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

Wang, Nicholas Mason

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

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

Copyright and License Information

Copyright 2022 Nicholas Wang

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