Homogeneous flow catalysis strategies for lab-scale kinetic investigation and reaction development

Predicated on vapor-liquid separations, we have developed methodologies to effectively immobilize homogeneous organometallic catalysts within a continuous reactor. Compared to the traditional investigation of these catalysts in a batch system, our advanced analysis under steady-state flow provides chemical insight that is not, otherwise, easily accessible. In this dissertation, we detail the design and implementation of these flow methodologies; and overall, the accumulation of our efforts demonstrates the benefit of coupling engineering and chemistry fundamentals toward the development of meaningful catalytic reactions. Chapter 1 contains a brief introduction to catalysis in addition to a mini-review of separation technologies used for the continuous processing of homogeneous catalysts. In Chapter 2, we introduce the catalytic ethanol coupling reaction (the Guerbet reaction), and we provide a detailed mechanistic investigation of a homogeneous ruthenium catalyst within a continuously stirred tank reactor. In a second project described in Chapter 3, we develop supported liquid phase catalysts to effectively immobilize two organometallic complexes for study in a packed bed reactor. We begin Chapter 4 with a summary of current polyolefin depolymerization strategies prior to introducing a new chemical depolymerization technique. By implementing tandem catalytic reactions (dehydrogenation, isomerization, and metathesis) we seek to selectively convert polyethylene to monomer (propylene and butene). Chapter 5 contains an extension of our depolymerization efforts to several promising heterogeneous catalysts.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Chemical Engineering

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2022

Author dc:creator

• Wang, Nicholas Mason

Contributors dc:contributor

• Guironnet, Damien S.
• Peters, Baron G.
• Zimmerman, Steven C.
• Su, Xiao

• Flow Chemistry
• Organometallics
• Heterogenization
• Reactor Engineering

Statement dc:rights

• Copyright 2022 Nicholas Wang

Language dc:language

en, eng

Handle dc:identifier

https://hdl.handle.net/2142/117878

OAI record oai:identifier

https://www.ideals.illinois.edu/oai-pmh?verb=GetRecord&metadataPrefix=etdms&identifier=oai%3Awww.ideals.illinois.edu%3A2142%2F117878