- Title
- Photocatalytic reduction of CO2 into green fuels on microspherical nanocomposites comprising of CdS, TiO2, ZnFe2O4 semiconductors and heterojunctions
- Creator
- Mudau, Rendani Julian
- Subject
- Heterojunctions
- Subject
- Chemistry, Inorganic
- Subject
- Nanochemistry
- Date Issued
- 2024-04
- Date
- 2024-04
- Type
- Master's theses
- Type
- text
- Identifier
- http://hdl.handle.net/10948/64214
- Identifier
- vital:73665
- Description
- Human anthropogenic activities have led to an increase in CO2 levels resulting in global warming. There is a need to reduce CO2 levels in the atmosphere by capturing the gas and converting the captured CO2 into fuels. Photocatalytic conversion of CO2 into valuable products via photoreduction is a promising technique to reduce carbon dioxide using sunlight and water. Redox reactions between CO2 and water using photocatalysts offer an effective method of lowering CO2, which has detrimental effects on the environment. This dissertation reports the synthesis and characterization of five photochemical catalysts comprising of CdS, TiO2, ZnFe2O4 semiconductors and heterojunctions and their use as photocatalysts for the photocatalytic reduction of CO2 into green fuels. Mott−Schottky plot of TiO2, CdS and CdS/TiO2 confirmed the formation of n-type, n-type, and n-n type material respectively. The band gap of TiO2, CdS, and CdS/TiO2 obtained were 3.21,2.24, 2.04 eV, respectively, the combination of TiO2 and CdS resulted in the lowering of band gap energy which is favourable for photocatalytic reduction studies. XRD of TiO2, CdS and CdS/TiO2 provided relevant information about the various phase reflections of the photocatalysts, it also supported reports confirming the increase in crystallite size of TiO2 anatase phase upon calcination. Chemical environment of the various photocatalysts, such as Ti2p1/2, Ti2p3/2, O1s, Cd3d3/2, Cd3d5/2, S2p1/2 and S2p3/2 were observed in TiO2, CdS and CdS/TiO2. BET surface area of TiO2, CdS and CdS/TiO2 was also observed to be 2.9243, 4.0605, and 9.8450 m2g, respectively. Photocatalytic reduction of CO2 resulted in formic acid, formaldehyde, acetic acid, carbon monoxide, ethanol, and methanol after 12 h. Modification of CdS with TiO2 to form CdS/TiO2 produced high yield of formic acid (217.7 μmol/g) compared to CdS (8.7 μmol/g) and TiO2 (122.5 μmol/g). CdS had high yield of formaldehyde (20.4 μmol/g) and ethanol (57.8 μmol/g) compared to TiO2 (12.9, 3.6 μmol/g of formaldehyde and ethanol, respectively) and CdS/TiO2 (19.7 μmol/g and there was no detection of ethanol). TiO2 shows high yield of methanol (145.2 μmol/g) and is the only catalysts that produced carbon monoxide (52.2 μmol/g) compared to CdS (87.8 μmol/g of methanol) and CdS/TiO2 (50.2 μmol/g of methanol). A detailed elucidation of the various products was reported by means of nuclear magnetic resonance (NMR) spectrometer. ZnFe2O4 and CdS/TiO2/ZnFe2O4 were characterized and employed for photocatalytic reduction of CO2 in water. XRD and XPS confirmed the presence Fe (2+) and Fe (3+) in tetrahedral/octahedral and Zn (2+) in tetrahedral on ZnFe2O4 and CdS/TiO2. CdS/TiO2/ZnFe2O4 presented a lowered band gap of 1.98 eV due to the presence of ZnFe2O4 while the band gap of ZnFe2O4 obtained is 1.95 eV. The Mott-Schottky plots confirmed the conduction (2.81 and 2.59 eV) and valence band (–0.86 and –6.1 eV) of ZnFe2O4 and CdS/TiO2/ZnFe2O4 together with their junctions, respectively. ZnFe2O4 and CdS/TiO2/ZnFe2O4 are p-type and p-n type junctions, respectively. Photocatalytic reduction of CO2 under visible light for 12 h using CdS/TiO2/ZnFe2O4 hollow microspheres nanocomposites produced methanol (182.1 μmol/g), formic acid (1.9 μmol/g), formaldehyde (9.5 μmol/g), ethanol (67.1 μmol/g), and oxalic acid (38.9 μmol/g). Amongst the synthesized catalysts, CdS/TiO2/ZnFe2O4 produced high yield of methanol, ethanol, and oxalic acid.
- Description
- Thesis (MSc) -- Faculty of Science, School of Computer Science, Mathematics, Physics and Statistics, 2024
- Format
- computer
- Format
- online resource
- Format
- application/pdf
- Format
- 1 online resource (157 pages)
- Format
- Publisher
- Nelson Mandela University
- Publisher
- Faculty of Science
- Language
- English
- Rights
- Nelson Mandela University
- Rights
- All Rights Reserved
- Rights
- Open Access
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| Thumbnail | File | Description | Size | Format | |||
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