Nature Chemical Biology,
Год журнала:
2023,
Номер
19(5), С. 651 - 662
Опубликована: Фев. 6, 2023
Abstract
Critical
to
a
sustainable
energy
future
are
microbial
platforms
that
can
process
aromatic
carbons
from
the
largely
untapped
reservoir
of
lignin
and
plastic
feedstocks.
Comamonas
species
present
promising
bacterial
candidates
for
such
because
they
use
range
natural
xenobiotic
compounds
often
possess
innate
genetic
constraints
avoid
competition
with
sugars.
However,
metabolic
reactions
these
underexplored,
regulatory
mechanisms
unknown.
Here
we
identify
multilevel
regulation
in
conversion
lignin-related
compounds,
4-hydroxybenzoate
vanillate,
plastics-related
compound,
terephthalate,
testosteroni
KF-1.
Transcription-level
controls
initial
catabolism
cleavage,
but
metabolite-level
thermodynamic
governs
fluxes
central
carbon
metabolism.
Quantitative
13
C
mapping
tricarboxylic
acid
cycle
cataplerotic
elucidates
key
routing
not
evident
enzyme
abundance
changes.
This
scheme
transcriptional
activation
coupled
fine-tuning
challenges
outcome
predictions
during
manipulations.
Metabolic Engineering,
Год журнала:
2021,
Номер
67, С. 250 - 261
Опубликована: Июль 12, 2021
Poly(ethylene
terephthalate)
(PET)
is
the
most
abundantly
consumed
synthetic
polyester
and
accordingly
a
major
source
of
plastic
waste.
The
development
chemocatalytic
approaches
for
PET
depolymerization
to
monomers
offers
new
options
open-loop
upcycling
PET,
which
can
leverage
biological
transformations
higher-value
products.
To
that
end,
here
we
perform
four
sequential
metabolic
engineering
efforts
in
Pseudomonas
putida
KT2440
enable
conversion
glycolysis
products
via:
(i)
ethylene
glycol
utilization
by
constitutive
expression
native
genes,
(ii)
terephthalate
(TPA)
catabolism
tphA2IIA3IIBIIA1II
from
Comamonas
tpaK
Rhodococcus
jostii,
(iii)
bis(2-hydroxyethyl)
(BHET)
hydrolysis
TPA
PETase
MHETase
Ideonella
sakaiensis,
(iv)
BHET
performance-advantaged
bioproduct,
β-ketoadipic
acid
(βKA)
deletion
pcaIJ.
Using
this
strain,
demonstrate
production
15.1
g/L
βKA
at
76%
molar
yield
bioreactors
catalytically
depolymerized
βKA.
Overall,
work
highlights
potential
tandem
catalytic
deconstruction
as
means
upcycle
waste
PET.
Chemical Reviews,
Год журнала:
2022,
Номер
123(9), С. 5521 - 5570
Опубликована: Дек. 30, 2022
Metabolic
engineering
aims
to
improve
the
production
of
economically
valuable
molecules
through
genetic
manipulation
microbial
metabolism.
While
discipline
is
a
little
over
30
years
old,
advancements
in
metabolic
have
given
way
industrial-level
molecule
benefitting
multiple
industries
such
as
chemical,
agriculture,
food,
pharmaceutical,
and
energy
industries.
This
review
describes
design,
build,
test,
learn
steps
necessary
for
leading
successful
campaign.
Moreover,
we
highlight
major
applications
engineering,
including
synthesizing
chemicals
fuels,
broadening
substrate
utilization,
improving
host
robustness
with
focus
on
specific
case
studies.
Finally,
conclude
discussion
perspectives
future
challenges
related
engineering.
Metabolic Engineering,
Год журнала:
2021,
Номер
71, С. 77 - 98
Опубликована: Дек. 21, 2021
The
plastic
crisis
requires
drastic
measures,
especially
for
the
plastics'
end-of-life.
Mixed
fractions
are
currently
difficult
to
recycle,
but
microbial
metabolism
might
open
new
pathways.
With
technologies
degradation
of
plastics
oligo-
and
monomers,
these
carbon
sources
can
be
used
in
biotechnology
upcycling
waste
valuable
products,
such
as
bioplastics
biosurfactants.
We
briefly
summarize
well-known
monomer
pathways
computed
their
theoretical
yields
industrially
interesting
products.
this
information
hand,
we
calculated
replacement
scenarios
existing
fossil-based
synthesis
routes
same
Thereby,
highlight
products
which
monomers
attractive
alternative
sources.
Notably,
not
highest
yield
product
on
substrate
biochemical
route,
rather
(in-)efficiency
petrochemical
(i.e.,
carbon,
energy
use)
determines
potential
upcycling.
Our
results
serve
a
guide
future
metabolic
engineering
efforts
towards
sustainable
economy.
ACS Catalysis,
Год журнала:
2022,
Номер
12(15), С. 9307 - 9324
Опубликована: Июль 18, 2022
Plastic
waste
triggers
a
series
of
concerns
because
its
disruptive
impact
on
the
environment
and
ecosystem.
From
point
view
catalysis,
however,
end-of-life
plastics
can
be
seen
as
an
untapped
feedstock
for
preparation
value-added
products.
Thus,
development
diversified
catalytic
approaches
valorization
is
urgent.
Previous
reviews
this
field
have
systematically
summarized
progress
made
plastic
reclamation.
In
review,
we
emphasize
design
processes
by
leveraging
state-of-the-art
technologies
from
other
developed
fields
to
derive
valuable
polymers,
functional
materials,
chemicals
plastics.
The
principles,
mechanisms,
opportunities
chemical
(thermo-,
electro-,
photocatalytic)
well
biocatalytic
ones
are
discussed,
which
may
provide
more
insights
future
processes.
Finally,
outlooks
perspectives
accelerate
toward
feasible
economy
discussed.
Chemical Reviews,
Год журнала:
2024,
Номер
124(7), С. 4393 - 4478
Опубликована: Март 22, 2024
Polyesters
carrying
polar
main-chain
ester
linkages
exhibit
distinct
material
properties
for
diverse
applications
and
thus
play
an
important
role
in
today's
plastics
economy.
It
is
anticipated
that
they
will
even
greater
tomorrow's
circular
economy
focuses
on
sustainability,
thanks
to
the
abundant
availability
of
their
biosourced
building
blocks
presence
bonds
can
be
chemically
or
biologically
cleaved
demand
by
multiple
methods
bring
about
more
desired
end-of-life
plastic
waste
management
options.
Because
this
potential
promise,
there
have
been
intense
research
activities
directed
at
addressing
recycling,
upcycling
biodegradation
existing
legacy
polyesters,
designing
biorenewable
alternatives,
redesigning
future
polyesters
with
intrinsic
chemical
recyclability
tailored
performance
rival
commodity
are
either
petroleum
based
and/or
hard
recycle.
This
review
captures
these
exciting
recent
developments
outlines
challenges
opportunities.
Case
studies
poly(lactic
acid),
poly(3-hydroxyalkanoate)s,
poly(ethylene
terephthalate),
poly(butylene
succinate),
poly(butylene-adipate
presented,
emerging
recyclable
comprehensively
reviewed.
Microbial Biotechnology,
Год журнала:
2022,
Номер
16(2), С. 195 - 217
Опубликована: Сен. 13, 2022
Global
economies
depend
on
the
use
of
fossil-fuel-based
polymers
with
360-400
million
metric
tons
synthetic
being
produced
per
year.
Unfortunately,
an
estimated
60%
global
production
is
disposed
into
environment.
Within
this
framework,
microbiologists
have
tried
to
identify
plastic-active
enzymes
over
past
decade.
Until
now,
research
has
largely
failed
deliver
functional
biocatalysts
acting
commodity
such
as
polyethylene
(PE),
polypropylene
(PP),
polyvinylchloride
(PVC),
ether-based
polyurethane
(PUR),
polyamide
(PA),
polystyrene
(PS)
and
rubber
(SR).
However,
few
are
known
act
low-density
low-crystalline
(amorphous)
terephthalate
(PET)
ester-based
PUR.
These
above-mentioned
represent
>95%
all
plastics
produced.
Therefore,
main
challenge
currently
facing
in
finding
polymer-active
targeting
majority
plastics.
identifying
either
implement
them
biotechnological
processes
or
understand
their
potential
role
nature
emerging
field.
The
application
these
still
its
infancy.
Here,
we
summarize
current
knowledge
microbial
enzymes,
distribution
impact
plastic
degradation
industrial
nature.
We
further
outline
major
challenges
novel
optimizing
ones
by
approaches
problems
arising
through
falsely
annotated
unfiltered
database
entries.
Finally,
highlight
applications
possible
re-
upcycling
concepts
using
microorganisms.
Chemical Society Reviews,
Год журнала:
2022,
Номер
52(1), С. 277 - 317
Опубликована: Дек. 15, 2022
The
review
presents
the
synthesis,
properties
and
applications
of
sustainable
cycloaliphatic
polyurethanes
from
various
renewable
building
blocks
such
as
biobased
terpenes,
carbohydrates,
fatty
acids
cholesterol
or
plastic
wastes
derivatives.
Cell Reports,
Год журнала:
2022,
Номер
42(1), С. 111908 - 111908
Опубликована: Дек. 29, 2022
More
than
70
million
tons
of
poly(ethylene
terephthalate)
(PET)
are
manufactured
worldwide
every
year.
The
accumulation
PET
waste
has
become
a
global
pollution
concern,
motivating
the
urgent
development
technologies
to
valorize
post-consumer
PET.
chemocatalytic
and
enzymatic
approaches
for
depolymerizing
its
corresponding
monomers
opens
up
new
opportunities
upcycling
through
biological
transformation.
Here,
we
identify
Rhodococcus
jostii
strain
(RPET)
that
can
directly
use
hydrolysate
as
sole
carbon
source.
We
also
investigate
potential
RPET
upcycle
into
value-added
chemicals,
using
lycopene
proof-of-concept
product.
Through
rational
metabolic
engineering,
improve
production
by
more
500-fold
over
wild
type.
In
addition,
demonstrate
approximately
1,300
μg/L
from
cascading
this
with
alkaline
hydrolysis.
This
work
highlights
great
conversion
means
achieving
upcycling.
