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dc.contributor.advisorIrvine, John T. S.
dc.contributor.authorFina, Federica
dc.coverage.spatial205en_US
dc.date.accessioned2015-03-25T14:37:15Z
dc.date.available2015-03-25T14:37:15Z
dc.date.issued2014-12-01
dc.identifier.urihttp://hdl.handle.net/10023/6322
dc.description.abstractThe need for green and renewable fuels has led to the investigation of ways to exploit renewable resources. Solar among all the renewables is the most powerful and its conversion into usable energy would help in solving the energy problem our society is facing. Photocatalytic water splitting for hydrogen production is an example of solar energy storage into chemical bonds. The hydrogen produced in this way can then be employed as carbon free fuel creating the “Hydrogen Cycle”. This work investigates the structure and the activity of graphitic carbon nitride (g-C₃N₄), an organic semiconductor that proved a suitable photocatalyst for hydrogen production from water. Synthesised by thermal polycondensation of melamine it is a graphitic like material with a band gap of 2.7 eV which makes it a visible light active catalyst. In a first instance the effect of the synthesis conditions on its structure and morphology are investigated to find the optimum parameters. The temperature of condensation is varied from 450°C up to 650°C and the length from 2.5 h to 15 h. The structural changes are monitored via X-ray diffraction (XRD) and elemental analysis while the effect on the morphology and the band gap of g-C₃N₄ are investigated by mean of scanning electron microscopy and UV-Vis absorption. Subsequently, a study of the crystal structure of the catalyst is carried out. Using structures proposed in the literature, X-ray diffraction and neutron scattering simulations are used to narrow down the number of possible 3D structures. After structural characterisation, the activity of g-C₃N₄ for photocatalytic hydrogen evolution is evaluated. It is confirmed that loading 1 wt.% Pt on its surface significantly increases the hydrogen evolution rate. The attention then focuses on the loading procedures, the reduction pre treatments of the co-catalyst and the reasons of the different performances when different procedures are employed. The catalytic system is characterised by means of X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and XRD. By investigating the composition and the morphology of the platinum nanoparticles under different conditions, the main factors responsible for the changes in activity of g-C₃N₄ for hydrogen evolution are identified. Additionally, the role of the co catalyst and its interaction with g-C₃N₄ is also elucidated. Finally, taking forward the knowledge acquired on the Pt-g-C₃N₄ system, the effect on the hydrogen evolution rate of alloying platinum with a second metal (Cu, Ag, Ni and Co) is studied. The nanoparticles are characterised by XRD and TEM. A screening of the loading procedures and bimetallic systems is performed to identify the most promising for photocatalytic hydrogen evolution with the aim of bringing them towards further investigation.en_US
dc.language.isoenen_US
dc.publisherUniversity of St Andrews
dc.rightsCreative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/
dc.subjectHydrogen evolutionen_US
dc.subjectGraphitic carbon nitrideen_US
dc.subjectPlatinumen_US
dc.subjectNanoparticlesen_US
dc.subjectBimetallic alloyen_US
dc.subject.lccQD716.P45F5
dc.subject.lcshPhotocatalysisen_US
dc.subject.lcshCatalysts--Synthesisen_US
dc.subject.lcshHydrogen as fuelen_US
dc.subject.lcshWater--Electrolysisen_US
dc.subject.lcshPlatinum alloysen_US
dc.subject.lcshNanoparticlesen_US
dc.titleMetal loaded g-C₃N₄ for visible light-driven H₂ productionen_US
dc.typeThesisen_US
dc.type.qualificationlevelDoctoralen_US
dc.type.qualificationnamePhD Doctor of Philosophyen_US
dc.publisher.institutionThe University of St Andrewsen_US


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Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
Except where otherwise noted within the work, this item's licence for re-use is described as Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International