Advanced fabrication strategies for functional soft materials: plasma, transient, and electrochemical approaches

Bowley, Emma Louise (2026) Advanced fabrication strategies for functional soft materials: plasma, transient, and electrochemical approaches. PhD thesis, University of Glasgow.

Abstract

Supramolecular soft materials derived from low molecular weight gelators (LMWG) have been widely prepared using pH-switching strategies, in which the method of inducing the pH change plays a critical role in determining material properties and applications. In this thesis, three distinct pH-switching approaches were explored. Although each approach relies on a change in pH, it has been demonstrated that they produce materials with significantly different behaviours, structures, and functionalities.

In chapter 2, plasma-induced gelation was investigated as a novel route for the in situ fabrication and 3D printing of supramolecular hydrogels. It was demonstrated that cold atmospheric plasma enables precise spatial and temporal control over gelation, allowing the formation of complex, patterned, and multilayered structures with defined geometries. Studies using Kineticolor showed that gelation is driven by plasma-induced pH changes. It was further demonstrated that this approach can be combined with the in situ formation of gold nanoparticles, enabling the fabrication of composite hydrogels with enhanced functionality.

In Chapter 3, transient pH-switching systems were explored by combining a urea/urease reaction with formate hydrolysis in DMSO/H₂O hydrogel systems. The scope of the system was expanded by incorporating a range of LMWGs, and it was demonstrated that variation of the ester component, including methyl, ethyl, and n-propyl formate, allows control over hydrolysis rates and thus temporal behaviour. The effects of temperature and ageing were also investigated, revealing complex, non-linear, and sometimes unpredictable dynamics that are important for practical applications.

In chapter 4, these pH triggers were further applied to a lipid-based system, where it was demonstrated that they can induce and control phase transitions in a monoolein-oleic acid mixture. Using flow-through small-angle X-ray scattering transitions, including Pn3m-to-HII, HII-to-Im3m, and HII-to-Im3m-to-HII, were successfully realised. It was shown that these nanoscale structural changes significantly influence the macroscopic properties of the materials, highlighting the versatility of transient pH control across different supramolecular systems.

Finally, in chapter 5, electrochemically induced gelation and polymerisation of carbazole-functionalised amino acid-based hydrogels were investigated. In situ electrochemical small-angle X-ray scattering was used to examine the dynamic processes of self-assembly and polymerisation, showing how subtle molecular changes govern structural evolution and material properties.

Overall, this thesis demonstrates that the choice of gelation method enables tailoring of material structure, dynamics, and functionality across multiple length scales.

• Item Type: Thesis (PhD)
• Qualification Level: Doctoral
• Subjects: Q Science > QD Chemistry
• Colleges/Schools: College of Science and Engineering > School of Chemistry
• Supervisor's Name: Adams, Professor Dave
• Date of Award: 2026
• Depositing User: Theses Team
• Unique ID: glathesis:2026-86135
• Copyright: Copyright of this thesis is held by the author.
• Date Deposited: 16 Jul 2026 14:54
• Last Modified: 19 Jul 2026 06:36
• Thesis DOI: 10.5525/gla.thesis.86135
• URI: https://theses.gla.ac.uk/id/eprint/86135

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