Doctor of Philosophy
Chemical and Life Science Engineering
Dr. B. Frank Gupton
Dr. Carlos E. Castano
Herein, a wholistic analysis of the viability of monolithic catalysts for redox reactions is presented. The interdisciplinary approach taken in this systematic study included preparation and investigation on Pd-on-carbon monoliths as catalysts in a flow and electrochemical settings.
The Suzuki-Miyaura reaction-focused study led to rational design, preparation, and successful application of Pd0-on-graphene oxide (GO) monolithic catalysts in flow conditions. In this study a combination of chemical reduction, freeze-casting, and vapor-phase reduction processes was applied to Pd-GO structures leading to the preparation of these monoliths. The Suzuki flow synthesis reactions revealed that the monolithic structure led to significantly improved catalytic longevity compared to 2D solid-supported catalysts. Nonetheless, the turnover frequency and product metal contamination (leaching-off) analysis indicated superior performance for monolithic catalysts.
Electrochemical Wacker-type oxidations are among the most common reactions in the industry. However, in order to prepare a rationally designed monolithic catalyst for this reaction, further catalyst studies were required. Therefore, a comprehensive study on 2-dimensional Pd-on-graphene nanoplatelets was conducted, leading to a proposed industrial design space for oxidation catalyst manufacturing. Afterwards, as a proof of concept viability of PdII-on glassy carbon (GC) monoliths were used as catalytic electrodes for Wacker-type oxidation in the electrochemical setting.
Via this approach, a comprehensive investigation and validation of monolithic catalyst preparation and applications in industrially feasible synthetic processes, including catalytically different redox reactions in flow and electrochemical settings, were successfully attained.
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Available for download on Thursday, August 05, 2021