Date of Award

Fall 12-18-2020

Level of Access Assigned by Author

Open-Access Thesis

Degree Name

Doctor of Philosophy (PhD)

Department

Chemical Engineering

Advisor

Thomas J. Schwartz

Second Committee Member

M. Clayton Wheeler

Third Committee Member

William J. DeSisto

Additional Committee Members

G. Peter van Walsum

Michael Kienzler

Abstract

The development of the technologies and the improved processes for the production of high value bio-based chemicals is one of the most important challenges at the present time. This new movement is not only important from an environmental perspective, but also it is a profitable approach to provide affordable and efficient processes. Therefore, the chemical catalytic upgrading processes over various homogenous and heterogeneous catalysis could be an outstanding modification to upgrade biomass-derived platform molecule to high value applications. In this dissertation, we highlight our recent progress in developing new chemistries and processes for upgrading biomass-derived molecules and address the challenges associated with the catalytic conversion processes.

Chapter 3 concentrates on the ethanol dehydrogenation reaction as a key step in the Lebedev reaction for butadiene formation. There recently has been a resurgence of interest in the production of butadiene from ethanol, which can be obtained from biomass. This route remains poorly explained with many inconsistent mechanisms having been proposed. Ethanol is converted to acetaldehyde over a well-defined model MgO-SiO2 catalyst. The proposed mechanism and microkinetic model of the ethanol dehydrogenation reaction further provides a basic understanding for the essential challenges related to the key step reaction in the butadiene production pathway.

Chapter 4 demonstrates the development of a new chemistry that utilizes a biosynthesis-derived molecule to produce a higher value pharmaceutical precursor that can be upgraded catalytically to important statin drugs. Glucose can be upgraded selectively over a combination of biological and chemical catalysts to yield 3-hydroxy-γ-butyrolactone (HBL) by using a multistep process. Chapter 4 shows a part of the catalytic chemical phase of upgrading a reactive intermediate called trione into HBL. This chapter focuses on the first step of upgrading trione to glycolate esters over various homogenous base catalysts. Ultimately, this work will serve as a solid background to future researchers in the pursuit of understanding to advance the potential remaining steps to produce HBL from glucose over single catalytic materials including enzymes.

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Feb 28 2024

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