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Title: Metal-loaded graphitic carbon nitride for photocatalytic hydrogen production and the development of an innovative photo-thermal reactor
Author: Caux, Marine
ISNI:       0000 0004 7234 4021
Awarding Body: University of St Andrews
Current Institution: University of St Andrews
Date of Award: 2018
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The path towards mitigation of anthropogenic greenhouse gas emissions lies in the transition from conventional to sustainable energy resources. The Hydrogen Economy, a cyclic economy based on hydrogen as a fuel, is suggested as a tool in the necessary energy transition. Photocatalysis makes use of sunlight to promote thermodynamically non-favoured reactions such as water splitting, allowing for sustainable hydrogen production. Harvesting thermal energy along with photonic energy is an interesting concept to decrease the activation energy of water splitting (i.e. ΔG = + 237.2 kJ∙mol−1). This work aims to confront this hypothesis in a gas phase photo-thermal reactor designed specifically for this study. The photocatalyst chosen is graphitic carbon nitride (g-C3N4), an organic semiconductor possessing a narrow band gap (i.e. 2.7 eV) as well as a band structure which theoretically permits water splitting. The photocatalytic performance of Pt/g-C3N4 for hydrogen evolution was tuned by altering its synthetic temperature. Electron paramagnetic resonance was used to gain insight on the evolution of the photocatalyst activity with synthesis temperature. Then, gold nanoparticles were deposited on g-C3N4 surface. Localized surface plasmon resonance properties of gold nanoparticles are reported in the literature to be influenced by temperature. Therefore Au/g-C3N4 appeared as a promising candidate for photo-thermal water splitting. X-ray spectroscopy unveiled interesting observations on the gold oxidation state. Moreover, under specific reduction conditions, gold nanoparticles with a wide variety of shapes characterized by sharp edges were formed. Finally, the development of the photo-thermal reactor is presented. The design process and the implementation of this innovative reactor are discussed. The reactor was successfully utilized to probe photoreactions. Then, the highly energy-demanding photocatalytic water splitting was proven not to be activated by temperature in the photo-thermal apparatus.
Supervisor: Irvine, John T. S. Sponsor: Sharikah al-Saʻūdīyah lil-Ṣināʻāt al-Asāsīyah (SABIC)
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: Electron paramagnetic resonance ; X-ray photoelectron spectroscopy ; Photocatalysis ; Hydrogen evolution ; Graphitic carbon nitride ; Liquid and gas phase catalysis ; Photo-thermal reactor ; Gold nanoparticle growth ; QD716.P45C2 ; Hydrogen as fuel ; X-ray spectroscopy ; Nanoparticles