Thesis

Conjugated polymers for photocatalytic hydrogen production from water and photocatalytic CO2 reduction

Creator
Rights statement
Awarding institution
  • University of Strathclyde
Date of award
  • 2026
Thesis identifier
  • T17670
Person Identifier (Local)
  • 202193294
Qualification Level
Qualification Name
Department, School or Faculty
Advisor / supervisor
  • Sprick, Reiner Sebastian
Resource Type
Note
  • Net Zero by 2050 remains one of the most pressing challenges facing human prosperity. Renewable energy is strongly desired to eliminate our dependence on fossil-fuel-derived energy sources, whilst building blocks essential for sustaining human life need to be produced by alternative feedstocks to fossil fuels. Photocatalytic hydrogen production from water is a promising strategy to use hydrogen for solar energy storage. Also, photocatalytic CO2 reduction is an attractive process to generate carbon-derived fuels and useful products for the chemical industry as an alternative to coal, oil and gas feedstocks. Conjugated polymers are semiconducting materials which have emerged as photocatalysts to facilitate these light-driven transformations. A major advantage is solution-processability and optoelectronic tuneability to target scale-up and efficient harvesting of visible light alike. Concerning hydrogen production, solution processable conjugated polymers were developed and systematically studied to elucidate structure-activity relationships that lead to high photocatalytic performance. Wettability was found to be one of the most important factors to enhance activity since conjugated polymers with hydrophilic side-chains significantly outperformed counterparts with hydrophobic side-chains. The scalability benefits of solution processable materials were demonstrated by studying films and nanoparticulate aqueous dispersions. In the latter case, donor-acceptor heterojunction nanoparticles were investigated using combinations of conjugated polymers with energetic offsets to induce heterojunctions. The goal was to contribute to the most efficient systems already reported and some specific systems were found to be promising to develop. Concerning photocatalytic CO2 reduction, this was enabled using conjugated polymers incorporated into hybrid photocatalyst systems. The combination of the polymers and supramolecular photocatalysts enabled new competitive materials for visible-light driven CO2 conversion to formate. The P10 hybrid photocatalyst enabled quantitative CO2 reduction, whilst highly concentrated solutions of formate were achieved by direct photocatalytic conversion for the first time. This development shifts the process closer to implementation and further optimisation strategies are envisaged to aid the transition to real-world application.
DOI
Date Created
  • 2025
Embargo Note
  • This thesis is restricted to Strathclyde users only until 13th March 2031.

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