Fluorescent carbon dots are a new class of carbon nanomaterials that have emerged recently, and have created a lot of interest as a potential competitor to classical semiconductor quantum dots. Carbon dots possess low toxicity, biocompatibility, easy and low-cost synthesis, and good optical properties. They show huge potential as novel and versatile nanomaterials for a wide range of applications such as bioimaging, drug delivery, chemical sensing, photocatalysis, and as sensitizers for photovoltaic solar cells. The main motivation for this research was the need to produce non-toxic, low-cost nanomaterials with good optical and electrical properties for the use in the fabrication of sustainable, inexpensive nanostructured solar cells with good efficiency. The main aims and objectives of this PhD research were: to synthesize fluorescent carbon dots from biomass-derived precursors by using the hydrothermal synthesis method, to understand and explain structural and optical properties of the as-synthesized carbon dots, and to use the carbon dots as sensitizers for nanostructured solar cells. Carbon dots (CDs) were synthesized using hydrothermal synthesis method from polysaccharides (chitosan and chitin), monosaccharide (D-glucose), amino acids (L-arginine and L-cysteine), and from real food waste in the form of lobster shells. Carbon dots were thoroughly characterized to obtain the information about their structural and optical properties. The as-synthesized carbon dots showed polydispersity and quasi-spherical morphology, with particle sizes ranging from 5-17 nm. Carbon dots showed predominantly amorphous nature, and the functional groups from the starting precursors were successfully incorporated into the as-synthesized carbon dots. Diluted solutions of carbon dots were transparent under daylight and showed blue-green photoluminescence emission under UV excitation. All carbon dots showed excitation-dependent photoluminescence emission which was more pronounced for excitation wavelengths larger than 320 nm. Chitosan CDs, L-cysteine CDs and lobster CDs also showed excitation-independent emission for excitation wavelength in the range of 200 - 320 nm. The highest fluorescence quantum yield of (43.3 ± 2.1) % was calculated for L-arginine CDs. It was concluded that the origin of light emission in carbon dots must be governed by the interplay between the absorption due to the carbon cores and the surface functional groups. Considering the application of the as-synthesized carbon dots, two types of solar cells were fabricated. Carbon dots were used as sensitizers for ZnO-nanorod-based and for TiO2-based nanostructured solar cells. Three types of carbon dots (chitosan CDs, chitin CDs and D-glucose CDs) were used as sensitizers for ZnO-nanorod-based solar cells. ZnO nanorods were successfully coated with carbon dots, and the chitosan-CDs-sensitized solar cells showed the efficiency of 0.061 %. When using layer-by-layer coating method, solar cells with combination of chitosan- and chitin-CDs as sensitizers showed the efficiency of 0.077 %. All six types of carbon dots (chitosan CDs, chitin CDs, D-glucose CDs, L-arginine CDs, L-cysteine CDs, and lobster CDs) were used as sensitizers for TiO2-based nanostructured solar cells. TiO2-based solar cells sensitized with carbon dots showed much higher efficiency compared to the ZnO-nanorod-based solar cells. L-arginine-CDs sensitized TiO2-based solar cells showed the highest efficiency of (0.362 ± 0.007) %, which was the best efficiency of all fabricated solar cells. By surveying a range of biomass-derived carbon dots, and demonstrating a clear link between functionalisation and solar cell performance, this PhD research project provides a guide to direct future development of low-cost, biomass-derived sensitizers for nanostructured solar cells.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:765805 |
| Date | January 2016 |
| Creators | Marinovic, Adam |
| Publisher | Queen Mary, University of London |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | http://qmro.qmul.ac.uk/xmlui/handle/123456789/23291 |
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