Identifier

etd-06032015-181706

Degree

Doctor of Philosophy (PhD)

Department

Engineering Science (Interdepartmental Program)

Document Type

Dissertation

Abstract

Millifluidics can be used as a simple tool and convenient platform to perform in-situ investigations on nanoparticles synthesis to generate real-time information in a continuous flow fashion. These investigations can be used to observe the relationship between the structure and performance of nanoparticles for catalytic applications as a function of space and time. These improvements in nanoparticles research offer unique advantages to develop catalysts with molecular strategies. In order to showcase these advantages of the millifluidic reactors, here we: A. Extensively covered a complete literature review on Lab-on-a-chip devices for gold nanoparticle synthesis and as a catalyst support for continuous flow catalysis. This first phase of the work provides detailed information on the synthesis and catalysis applications of nanostructured gold using the lab-on-a-chip systems. The second phase is an experimental investigation, where the millifluidic reactor was used for: B. Continuous flow process for production of water-soluble Platinum-Dimercaptosuccinic acid (Pt(DMSA)) nanoparticles at ambient conditions. The process development was based on in-situ synchrotron radiation-based X-ray absorption spectroscopy (XAS) investigations. The XAS revealed that the nucleation and growth of the Pt(DMSA) nanoparticles was extremely fast. Such a fast nucleation and growth process was also found to hinder coating of the channel walls, except at the zone 1 where the reactants first interact. C. Catalytic oxidation of 5-(Hydroxymethyl)furfural (HMF) to 2,5-Furandicarboxylic acid (FDCA) with nanostructured gold catalyst using millifluidics. The conversion leading from the reactant to primary and secondary products within the millifluidic reactor was analyzed at various spatial intervals to understand the reaction mechanism. The entire process was carried out using an aqueous phase oxidizing agent, tert-Butyl hydroperoxide (TBHP) at ambient temperature and pressure in a continuous flow conditions. The turnover frequency for the catalytic oxidation of HMF using the millifluidic reactor was obtained in the order of 10-26 molecules s-1 in for HMFCA and FDCA after 50 minutes. The results demonstrated in this work highlight significant advantages in carrying out time-resolved continuous flow catalytic reactions using millifluidic reactors.

Date

2015

Document Availability at the Time of Submission

Secure the entire work for patent and/or proprietary purposes for a period of one year. Student has submitted appropriate documentation which states: During this period the copyright owner also agrees not to exercise her/his ownership rights, including public use in works, without prior authorization from LSU. At the end of the one year period, either we or LSU may request an automatic extension for one additional year. At the end of the one year secure period (or its extension, if such is requested), the work will be released for access worldwide.

Committee Chair

Theegala, Chandra S.

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