% IMPORTANT: The following is UTF-8 encoded. This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.
@PHDTHESIS{Milke:877282,
author = {Milke, Lars},
title = {{E}ngineering of {C}orynebacterium glutamicum towards
increased malonyl-{C}o{A} availability for polyketide
synthesis},
volume = {223},
school = {Heinrich-Heine-Universität Düsseldorf},
type = {Dr.},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2020-02105},
isbn = {978-3-95806-480-5},
series = {Schriften des Forschungszentrums Jülich. Reihe
Schlüsseltechnologien / Key Technologies},
pages = {IX, 117 S.},
year = {2020},
note = {Biotechnologie 1; Heinrich-Heine-Universität Düsseldorf,
Diss., 2020},
abstract = {Polyketides are a structurally highly diverse group of
natural products with interesting healthpromoting effects on
humans. Despite all structural differences, polyketides are
synthesized from simple CoA-activated carboxylic acid
derivatives, such as acetyl-CoA or malonyl-CoA following a
mechanism closely related to fatty acid biosynthesis.
Unfortunately, polyketides are only synthesized in small
quantities by the respective native organism. In contrast,
microbial polyketide synthesis using engineered bacteria is
a promising approach to get access to the desired products.
Against this background, $\textit{Corynebacterium
glutamicum}$ strains for the production of different plant
polyketides such as stilbenes and flavonoids have been
constructed recently. However, it soon became evident that
the intracellular availability of malonyl-CoA is limiting
the overall product formation in these strains. Hence, the
main goal of this thesis was to optimize the intracellular
malonyl-CoA availability in $\textit{C. glutamicum}$ by
metabolic engineering. Additionally, the tailored strains
should be used for establishing synthesis of
biotechnological interesting polyketides. The following
results were obtained: 1) Reduction of the citrate synthase
activity to 5.5 \% compared to the $\textit{C. glutamicum}$
wild type by exchanging the promotor of the encoding
$\textit{gltA}$ gene, reduced acetyl-CoA consumption via the
tricarboxylic acid cycle, which in turn improved malonyl-CoA
availability. Upon transcriptional deregulation of
$\textit{accBC}$ and $\textit{accD1}$ encoding the two
subunits of acetyl-CoA carboxylase, malonyl-CoA synthesis
from acetyl-CoA was drastically improved allowing for the
synthesis of 65 mg/L (0.24 mM) naringenin und 450 mg/L (1.97
mM) resveratrol. Furthermore, improving the glucose uptake
and elimination of anaplerotic pyruvate carboxylation
reaction further contributed to an improved intracellular
malonyl-CoA availability in the ultimately constructed
strain $\textit{C. glutamicum}$ M-CoA. 2) Through episomal
expression of genes encoding heterologous type III
polyketide synthases from various plant species in the
constructed strain $\textit{C. glutamicum}$ M-CoA, microbial
synthesis of a pentaketide (noreugenin) but also
phenylbutanoids (raspberry ketone, zingerone, benzylacetone)
with a $\textit{ldhA}$-deficient variant could be
established. The respective strains allowed for the
synthesis of up to 53.3 mg/L (0.28 mM) noreugenin, 100 mg/L
(0.61 mM) raspberry ketone, 70 mg/L (0.36 mM) zingerone and
10.5 mg/L (0.07 mM) benzylacetone from simple precursor
molecules, respectively. 3) Hitherto, only type III
polyketides can be synthesized by engineered $\textit{C.
glutamicum}$ strains. In the context of this study,
functional expression of a codon-optimized gene variant
encoding the type I polyketide synthase 6-methylsalicylic
acid synthase ChlB1 from $\textit {Streptomyces
antibioticus}$ of 1,756 amino acids size was achieved. This
allowed for the synthesis of up to 41 mg/L (0.27 mM)
6-methylsalicylic acid. It was found that $\textit{C.
glutamicum}$ has an endogenous
phosphopantetheinyltransferase activity, which can
post-translationally activate ChlB1. This makes $\textit{C.
glutamicum}$ a promising host for the production of other
interesting type I polyketides.},
cin = {IBG-1},
cid = {I:(DE-Juel1)IBG-1-20101118},
pnm = {581 - Biotechnology (POF3-581)},
pid = {G:(DE-HGF)POF3-581},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
urn = {urn:nbn:de:0001-2020072314},
url = {https://juser.fz-juelich.de/record/877282},
}