This thesis presents investigations into the design and synthesis of nanomaterials in supercritical carbon dioxide (sc-CO₂) as well as novel experimental design methodologies. First, the process-structure-property relationships are studied for the deposition of materials from organometallic precursors in sc-CO₂. The materials that were investigated in these studies were: (1) the semiconductor material copper zinc tin sulfide (Cu₂ZnSnS₄, or CZTS), which has application in solar energy capture; (2) zinc sulfide nanoparticles deposited onto carbon nanotubes, which have application in optoelectronics; and (3) silver nanoparticles deposited on silicon and glass wafer surfaces, which find application as biosensors via surface enhanced Raman spectroscopy. Next, two novel experimental design methodologies were implemented. The first is termed layers of experiment with adaptive combined design (LoE/ACD), which efficiently optimizes a process that is expensive and time consuming to study by zooming in on the process optimum through successive layers. The mean silver nanoparticle size was optimized as a function of temperature in the sc-CO₂ system using the LoE/ACD approach. The second experimental design methodology is called initial experimental design (IED). The IED methodology was developed to choose the first round of experiments for a system that is expensive to study (in terms of time and money), poorly understood, and possesses a related, non-identical system that is well-studied. The IED approach was used to optimize the mean iridium nanoparticle size as a function of temperature given expert opinion, prior data, and an engineering model for silver nanoparticles synthesized in sc-CO₂.
| Identifer | oai:union.ndltd.org:GATECH/oai:smartech.gatech.edu:1853/49059 |
| Date | 20 September 2013 |
| Creators | Casciato, Michael John |
| Contributors | Grover, Martha A., Hess, Dennis W. |
| Publisher | Georgia Institute of Technology |
| Source Sets | Georgia Tech Electronic Thesis and Dissertation Archive |
| Language | en_US |
| Detected Language | English |
| Type | Dissertation |
| Format | application/pdf |
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