Angewandte Chemie,
Год журнала:
2023,
Номер
136(8)
Опубликована: Ноя. 10, 2023
Abstract
Die
Herstellung
von
chemischen
Grundstoffen
wie
Benzol,
Toluol,
Ethylbenzol
und
Xylol
(BTEX)
aus
erneuerbaren
Ressourcen
ist
der
Schlüssel
zu
einer
nachhaltigen
Gesellschaft.
Biokatalyse
ermöglicht
die
Ein‐Topf‐Mehrschritt‐Transformation
Bioressourcen
unter
milden
Bedingungen,
jedoch
oft
auf
Biochemikalien
beschränkt.
Wir
haben
eine
nicht‐natürliche
Drei‐Enzym‐Kaskade
für
Ein‐Topf‐Umwandlung
biobasiertem
l
‐Phenylalanin
in
entwickelt.
geschwindigkeitsbestimmende
Photodecarboxylase
als
Schlüsselenzym
wurde
einem
strukturbasierten
semi‐rationalem
Engineering
unterzogen
es
Dreifachmutante
CvFAP(Y466T/P460A/G462I)
mit
6.3‐fach
höheren
Produktivität
erhalten.
Mit
dieser
verbesserten
ein
optimiertes
sequentielles
E.
coli
Zwei‐Zellsystem‐Verfahren
zur
Umwandlung
82
%
Umsatz
Kaskadenreaktion
Fermentation
integriert,
um
Ein‐Topf‐Bioproduktion
Glycerin
erreichen.
Dies
zeigt
das
Potenzial
Kaskaden‐Biokatalyse
Kombination
Enzym‐Engineering
Produktion
biobasierten
auf.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(42)
Опубликована: Сен. 1, 2023
A
mild,
scalable
(kg)
metal-free
electrochemical
decarboxylation
of
alkyl
carboxylic
acids
to
olefins
is
disclosed.
Numerous
applications
are
presented
wherein
this
transformation
can
simplify
alkene
synthesis
and
provide
alternative
synthetic
access
valuable
from
simple
acid
feedstocks.
This
robust
method
relies
on
alternating
polarity
maintain
the
quality
electrode
surface
local
pH,
providing
a
deeper
understanding
Hofer-Moest
process
with
unprecedented
chemoselectivity.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(33)
Опубликована: Май 22, 2024
Abstract
Drawing
inspiration
from
nature
has
long
been
a
cornerstone
of
chemical
innovation,
with
natural
systems
offering
wealth
untapped
potential
for
discovery.
In
this
minireview,
we
delve
into
the
burgeoning
field
cobaloxime
catalysis
in
organic
synthesis,
which
mimics
catalytic
activity
organometallic
alkylcobalamine
enzymes.
Our
focus
lies
on
elucidating
latest
advancements
area,
as
well
delineating
primary
mechanistic
pathways
at
play.
By
describing,
and
comparing
these
mechanisms,
provide
comprehensive
overview
current
state‐of‐the‐art,
while
also
shedding
light
key
unresolved
challenges
that
await
further
exploration.
ACS Applied Polymer Materials,
Год журнала:
2023,
Номер
5(7), С. 5650 - 5661
Опубликована: Июль 5, 2023
A
series
of
biobased
benzoxazine
monomers
(TF-BOZs)
were
designed
and
synthesized
using
tyrosine
methyl
ester,
furfural,
five
amine
sources
through
the
Mannich
condensation
reaction.
The
structures
BOZs
examined
1H
NMR,
13C
mass
spectra
(MS),
Fourier
transform
infrared
(FT-IR),
which
indicated
successful
synthesis
TF-BOZ
monomers.
Curing
behavior
was
studied,
revealed
that
BOZ
could
form
polybenzoxazine
resins
(PBOZs)
via
ring-opening
polymerization.
In
addition,
PBOZs
exhibited
remarkable
thermal
stability,
is
better
than
traditional
bisphenol
A–aniline
polybenzoxazine.
antibacterial
properties
antibiofilm
performances
investigated.
TF-BOZs
showed
significant
broad-spectrum
activity
against
Gram-positive
Staphylococcus
aureus
(S.
aureus),
Gram-negative
Escherichia
coli
(E.
coli),
Pseudomonas
aeruginosa
(P.
aeruginosa).
BOZ-Ola
best
property
with
minimum
inhibitory
concentration
(MIC)
5
μg/mL
S.
aureus,
which,
based
on
electrostatic
interaction
acts
bacterial
surface
hydrophobic
destroys
cell
membrane
integrity.
Notably,
resistance
to
adhesion
because
their
antimicrobial
properties,
stable
hydrophobicity,
low
energy,
indicating
application
potential
as
antifouling
materials.
Those
results
indicate
great
agents
materials
solve
contamination
expand
range
sustainable
Applied Microbiology and Biotechnology,
Год журнала:
2024,
Номер
108(1)
Опубликована: Окт. 30, 2024
Tyramine
has
attracted
considerable
interest
due
to
recent
findings
that
it
is
an
excellent
starting
material
for
the
production
of
high-performance
thermoplastics
and
hydrogels.
Furthermore,
tyramine
a
precursor
diversity
pharmaceutically
relevant
compounds,
contributing
its
growing
importance.
Given
limitations
chemical
synthesis,
including
lack
selectivity
laborious
processes
with
harsh
conditions,
biosynthesis
by
decarboxylation
L-tyrosine
represents
promising
sustainable
alternative.
In
this
study,
de
novo
from
simple
nitrogen
carbon
sources
was
successfully
established
metabolic
engineering
overproducing
Corynebacterium
glutamicum
strain
AROM3.
A
phylogenetic
analysis
aromatic-L-amino
acid
decarboxylases
(AADCs)
revealed
potential
candidate
enzymes
tyramine.
The
heterologous
overexpression
respective
AADC
genes
resulted
in
successful
production,
highest
titer
1.9
g
L
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Ноя. 24, 2024
Abstract
While
selective
defunctionalizations
are
valuable
in
organic
synthesis,
hydrodeamination
of
primary
amines
poses
challenges.
Deuterodeamination,
analogous
to
hydrodeamination,
presents
even
greater
difficulties
due
its
frequently
slower
deuteration
rate,
interference
by
hydrogenation
and
constraints
deuterated
sources.
This
study
introduces
a
reliable,
robust,
scalable
hydro-
deuterodeamination
method
capable
handling
various
amines.
Defined
mild
reaction
conditions,
rapid
completion,
simplified
purification
facilitated
water-soluble
byproducts,
the
leverages
deuterium
oxide
as
source
employs
commercialized
O-diphenylphosphinylhydroxylamine
for
deamination.
Applied
diverse
range
biologically
active
molecules,
it
has
consistently
achieved
high
yields
efficient
incorporation.
By
synergizing
with
site-selective
C–H
functionalization
aliphatic
amines,
our
reveals
synthetic
strategies
utilizing
nitrogen
atom
traceless
directing
group,
encompassing
deaminative
alkylation,
1,1-deuteroalkylation,
1,1-dialkylation,
1,1,1-deuterodialkylation,
arylation,
1,3-deuteroarylation.
Emphasizing
this
innovation,
processes
degree-controlled
have
been
developed.
Organic & Biomolecular Chemistry,
Год журнала:
2024,
Номер
22(13), С. 2562 - 2565
Опубликована: Янв. 1, 2024
Various
alkyl
isocyanides
participated
in
the
defunctionalization
with
tris(trimethylsilyl)silane
under
blue
light
irradiation
at
room
temperature
high
chemoselectivity.
ACS Catalysis,
Год журнала:
2023,
Номер
13(21), С. 14205 - 14212
Опубликована: Окт. 20, 2023
Herein,
we
present
a
biomimetic
method
for
the
catalytic
deammoniation
of
diverse
primary
amines,
including
amino
acids,
natural
products,
and
pharmaceuticals.
This
innovative
approach,
characterized
by
its
operational
simplicity
high
selectivity,
provides
rapid
easily
accessible
pathway
to
wide
range
olefin
products
derived
from
nonfossil-based
chemicals.
The
transformation
relies
on
utilization
two
readily
available
photoactive
catalysts:
acridinium
salt
cobaloxime.
Through
combination
experimental
theoretical
studies,
have
gained
valuable
insights
into
fundamental
steps
underlying
this
unconventional
dehydroamination
process.
Current Opinion in Biotechnology,
Год журнала:
2023,
Номер
85, С. 103058 - 103058
Опубликована: Дек. 27, 2023
For
the
valorization
of
various
bio-based
feedstocks,
combination
different
catalytic
systems
with
biocatalysis
in
chemoenzymatic
cascades
has
been
shown
to
have
high
potential.
However,
development
such
integrated
is
often
limited
by
catalyst
incompatibility.
Therefore,
incorporating
novel
concepts
into
feedstocks
currently
great
interest.
This
article
provides
an
overview
methods/approaches
used
advance
for
upgrading
feedstocks.
It
specifically
focuses
on
recent
developments
enzymes
organo-
and
chemocatalysis.
Furthermore,
current
applications
future
perspectives
integrating
as
photo-
electrocatalysis
toward
new
synthetic
routes
utilization
highly
functionalized
compounds
are
reviewed.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
63(8)
Опубликована: Ноя. 10, 2023
Abstract
Production
of
commodity
chemicals,
such
as
benzene,
toluene,
ethylbenzene,
and
xylenes
(BTEX),
from
renewable
resources
is
key
for
a
sustainable
society.
Biocatalysis
enables
one‐pot
multistep
transformation
bioresources
under
mild
conditions,
yet
it
often
limited
to
biochemicals.
Herein,
we
developed
non‐natural
three‐enzyme
cascade
conversion
biobased
l
‐phenylalanine
into
ethylbenzene.
The
rate‐limiting
photodecarboxylase
was
subjected
structure‐guided
semirational
engineering,
triple
mutant
CvFAP(Y466T/P460A/G462I)
obtained
with
6.3‐fold
higher
productivity.
With
this
improved
photodecarboxylase,
an
optimized
two‐cell
sequential
process
convert
ethylbenzene
82
%
conversion.
reaction
integrated
fermentation
achieve
the
bioproduction
glycerol,
demonstrating
potential
biocatalysis
plus
enzyme
engineering
production
chemicals.
