form unidirectional triangular islands. The Raman spectra of MoS2 demonstrate a linear relationship with the crystal size of MoS2. 3. The orientation of sapphire substrate has an of importance effect on the critical size of MoS2 nanocrystals. The MoS2 nanocrystals have the smallest size on the r-plane sapphire, besides, the MoS2 on r-plane sapphire demonstrates the sintering-resistance feature, which is attributed to the edge-pinning effect when MoS2 edges are anchored on the sapphire surface. 4. The MoS2 nanocrystalline layer was utilized as the adhesion layer for Au film depositing on a sapphire substrate. The Au films on MoS2 displayed superior transmittance and electrical conductivity as well as outstanding thermal stability, which lay in the strong binding of Au film with MoS2 nanocrystalline layer.
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(2023)ThesisBiodegradable implant materials are more appropriate for temporary support applications compared with their inert counterparts since the former requires no removal surgery because they naturally degrade and eventually dissolve completely during healing. Iron and its alloys are a possible substitute for the commercial magnesium biodegradable implants because of their superior mechanical properties and slower corrosion rates. The addition of manganese and silicon in iron imparts another interesting property to the material–the shape memory effect. There is copious research on the structure and properties of the biodegradable face centred cubic (FCC) Fe-30Mn-6Si shape memory alloy (SMA) that exhibits the reversible FCC austenite to hexagonal close packed (HCP) ε-martensite transformation. However, recent advances in additive manufacturing of metals, brought by the development of the laser powder bed fusion (LPBF) technique, warrant the need for an investigation on the adaptability of the technique in fabricating this alloy composition. The LPBF technique is limited by the need for specialty raw material powder, and this thesis extends the application of the technique in fabricating the Fe-30Mn-6Si shape memory alloy (SMA) from homogenised powder precursors. More so, LPBF processing of Fe-30Mn-6Si alloy from either pre-alloyed powder or blended powder has not been reported. To successfully fabricate a Fe-30Mn-6Si LPBF product, the influence of key LPBF processing parameters on product quality was identified as a major challenge. This was addressed by investigating the influence of laser power, laser scan speed, laser re-scanning, and their equivalent input energy on the relative density and defect formation. A relative density of over 99% with few processing defects was achieved using the optimised parameters of 175 W laser power, 400 mm/s scan speed, and no re-scanning. The influence of these parameters on the solidification microstructure was also investigated using key techniques, such as X-ray diffraction (XRD) and scanning electron microscopy (SEM) in conjunction with energy dispersive spectroscopy (EDS) and electron backscatter diffraction (EBSD). Further, the simulated thermal profile of the melt pool region as a function of process parameters via single scan track experiments was calculated using the finite element method (FEM). These data were used to explain the key microstructural features observed in the as-solidified microstructure of the LPBF alloy as a function of the processing parameters. The mechanical properties of the LPBF alloy were then assessed by hardness and tensile testing and then compared with a reference alloy produced by arc melting. The hardness of the LPBF as-built alloy was ∼20% higher than the reference alloy. To identify the factors affecting the increased hardness of the former, the influence of grain size and morphology, crystallographic texture, phase constituents (mainly austenite and martensite), and residual strain were investigated. The hardness of the reference alloy was affected mainly by the grain size and residual strain, but for the LPBF-built alloy, the relative volume fractions of austenite and martensite strongly influenced the hardness. Meanwhile, the tensile properties of the LPBF alloy, such as the yield stress, ultimate tensile stress, and ductility, were adversely affected by the internal defects present, such that high temperature homogenisation and hot isostatic pressing (HIP) post-process treatments were investigated to improve these properties. The homogenisation and HIP treatments increased both the tensile strength and ductility of the LPBF-built alloy. Homogenisation altered the grain morphology by promoting recrystallisation and grain growth, and this increased the tensile strength by ∼80%. The hardness, however, decreased due to a reduction in the volume fraction of HCP martensite in the FCC austenitic microstructure. HIP retained some of the columnar microstructure generated by the LPBF process, marginally increased the density, and increased the tensile strength by ∼65%. The improvement in tensile properties through these post-process treatments allowed for the measurement of LPBF alloy’s shape memory behaviour, whereby a tensile recovery strain of 2% was achieved for the HIP-treated alloy. Finally, the biocorrosion behaviour of the LPBF-processed and HIP-treated alloy was investigated, whereby the in vitro corrosion potential and current density of the alloy were determined to be -769 mV and 5.6 μA/cm2, respectively, indicating a reasonable corrosion rate for this material. Overall, this thesis enabled the first demonstration of the shape memory effect in an LPBF-built Fe-based alloy fabricated from homogenised powder, an alloy which also exhibits biodegradable properties.
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(2022)ThesisIncreasing population and resource demands, a changing hydroclimate, and increasing risks of extreme events means that sustainable water management is more important now than ever before. Water planners are increasingly recognising that short instrumental records are insufficient to understand fully natural trends and variability in climate. High resolution paleoclimate proxies, like tree rings, can provide long time series of observations prior to the instrumental period, to better understand instrumental and pre-instrumental variability, the occurrence, trends, and drivers of extreme events, and provide insights into possible future hydroclimatic scenarios. However, tree-ring proxies are not evenly distributed in the landscape, and the South Pacific has very few high-resolution paleoclimate proxies to develop detailed reconstructions of climate variability. This thesis explores whether the relationships between tree-ring proxies in regions with strong teleconnections to the Pacific (i.e., ‘remote’ tree rings) can be exploited to reconstruct hydroclimatic indices across eastern Australia and the South Pacific Islands. Methods for hydroclimatic reconstruction are investigated, considering the unique challenges of the region: strong inter-annual and inter-decadal variability, very short data records, data gaps, and potential non-stationarities in climate teleconnections. Existing methods for tree-ring reconstructions have been successfully applied in the South Pacific (Chapter 2); however, overcoming the challenges posed by very short and non-continuous records required adaptations to existing methods (Chapter 3) and the development of new methods (Chapter 5). In the final two chapters, the thesis focuses on how catchment-scale tree-ring reconstructions can be most useful to water managers. In these chapters, methods of identifying, explaining, and representing extreme event frequency, return periods, and trends are explored, as are methods for using paleoclimate data along with climate model projections to help contextualise future risks of climate change. Overall, this thesis highlights the enormous potential of remote tree-rings for improving our understanding of past climate in the South Pacific. The reconstructions consistently demonstrate that the instrumental period underestimates the full range of natural climate variability and shows how century-long records provided by tree rings can help us better understand past climate drivers, contextualise the instrumental period, and refine estimates of future climate risks. This thesis builds upon a growing body of work that demonstrates the considerable value of tree-ring based reconstructions for current and future water resource decision making, most notably in remote regions that are highly vulnerable to climate change but where there are limited instrumental records. Maximising the potential of tree-ring data for water management will require ongoing collaboration between dendrochronologists and water managers.
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(2022)ThesisThere has been a rapid-growing market and academic enthusiasm for small wearable molecular diagnostic platforms driven by the growing demand for continuous monitoring of human health. Wearable devices need to be portable, stretchable, and ideally re-configurable to be able to work for different analytes. Such flexible physiological monitoring devices which are non-invasive or minimally-invasive represent the next frontier of biomedical diagnostics. They may make it possible to predict and prevent diseases or facilitate treatment by diagnosing diseases at the initial stages. However, there are many problems that restrict further applications of these devices. Firstly, there are a limited number of bio-materials which are highly flexible, biocompatible and have anti-fouling properties; such biomaterials are needed as substrates for wearable devices. Secondly, traditional biosensors used in wearable devices focus on the detection of physical signals (such as heartbeat) and small chemical molecules, e.g. Na+, K+. These are not sufficient to provide in depth health information which requires sensing of large molecules such as proteins, ideally in real time, which is currently challenging. This provides a motivation to develop highly sensitive wearable biosensors for the detection of large molecules in sweat. This thesis centres on the development of a bio-material based wearable device for continuous detection of crucial analytes in human sweat. To achieve this target, our first aim was to design a highly bio-compatible flexible material as a substrate for wearable devices. A tough and anti-fouling three-network hydrogel has been prepared by integrating a zwitterionic polymer network into a robust double-network hydrogel. Secondly, to fill the gap between technological development of continuous and non-invasive detection of different analytes in human sweat, a patterned sweat-based biosensor was created for the detection of key biomolecules. This sensor was produced by placing specific aptamers or enzymes on flexible working electrodes. In addition, nanotechnology methods have been applied to refine the bio-sensing interface to further increase the sensitivity of our sensors. Finally, a sample collection chip has been combined with our high sensitivity sensors to fabricate a wearable device for sweat bio-sensing purposes. Future research may involve integration of a commercially available wireless signal readout module with this wearable biosensing device. The outcomes of this work may provide new insights for the development of wearable devices for continuous measurement of a spectrum of analytes in sweat, as an important step towards point-of-care diagnostics
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(2022)ThesisDissolved organic carbon is stored and processed in groundwater in three ways. It is stored on minerals by adsorption, it is biologically processed through biodegradation, and it also undergoes a process to return to groundwater called desorption. This biophysiochemical research shows that the groundwater system is therefore a vital part of the global carbon cycle and carbon sink. This research fills a gap in the existing understanding of how to calculate the global carbon budget, as does not yet include the dissolved organic carbon that is stored in groundwater. This thesis exclusively explores processes determining dissolved organic carbon character and concentration in groundwater in different geological environments. This is new, useful knowledge to describe the biophysiochemical process. This research did not examine human interference in adding carbon to groundwater. This research found how dissolved organic carbon is stored and processed in groundwater due to biodegradation and desorption, and how it is adsorbed onto sediment surface. This research explored the characteristics and concentration of Dissolved organic carbon in groundwater by using Liquid Chromatography-Organic Carbon Detection, and other techniques, to examine dissolved organic carbon in terms of its fractions: humic substances, hydrophobic organic carbon, biopolymers, building blocks (BB), low molecular weight neutrals and low molecular weight acids. There were several key findings. First, the results showed that both semi-arid inland low sedimentary organic carbon environments – i.e., Maules Creek and Wellington – were a carbon source; while the high rainfall temperate coastal peatland environment of Anna Bay was a carbon sink. Secondly, another key finding was that dissolved organic carbon was not processed as a whole chemical compound, but it was processed by its fractions where each fraction was processed distinctly. For example, humic substances were only adsorbed/desorbed in groundwater; while low molecular weight neutrals were only consumed by microbes in the biodegradation process in groundwater.
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(2023)ThesisWith the rapid growth of e-commerce, the surging freight traffic is imposing unprecedented pressure on urban transport systems. To mitigate negative impacts of urban freight traffic, the integrated public transport system, i.e., urban co-modality, has been proposed to utilize the existing urban passenger transport system to also carry freight during off-peak hours. Despite the benefits, the co-modal system might reduce public transport reliability and demand due to freight loading/unloading and transshipment operations. This thesis focuses on understanding and modelling the emerging integrated co-modal system for passengers and freight, and investigating and managing its system-wide impacts. This thesis first uses the smart transit card data to understand the travel behaviour of public transport users, and quantify the impact of public transport reliability on users’ day-to-day travel choices. We find that public transport users tend to reserve safety margin for the unforeseen service unreliability. Besides, we also find that there was under-utilized capacity in transit services operating during off-peak hours, which indicates the potential for transporting freight in the public transport system. With the understanding of service-reliability-based travel choices, this thesis then models the mixed freight-passenger cross-type flow and strategic interactions among operators and users in a standalone co-modal system. We first construct a fundamental game-theoretical model based on the essential characteristics of the co-modal system, such as negative impacts of freight on passenger demand. In the fundamental model, we examine the strategic interaction between a transit operator and a freight operator. We show that introducing the co-modality has the potential to generate Pareto-improving outcomes for the operators. This model is extended by considering the endogenous interactions among freight customers, passengers, freight and transit operators. We find that the co-modal system may enhance levels of services for both passengers and freight customers. Building upon these, this thesis further explores the impact of the co-modal system on the freight transport market with outsourcing arrangements. The non-cooperative and cooperative games among a freight carrier, a freight integrator, and a transit operator are modelled, and the co-modal system performance is quantified.
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(2023)ThesisThe high cooling rates in metal additive manufacturing (AM) of high-entropy alloys (HEAs) can not only prohibit the formation of intermetallic compounds and detrimental elemental segregation but also facilitate microstructural refinement, thereby providing improved mechanical properties. However, there are still many challenges, including the presence of AM fabrication defects and residual stresses as well as anisotropic properties. Thus, further understanding is needed regarding applying post heat treatment to release residual stresses in as-built HEAs, and the techniques that can be employed to reduce or minimize the property anisotropy in as-built HEAs. In this thesis, a model Cantor alloy was fabricated and subject to a series of post heat treatment conditions. The results showed that annealing at a temperature lower than 900 °C gave rise to the formation of M23C6 carbides while recrystallization took place at temperatures over 900 °C. Interestingly, three distinct types of microstructures were exhibited at the annealing temperature of 900 °C. This is primarily attributable to the different thermal histories undergone through the LPBF process among these areas where heterogeneity in chemical elements and microstructure was revealed. The second group of samples were fabricated to develop a machine learning coupled microstructure mapping approach for tailoring mechanical property anisotropy. Three distinct types of microstructures were generated by varying the laser power and scanning speed, namely, herringbone, bimodal, and columnar microstructures. Epitaxial grain growth and side-branching in the melt pool center and overlapped regions are the main reasons responsible for the different microstructures. The underlying mechanisms were discussed in terms of effective grain size, heterogeneous microstructure, and the twinning induced plasticity (TWIP) effect. Subsequently, pre-deforamtion was applied before post heat treatment to study the influence of grain boundary engineering (GBE) on the recrystallization and resultant deformation behavior. Twinning-assisted recrystallization nucleation accelerated the formation of a nearly a fully recrystallized microstructure in the heavily deformed sample. As a result, the present strategy of GBE can provide further insight regarding the manipulation of the post heat treatment in as-built alloys particularly for those precipitation hardenable alloys where precipitation kinetics can be varied.
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(2023)ThesisDue to the unique photovoltaic properties and ease of fabrication, organic-inorganic halide perovskites have generated considerable research interest. The perovskite solar cell can be applied to many applications, by tuning the bandgap. Inter of Things (IoT) devices and tandem solar cell applications, in particular, have been required for the wide bandgap perovskite solar cells. However, wide bandgap perovskite solar cells have band alignment mismatch problems, leading to charge recombination at the interface of perovskite, resulting in encouraging low device performance and decrease device stability. The first part of this thesis includes the study of the structure and working mechanism of perovskite solar cells. In addition, the defect of the perovskite was explained about how the majority of defects formed. This is caused by shallow defect energies within the bandgap, low density of deep traps, and low trap-charge interaction cross-sections which are occurred during the interaction between traps and charges. After that, the explanation of the reason how wide bandgap is applied for the indoor application. There is previous work on the tuning of the band alignment between perovskite and hole transfer layer which improved the efficiency of hole transfer, resulting in high device performance under the low light intensity condition. Lastly, the experiment of the thesis is focused on the address of the band alignment mismatch by adding two dimensional (2D) BA2PbBr4 perovskite layer for the tunnelling effect between the electron transport layer (ETL) and perovskite layer. The tunnelling layer of 2D perovskite improved the 3D perovskite crystal quality and charge transport from the 3D perovskite to ETL. As a result, the power conversion efficiency under the 200 lux white light emitting diodes (LED) light for the IoT devices was 43.70% with around 1 V of open circuit voltage and improved the device stability under the 1000 lux of white LED up to 1200 hrs.