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Bridging the Gap Between Chemical an...

MacRae, Austin Lee.

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Bridging the Gap Between Chemical and Biochemical Catalysis Utilizing Metal-Organic Frameworks.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Bridging the Gap Between Chemical and Biochemical Catalysis Utilizing Metal-Organic Frameworks./
Author:	MacRae, Austin Lee.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2023,
Description:	208 p.
Notes:	Source: Dissertations Abstracts International, Volume: 85-07, Section: B.
Contained By:	Dissertations Abstracts International85-07B.
Subject:	Chemistry. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30695417
ISBN:	9798381426014

Bridging the Gap Between Chemical and Biochemical Catalysis Utilizing Metal-Organic Frameworks.
MacRae, Austin Lee.

Bridging the Gap Between Chemical and Biochemical Catalysis Utilizing Metal-Organic Frameworks. - Ann Arbor : ProQuest Dissertations & Theses, 2023 - 208 p.

Source: Dissertations Abstracts International, Volume: 85-07, Section: B.

Thesis (Ph.D.)--North Dakota State University, 2023.

Catalysis is a powerful approach to carry out chemical reactions with reduced energy consumption and/or enhanced reaction rate and thus, an important principle of green chemistry that is essential for chemistry research and the industrial production of most compounds. Catalysis is often categorized as chemical catalysis and biocatalysis wherein regular chemical compounds especially organometallic complexes and enzymes are employed as the catalysts, respectively. Chemical catalysis and biocatalysis possess different mechanisms, advantages, and disadvantages and thus, are often studied and applied separately. Recently, we found an opportunity to bridge the two wherein chemical catalysis assists in the efficiency of biocatalysis through a unique connection, namely co-crystallization of enzymes in catalytically functional metal-organic frameworks (MOFs). Such unique enzyme immobilization approach provides enhanced enzyme stability and reusability under harsh conditions while removing the size limitation when loading enzymes to pre-formed MOFs. This dissertation presents our research of varied principles in chemical catalysis, biocatalysis, and bridging the two with MOFs.We started with preparing and characterizing the oxidation potentials and catalytic oxidation of organic model substrates of unique ruthenium organometallic complexes via electrochemical measurements and gas chromatography, respectively, with the goal of using these complexes for hydroxylation reactions. We then explored experimental approaches to promote biocatalysis and understand the underlying structural basis of the biocatalytic function. Our efforts include i) promoting the crystallinity and yield of the enzyme MOF co-crystals by developing an advanced version of mechnosynthetic method based on liquid-assisted grinding (LAG) and ii) determining the structural basis of the biocatalysis of a model enzyme, T4 phage lysozyme (T4L), upon immobilization in MOFs via co-crystallization using site-directed spin labeling (SDSL) electron paramagnetic resonance (EPR) spectroscopy. Lastly, we explore MOF photo harvesting capabilities to generate photocurrent/high energy electrons that can be utilized by immobilized redox enzymes in the same MOF, bridging chemical catalysis and biocatalysis.This dissertation demonstrates the feasibility of simultaneous researching and connecting chemical and biochemical catalysis using various experimental techniques to promote both fundamental science and industrial applications of catalysis principles. The results are meaningful for the rational design of novel chemical and biochemical catalysts as well as probing their working mechanisms.

ISBN: 9798381426014Subjects--Topical Terms:

516420
Chemistry.
Subjects--Index Terms:

Chemical reactions

Bridging the Gap Between Chemical and Biochemical Catalysis Utilizing Metal-Organic Frameworks.
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