University of Illinois Urbana-Champaign

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

Wang, Nicholas Mason

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WANG-DISSERTATION-2022.pdf

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

Description

Title
Homogeneous flow catalysis strategies for lab-scale kinetic investigation and reaction development
Author(s)
Wang, Nicholas Mason
Issue Date
2022-04-21
Director of Research (if dissertation) or Advisor (if thesis)
Guironnet, Damien S.
Doctoral Committee Chair(s)
Guironnet, Damien S.
Committee Member(s)
  • Peters, Baron G.
  • Zimmerman, Steven C.
  • Su, Xiao
Department of Study
Chemical & Biomolecular Engr
Discipline
Chemical Engineering
Degree Granting Institution
University of Illinois at Urbana-Champaign
Degree Name
Ph.D.
Degree Level
Dissertation
Keyword(s)
Flow Chemistry, Organometallics, Heterogenization, Reactor Engineering
Abstract
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.
Graduation Semester
2022-05
Type of Resource
Thesis
Handle URL
https://hdl.handle.net/2142/117878
Copyright and License Information
Copyright 2022 Nicholas Wang

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