SACM - United Kingdom
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Item Restricted Plasmonic Metal Nanoparticles for Studying Complex Interactions and Dynamics in Biological Systems Using Surface-Enhanced Raman Spectroscopy: Insights from Biofilms(Queen's University Belfast, 2024) Aljuhani, Wafaa; J. Bell, Steven E.This PhD thesis addresses the challenges posed by complex biological systems on molecular detection and analysis using biofilms as a model system. Biofilms, with their sticky and heterogeneous extracellular matrix of polysaccharides, proteins and nucleic acids, exhibit strong matrix interference. The presence of multiple interacting components complicates the identification of specific interactions and alters the behavior of probing molecules or nanoparticles, affecting detection sensitivity and reproducibility. Surface-enhanced Raman spectroscopy (SERS) was used in this thesis as a robust, label-free analytical tool to investigate these challenges and advance its application for analyzing complex biological systems. In Chapter 3, interactions between SERS-active nanoparticles (Au and Agnanospheres and Au nanostars) and ex-situ biofilms were systematically studied. The ex-situ biofilm reduced SERS signals through impaired nanoparticle aggregation and surface site blocking. Aunanostars (NS), however, were less affected, providing reproducible signals, making them suitable for more complex in-situ biofilms. Building on this, SERS with NS was used to probe how interactions within ex-situ biofilms affect the detection of the antibiotics, levofloxacin and ampicillin. This study demonstrated, for the first time, label-free SERS detection of antibiotics in ex-situ biofilms at clinically relevant concentrations, although with reduced sensitivity. The decrease in sensitivity was attributed to interactions between biofilm components and the NS, which are governed by coupled equilibria rather than simple additive effects. Finally, SERS with NS was used to monitor levofloxacin diffusion within in-situ biofilms. By embedding NS at specific depths, Levo penetration was quantified using a label-free approach that allows direct detection of unmodified drug molecules while avoiding artefacts associated with fluorescence-based techniques. The method proved to be reproducible across multiple biofilm samples, demonstrating the reliability of SERS with NS for studying antibiotic transport and behavior in biofilms.17 0Item Restricted Characterization of trace metals in E-cigarettes(2023-11) Alanazi, Ahmed; Macphee, Donald; Mccue, AlanElectronic cigarettes (e-cigarettes) are devices that are designed to replace conventional cigarettes (Hartmann-Boyce et al., 2021). E-cigarettes are electronic devices that heat a liquid to produce a vapour for inhalation by users. They were invented to provide smokers with a safer and cleaner way to inhale tobacco and to enable them to cease their smoking habit. These types of cigarettes are considered to be safer than conventional cigarettes because they do not contain harmful tobacco; however, like conventional cigarettes, most contain nicotine – which is toxic and addictive – and the presence of other hazardous components is inherent in their design (Gaur & Agnihotri, 2018). The e-cigarette liquids, atomisers and aerosols are major sources of trace heavy metals, also known as trace elements (TEs), which pose risks to human health at certain concentrations in the body. TEs such as tin (Sn), nickel (Ni), aluminium (Al), chromium (Cr) and cadmium (Cd) leak from the core assembly (Jaishankar et al., 2014), while others such as lead (Pb) and zinc (Zn) are present in the liquid. Although some of these metals are essential elements at low doses, they are toxic at high concentrations, especially when they are inhaled. They are potentially carcinogenic and have been linked to the development of fatal health problems such as anaemia (US Centers for Disease Control and Prevention [CDC], 2022). Thus, although e-cigarettes are characterised as safer than conventional cigarettes, they can still pose a threat to human health. When a user smokes a conventional cigarette, the harmful elements in tobacco smoke enter the user’s nervous system (heart and vital organs) within a few seconds of the initial inhalation and subsequently affect many parts of the body. However, inhalation of vapourised electronic cigarette liquid (e-liquid) is becoming increasingly popular. This vapour is generally considered safer than the contents of conventional cigarette smoke. The active components of e-cigarettes are mixtures of propylene glycol (PG) and vegetable glycerine (VG) that contain different proportions of nicotine and flavouring (Stratton et al., 2018). The two most harmful components of tobacco smoke, tar and carbon monoxide, are absent from e-cigarettes, which are subject to strict safety and quality regulations. However, e-cigarettes still pose risks because they are only slightly safer than conventional cigarettes (Uchiyama et al., 2020). This research project was designed to investigate the source of TEs in e-cigarettes. The identified sources included the metal cover, inner clamp and wick. Inductively Coupled Plasma Mass Spectrometry (ICP-MS) was utilised to determine the levels at which various elements were present in e-cigarette samples. ICP-MS in single particle mode was used to determine the presence of nanoparticles. Due to the solubility properties of the e-liquids, many e-cigarettes contain dissolved TEs, such as Ni, Pb and Zn. The concentrations of VG and PG vary according to the e-liquid brand, so the proportions of TEs vary among e-cigarettes. There is a close relationship between a high concentration of VG and a high amount of TEs in e-cigarettes. In this project, increased ratios of VG to PG resulted in increased concentrations of TEs in the e-liquids. Parameters of the e-cigarettes, such as power and number of puffs, were studied and were discovered to influence the concentrations of TEs found in the e-liquids.53 0