Efficient bio-production of citramalate using an engineered Escherichia coli strain

Citramalic acid is a central intermediate in a combined biocatalytic and chemocatalytic route to produce bio-based methylmethacrylate, the monomer used to manufacture Perspex and other high performance materials. We developed an engineered E. coli strain and a fed-batch bioprocess to produce citrama...

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Main Authors: Webb, Joseph P., Arnold, S. Alison, Baxter, Scott, Hall, Stephen J., Eastham, Graham, Stephens, Gill
Format: Article
Published: Society for General Microbiology 2018
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Online Access:https://eprints.nottingham.ac.uk/48425/
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author Webb, Joseph P.
Arnold, S. Alison
Baxter, Scott
Hall, Stephen J.
Eastham, Graham
Stephens, Gill
author_facet Webb, Joseph P.
Arnold, S. Alison
Baxter, Scott
Hall, Stephen J.
Eastham, Graham
Stephens, Gill
author_sort Webb, Joseph P.
building Nottingham Research Data Repository
collection Online Access
description Citramalic acid is a central intermediate in a combined biocatalytic and chemocatalytic route to produce bio-based methylmethacrylate, the monomer used to manufacture Perspex and other high performance materials. We developed an engineered E. coli strain and a fed-batch bioprocess to produce citramalate at concentrations in excess of 80 g l-1 in only 65 h. This exceptional efficiency was achieved by designing the production strain and the fermentation system to operate synergistically. Thus, a single gene encoding a mesophilic variant of citramalate synthase from Methanococcus jannaschii, CimA3.7, was expressed in E. coli to convert acetyl-CoA and pyruvate to citramalate, and the ldhA and pflB genes were deleted. By using a bioprocess with a continuous, growth-limiting feed of glucose, these simple interventions diverted substrate flux directly from central metabolism towards formation of citramalate, without problematic accumulation of acetate. Furthermore, the nutritional requirements of the production strain could be satisfied through the use of a mineral salts medium supplemented only with glucose (172 g l-1 in total) and 1.4 g l-1 yeast extract. Using this system, citramalate accumulated to 82±1.5 g l-1, with a productivity of 1.85 g l-1 h-1 and a conversion efficiency of 0.48 gcitramalate g-1 glucose. The new bioprocess forms a practical first step for integrated bio- and chemocatalytic production of methylmethacrylate.
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spelling nottingham-484252020-05-04T19:30:35Z https://eprints.nottingham.ac.uk/48425/ Efficient bio-production of citramalate using an engineered Escherichia coli strain Webb, Joseph P. Arnold, S. Alison Baxter, Scott Hall, Stephen J. Eastham, Graham Stephens, Gill Citramalic acid is a central intermediate in a combined biocatalytic and chemocatalytic route to produce bio-based methylmethacrylate, the monomer used to manufacture Perspex and other high performance materials. We developed an engineered E. coli strain and a fed-batch bioprocess to produce citramalate at concentrations in excess of 80 g l-1 in only 65 h. This exceptional efficiency was achieved by designing the production strain and the fermentation system to operate synergistically. Thus, a single gene encoding a mesophilic variant of citramalate synthase from Methanococcus jannaschii, CimA3.7, was expressed in E. coli to convert acetyl-CoA and pyruvate to citramalate, and the ldhA and pflB genes were deleted. By using a bioprocess with a continuous, growth-limiting feed of glucose, these simple interventions diverted substrate flux directly from central metabolism towards formation of citramalate, without problematic accumulation of acetate. Furthermore, the nutritional requirements of the production strain could be satisfied through the use of a mineral salts medium supplemented only with glucose (172 g l-1 in total) and 1.4 g l-1 yeast extract. Using this system, citramalate accumulated to 82±1.5 g l-1, with a productivity of 1.85 g l-1 h-1 and a conversion efficiency of 0.48 gcitramalate g-1 glucose. The new bioprocess forms a practical first step for integrated bio- and chemocatalytic production of methylmethacrylate. Society for General Microbiology 2018-02-01 Article PeerReviewed Webb, Joseph P., Arnold, S. Alison, Baxter, Scott, Hall, Stephen J., Eastham, Graham and Stephens, Gill (2018) Efficient bio-production of citramalate using an engineered Escherichia coli strain. Microbiology, 164 . pp. 133-141. ISSN 1465-2080 citramalic acid; methyl methacrylate; fed-batch fermentation; bio-based chemicals http://mic.microbiologyresearch.org/content/journal/micro/10.1099/mic.0.000581 doi:10.1099/mic.0.000581 doi:10.1099/mic.0.000581
spellingShingle citramalic acid; methyl methacrylate; fed-batch fermentation; bio-based chemicals
Webb, Joseph P.
Arnold, S. Alison
Baxter, Scott
Hall, Stephen J.
Eastham, Graham
Stephens, Gill
Efficient bio-production of citramalate using an engineered Escherichia coli strain
title Efficient bio-production of citramalate using an engineered Escherichia coli strain
title_full Efficient bio-production of citramalate using an engineered Escherichia coli strain
title_fullStr Efficient bio-production of citramalate using an engineered Escherichia coli strain
title_full_unstemmed Efficient bio-production of citramalate using an engineered Escherichia coli strain
title_short Efficient bio-production of citramalate using an engineered Escherichia coli strain
title_sort efficient bio-production of citramalate using an engineered escherichia coli strain
topic citramalic acid; methyl methacrylate; fed-batch fermentation; bio-based chemicals
url https://eprints.nottingham.ac.uk/48425/
https://eprints.nottingham.ac.uk/48425/
https://eprints.nottingham.ac.uk/48425/