Abstract/Details

Synthesis of 3-Hydroxypropionic Acid from Acetylenecarboxylic Acid

Mathes Hewage, Amaya Nethmini Sirinimal.   Michigan State University ProQuest Dissertations Publishing,  2022. 29390957.

Abstract (summary)

Throughout the past several decades, the petroleum industry has remained a dominant player in the production of fuels, chemicals, and consumer products. However, rising global temperatures and declining fossil fuel reserves demand the need for sustainable processes that can compete with the existing crude oil-based economy. Employing microbes such as E. coli for the chemical production using renewable starch-derived feedstocks such as glucose has been identified as a preferred alternative. Although lignocellulosic feedstocks have been explored as an alternative to renewable sugars, these processes are yet to be successfully implemented in an industrial setting. Despite more recent research efforts to incorporate C1 feedstocks such as methane, methanol and carbon dioxide in microbial catalysis, development of efficient bacterial metabolic pathways using these feedstocks have proven to be challenging. Herein, acetylenecarboxylic acid (ACA) is proposed as a unique feedstock for microbial catalysis. ACA can be derived from dehydrodimerization of methane to acetylene and subsequent carboxylation of acetylene. Cg10062 was previously identified as an enzyme capable of hydrating ACA to form a mixture of malonate semialdehyde (MSA) and acetaldehyde. In this study, novel variant Cg10062(E114N)) that forms exclusively MSA from ACA was discovered using rational mutagenesis. Cg10062(E114N) was coupled with NADPH-dependent dehydrogenase YdfG to develop a unique biocatalytic route to building block chemical 3-hydroxypropionic acid (3-HP). In vitro synthesis of 3-HP from ACA was demonstrated using catalytic amounts of NADP(H) where cofactor regeneration was achieved using NADP+-dependent phosphite dehydrogenase PTDH.

Indexing (details)


Subject
Chemistry;
Molecular biology
Classification
0485: Chemistry
0307: Molecular biology
Identifier / keyword
3-hydroxypropanoic acid; Acetylenecarboxylic acid; Carbon dioxide; Methane; Propiolic acid
Title
Synthesis of 3-Hydroxypropionic Acid from Acetylenecarboxylic Acid
Author
Mathes Hewage, Amaya Nethmini Sirinimal  VIAFID ORCID Logo 
Number of pages
252
Publication year
2022
Degree date
2022
School code
0128
Source
DAI-B 84/2(E), Dissertation Abstracts International
Place of publication
Ann Arbor
Country of publication
United States
ISBN
9798845422248
Advisor
Draths, Karen
Committee member
Borhan, Babak; Jackson, James E.; Odom, Aaron L.
University/institution
Michigan State University
Department
Chemistry - Doctor of Philosophy
University location
United States -- Michigan
Degree
Ph.D.
Source type
Dissertation or Thesis
Language
English
Document type
Dissertation/Thesis
Dissertation/thesis number
29390957
ProQuest document ID
2708763781
Copyright
Database copyright ProQuest LLC; ProQuest does not claim copyright in the individual underlying works.
Document URL
https://www.proquest.com/docview/2708763781