DOI
https://doi.org/10.25772/GJMW-JC82
Author ORCID Identifier
https://orcid.org/0000-0003-1506-0260
Defense Date
2021
Document Type
Dissertation
Degree Name
Doctor of Philosophy
Department
Chemical and Life Science Engineering
First Advisor
B. Frank Gupton
Second Advisor
Carlos E. Castano L.
Third Advisor
Christina Tang
Fourth Advisor
James K. Ferri
Fifth Advisor
Anne M. Gaffney
Abstract
Transition metal heterogeneous catalysts are widely used across many chemical industries to reduce waste and emissions and reduce production time while increasing rate. The prevalence of these materials results from the complex relationship between metal nanoparticles and supports affecting final catalytic performance. Rational catalyst synthesis describes the ability to precisely engineer structures through controlled preparation. Novel materials and continuous processing represent a promising approach for rational catalyst synthesis.
The application of these catalysts in continuous, multiphase processes, such as cross-coupling reactions, oxidation chemistry, and nitroreduction processes, are paramount to developing new commercial routes for high-value products. Pd/G catalysts synthesized by flow MW irradiation for cross-coupling reactions exhibited remarkable durability, only 347 ppb Pd leached. Implementing a tube-in-tube sparge with a packed bed increased reactor productivity (STY) 4-fold for the oxidation of BA in flow. A flow nitroreduction process was optimized with a Pd/C catalyst to mitigate water accumulation and increase STY by a factor of 10 over 6.5 h with no loss in activity or fouling.
Silver epoxidation catalysts are perhaps one of the most important industrial catalysts for EO synthesis. Direct PO synthesis by Ag catalysts represent a “holy grail” in chemical catalysis. Ag supported on CaCO3 and α-Al2O3 were prepared with different amounts of K+ promoter (0 – 19000 ppmw) and feed additives (EtCl, NO; 0 – 400 ppmv) to evaluate their effects on PO selectivity and propylene conversion. The subsequent investigation into the fundamental nature of epoxidation represents the culmination of synthesis, characterization, and kinetics of novel reacting systems.
Rights
© The Author
Is Part Of
VCU University Archives
Is Part Of
VCU Theses and Dissertations
Date of Submission
8-13-2021
Included in
Catalysis and Reaction Engineering Commons, Nanoscience and Nanotechnology Commons, Other Materials Science and Engineering Commons, Thermodynamics Commons