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

Available for download on Wednesday, August 12, 2026

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