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Porous Materials and Their Applications in Catalysis and Adsorption

Date Issued
2015
Date
2015
Author(s)
Hong, Chen-Yu
URI
http://ntur.lib.ntu.edu.tw//handle/246246/272009
Abstract
Porous nanoparticles are highly effective as catalysts because of a well-oriented structure, large surface area and uniform pore size. Metal oxides with a porous structure are widely used to augment optical characteristics and conversion efficiency. This dissertation focusses on applications of mesoporous titania/zirconia nanoparticles (MTNs/MZrNs) and dealuminated beta zeolite (deAl BEA). A thin film of gold nanoparticles inlaid with mesoporous titania nanoparticles (Au@MTNs) was fabricated on a conductive plastic substrate using low-temperature electrophoretic deposition (EPD) followed by a compression post-treatment. The resulting Au@MTNs electrode exhibits excellent light trapping performance thanks to the formation of surface plasmons on the Au nanoparticles (NPs). The use of 0.8 wt% Au NPs in the Au@MTNs photoanode resulted in power conversion efficiency (η) of 5.62% under illumination of 100 mW cm–2. This represents a 14% improvement in conversion efficiency, compared to the DSSC fabricated using pure a titanium dioxide (TiO2) photoanode (4.93%), due to the plasmonic light trapping provided by the Au NPs. Our aim was to study the relationship between 5-fluorouracil (5FU)/disulfiram (DSF) and various framework zeolites. The 5FU and DSF respectively deemed a hydrophilic and a hydrophobic guest molecule to observe the adsorption on MFI, BEA and FAU zeolites. Three isotherm models were fitted and discussed in 5FU loaded zeolite isotherm. The 5FU/DSF loading amount can be attributed to the chelating effect, hydrogen bond, Van Deer Waal interaction, and size of pores in the zeolite. The deAl BEA reached a high 5FU loading as FAU zeolite because of the structure defects. The DSF furthermore served as a cap to prolong the 5FU release. MZrNs and Sn_MZrNs were synthesized and applied in pyruvaldehyde to perform a methyl lactate reaction. Amorphous MZrNs were first reported in this study to demonstrate high catalytic activity. In addition, Sn_MZrNs exhibit a large surface area in amorphous particles and a mixing tetragonal/monoclinic crystallite after hydrothermal treatment. Tin synthesized inside the MZrNs provided strong Lewis acid sites, which strengthened the Meerwein–Ponndorf–Verley reductions/Oppenauer oxidations and achieved 90% methyl lactate conversion. The high conversion rate and efficiency are attributed to a high surface area and tetragonal structure of Sn_MZrNs.
Subjects
mesoporous materials
mesoporous titania nanaoparticles (MTNs)
mesoporous zirconia nanoparticles (MZrNs)
dealuminated beta
flexible dye sensitized solar cells (flexible DSSC)
5-fluorouracil (5FU)
methyl lactate
Type
thesis

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