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@PHDTHESIS{Rnitz:1044386,
author = {Rönitz, Jakob},
title = {{M}etabolic engineering of {P}seudomonas taiwanensis for
the improved production of styrene},
volume = {297},
school = {Düsseldorf},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2025-03157},
isbn = {978-3-95806-841-4},
series = {Schriften des Forschungszentrums Jülich Reihe
Schlüsseltechnologien / Key Technologies},
pages = {XII, 147},
year = {2025},
note = {Dissertation, Düsseldorf, 2025},
abstract = {Styrene is an important building block for polymers and
that is found in a broad spectrum of products that are
omnipresent in our modern society, including consumer
electronics, toys, packaging material, and car tires.
However, the production of styrene is currently solely based
on the petrochemical industry, which does not represent a
viable long-term strategy due to the limited abundance of
fossil resources. Biotechnological production of this
compound provides a sustainable alternative to the supply
issue, but the high toxicity and volatility of styrene poses
challenges for the development of a bioprocesses. Due to
high product toxicity, the use of a solvent-tolerant host
organism such as Pseudomonas taiwanensis VLB120 is
favourable for this application. However, cultivation of
bacteria in presence of volatile solvents also poses special
requirements to the cultivation system, resulting in limited
throughput and high manual workload for experiments. In this
thesis, this challenge was addressed by the development of
the SIGHT (solvent-tight incubation and growth monitoring in
high throughput) system, which prevents evaporation of
volatile compounds and allows to utilise the Growth Profiler
(EnzyScreen) platform, enabling incubation and non-invasive
online growth monitoring of up to 240 cultures in parallel.
The high-throughput capacity of the SIGHT system was
demonstrated by adaptive laboratory evolution (ALE) of P.
taiwanensis GRC3 to further increase styrene tolerance,
which allowed isolation of clones with improved growth in
presence of a second phase of styrene. Furthermore, a
solvent-inducible biosensor was applied to determine styrene
concentrations in the cytosol of a solvent-sensitive and
solventtolerant P. taiwanensis strain at different levels of
exposure, which enabled calculation of styrene accumulation
in the inner membrane. When exposed to a second phase of
styrene, the concentration in the cytosol of
solvent-tolerant P. taiwanensis GRC2 was only 0.45 mM, which
is 6.2-fold lower compared to the medium, due to activity of
the TtgGHI solvent efflux pump harboured by this strain.
This allowed to gain new insights into the physiology of
solvent-tolerant Pseudomonads under stress conditions and
further highlighted their suitability as hosts for styrene
bioproduction. However, maintaining activity of the TtgGHI
solvent efflux pump is highly energy demanding and puts an
additional burden on the metabolism of styrene production
strains, which also need to overproduce L-phenylalanine, the
precursor required for styrene biosynthesis. The styrene
biosynthesis pathway consisting of a phenylalanine
ammonia-lyase (PAL) from Arabidopsis thaliana and ferulic
acid decarboxylase (FDC) from Saccharomyces cerevisiae was
integrated into the genome of L-phenylalanine-overproducing
strain P. taiwanensis GRC3 Δ8ΔpykA-tap and genetic
engineering was applied to balance precursor biosynthesis
and strain fitness. This optimisation increased de novo
production of styrene from glucose to a concentration of
1.30 mM in the aqueous phase (2.68 mM in total, including
gas phase), representing an improvement of $8.1\%$ compared
to the starting strain. Furthermore, highly styrene-tolerant
P. taiwanensis strains without modified L-phenylalanine
biosynthesis were applied for biotransformation of
t-cinnamate to styrene as an alternative to de novo
biosynthesis. This approach allowed complete conversion of
up to 50 mM t-cinnamate, which corresponds to saturation of
the medium and formation of a second phase of styrene in the
culture. Overall, this thesis contributed to physiological
understanding of solvent tolerance in P. taiwanensis as well
as the balance between tolerance and styrene biosynthesis,
which facilitates the suitability of this host organism for
further development of a sustainable styrene production
process.},
cin = {IBG-1},
cid = {I:(DE-Juel1)IBG-1-20101118},
pnm = {2171 - Biological and environmental resources for
sustainable use (POF4-217)},
pid = {G:(DE-HGF)POF4-2171},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
urn = {urn:nbn:de:0001-2508051118123.694702301970},
doi = {10.34734/FZJ-2025-03157},
url = {https://juser.fz-juelich.de/record/1044386},
}