Advanced Synthesis and Rational Design of Support Structures for Nobel Metal Heterogeneous Catalysis: Towards Enhanced Activity and Continuous Processes

Author

Brian R. Clark, Virginia Commonwealth UniversityFollow

Author ORCID Identifier

https://orcid.org/0009-0005-2406-3772

Defense Date

2024

Document Type

Dissertation

Degree Name

Doctor of Philosophy

Department

Chemical and Life Science Engineering

First Advisor

Frank Gupton

Second Advisor

James Ferri

Third Advisor

Nastassja Lewinski

Fourth Advisor

Everett Carpenter

Fifth Advisor

Katharine Tibbetts

Abstract

The field of catalysis has a wide-ranging impact. Our group has identified the constant need for improved catalytic activity in high-impact applications such as hydrosilylation and cross-coupling reactions. For these reactions, precious metal catalysts often exhibit markedly better performance than their counterparts, but they can be a significant process cost that decreases overall economic efficiencies. To address this challenge, we explored support structures that can enhance catalytic activity at low metal loadings and improve precious metal recovery through simple filtration. We found that a platinum on graphene nanoplatelet catalyst (PtGNP) synthesized via strong electrostatic adsorption with microwave irradiation (SEA-MW) exhibits high activity compared to the industrially relevant Karstedt’s catalyst for hydrosilylation reactions. Due to the inherent high surface area of the GNPs, we focused our attention on developing a more robust catalyst for their use in packed bed reactors. We successfully developed a facile method for depositing GNPs onto 0.5 mm gamma-alumina particles. We used a modified controlled surface tension method to reduce platinum nanoparticles onto the surface of the GNP/alumina material. The resulting catalyst performed exceptionally well in a packed bed, generating pressures that were easily handled on a commercially available packed bed reactor platform. Lastly, we deployed a rational design approach toward a 3D printed fixed bed reactor that could be functionalized with active palladium nanoparticles for Suzuki cross-coupling reactions. The intended benefit of this approach is to provide practical, efficient, and low-cost methods for the synthesis and use of precious metal nanoparticles.

Rights

© Brian Clark

Is Part Of

VCU University Archives

Is Part Of

VCU Theses and Dissertations

Date of Submission

8-9-2024