Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(26)
Опубликована: Фев. 25, 2022
Enzyme
catalysis
has
been
increasingly
utilized
in
reversible
deactivation
radical
polymerization
(Enz-RDRP)
on
account
of
its
mildness,
efficiency,
and
sustainability.
In
this
Minireview
we
discuss
the
key
roles
enzymes
play
RDRP,
including
their
ATRPase,
initiase,
deoxygenation,
photoenzyme
activities.
We
use
selected
examples
to
highlight
applications
Enz-RDRP
surface
brush
fabrication,
sensing,
polymerization-induced
self-assembly,
high-throughput
synthesis.
also
give
our
reflections
challenges
future
directions
emerging
area.
Chemical Society Reviews,
Год журнала:
2021,
Номер
50(14), С. 8003 - 8049
Опубликована: Янв. 1, 2021
Technological
developments
enable
the
discovery
of
novel
enzymes,
advancement
enzyme
cascade
designs
and
pathway
engineering,
moving
biocatalysis
into
an
era
technology
integration,
intelligent
manufacturing
enzymatic
total
synthesis.
Chemical Reviews,
Год журнала:
2022,
Номер
122(6), С. 5842 - 5976
Опубликована: Янв. 24, 2022
Benefiting
from
the
impressive
increase
in
fundamental
knowledge,
last
20
years
have
shown
a
continuous
burst
of
new
ideas
and
consequently
plethora
catalytic
methods
for
enantioselective
radical
reactions.
This
review
aims
to
provide
complete
survey
progress
achieved
over
this
latter
period.
The
first
part
focuses
on
use
chiral
organocatalysts,
these
include
catalysts
covalently
linked
substrate
those
that
interact
with
by
weaker
interactions
like
hydrogen
bonds.
second
is
devoted
transition-metal
redox
catalysis
which
organized
according
increasing
atomic
number
first-row
transition
metals
(Ti,
Cr,
Fe,
Mn,
Co,
Ni,
Cu).
Bioinspired
manganese-
iron-mediated
hydroxylations
oxidations
are
also
discussed.
A
specific
section
dedicated
reactivity
Ru,
Rh,
Ir
complexes
as
Lewis
acids
special
focus
at
metal.
Absorption
photons
result
different
events
such
energy
transfer,
single-electron
hydrogen-atom
transfer
facilitating
formation
radicals.
Organocatalysis
has
been
successfully
combined
photocatalysts,
opened
pathways
enlarging
precursors
available.
merger
photocatalysis
organo-
or
metalla-photocatalysis
brought
novelty
allowed
discovery
large
original
transformations.
enzyme-catalyzed
reactions
involving
intermediates
largely
benefit
visible-light
irradiation
included
review.
provides
comprehensive
inventory
goal
detailing
reaction
mechanisms
involved
transformations
any
nonspecialist
could
find
their
own
creativity
invent
yet
unknown
applications.
Chemical Reviews,
Год журнала:
2021,
Номер
122(1), С. 1052 - 1126
Опубликована: Ноя. 30, 2021
Biocatalysis,
using
enzymes
for
organic
synthesis,
has
emerged
as
powerful
tool
the
synthesis
of
active
pharmaceutical
ingredients
(APIs).
The
first
industrial
biocatalytic
processes
launched
in
half
last
century
exploited
whole-cell
microorganisms
where
specific
enzyme
at
work
was
not
known.
In
meantime,
novel
molecular
biology
methods,
such
efficient
gene
sequencing
and
triggered
breakthroughs
directed
evolution
rapid
development
process-stable
with
broad
substrate
scope
good
selectivities
tailored
substrates.
To
date,
are
employed
to
enable
shorter,
more
efficient,
sustainable
alternative
routes
toward
(established)
small
molecule
APIs,
additionally
used
perform
standard
reactions
API
efficiently.
Herein,
large-scale
synthetic
containing
key
steps
>130
APIs
approved
drugs
drug
candidates
compared
corresponding
chemical
protocols
(if
available)
regarding
steps,
reaction
conditions,
scale.
review
is
structured
according
functional
group
formed
reaction.
Chemical Society Reviews,
Год журнала:
2021,
Номер
51(2), С. 594 - 627
Опубликована: Дек. 20, 2021
The
many
waves
of
biocatalysis
have
arisen
to
solve
long-standing
synthetic
challenges.
From
industrially
applied
hydrolases
enzymes
catalysing
selective
C–C-bond
formation,
enables
new
tools
access
a
plethora
compounds.
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 5702 - 5754
Опубликована: Янв. 24, 2023
Enzymatic
carbon
dioxide
fixation
is
one
of
the
most
important
metabolic
reactions
as
it
allows
capture
inorganic
from
atmosphere
and
its
conversion
into
organic
biomass.
However,
due
to
often
unfavorable
thermodynamics
difficulties
associated
with
utilization
CO
The
role
and
power
of
biocatalysis
in
sustainable
chemistry
has
been
continuously
brought
forward
step
by
to
its
present
outstanding
position.
problem-solving
capabilities
have
realized
numerous
substantial
achievements
biology,
engineering.
Advances
breakthroughs
the
life
sciences
interdisciplinary
cooperation
with
clearly
accelerated
implementation
biocatalytic
synthesis
modern
chemistry.
Resource-efficient
manufacturing
processes
already
provided
benefits
as
well
customer-centric
value
creation
pharmaceutical,
food,
flavor,
fragrance,
vitamin,
agrochemical,
polymer,
specialty,
fine
chemical
industries.
Biocatalysis
can
make
significant
contributions
not
only
processes,
but
also
design
completely
new
value-creation
chains.
now
be
considered
a
key
enabling
technology
implement
Nature Communications,
Год журнала:
2022,
Номер
13(1)
Опубликована: Фев. 18, 2022
Abstract
Enzyme
catalysts
are
an
integral
part
of
green
chemistry
strategies
towards
a
more
sustainable
and
resource-efficient
chemical
synthesis.
However,
the
use
biocatalysed
reactions
in
retrosynthetic
planning
clashes
with
difficulties
predicting
enzymatic
activity
on
unreported
substrates
enzyme-specific
stereo-
regioselectivity.
As
now,
only
rule-based
systems
support
using
biocatalysis,
while
initial
data-driven
approaches
limited
to
forward
predictions.
Here,
we
extend
reaction
as
well
pathway
prediction
models
based
Molecular
Transformer
architecture
biocatalysis.
The
knowledge
is
learned
from
extensive
data
set
publicly
available
biochemical
aid
new
class
token
scheme
enzyme
commission
classification
number,
which
captures
catalysis
patterns
among
different
enzymes
belonging
same
hierarchy.
model
(top-1
accuracy
49.6%),
single-step
round-trip
39.6%)
curated
made
facilitate
adoption
design
greener
processes.
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 5297 - 5346
Опубликована: Янв. 10, 2023
The
combination
of
metal-,
photo-,
enzyme-,
and/or
organocatalysis
provides
multiple
synthetic
solutions,
especially
when
the
creation
chiral
centers
is
involved.
Historically,
enzymes
and
transition
metal
species
have
been
exploited
simultaneously
through
dynamic
kinetic
resolutions
racemates.
However,
more
recently,
linear
cascades
appeared
as
elegant
solutions
for
preparation
valuable
organic
molecules
combining
bioprocesses
metal-catalyzed
transformations.
Many
advantages
are
derived
from
this
symbiosis,
although
there
still
bottlenecks
to
be
addressed
including
successful
coexistence
both
catalyst
types,
need
compatible
reaction
media
mild
conditions,
or
minimization
cross-reactivities.
Therefore,
here
also
provided
by
means
coimmobilization,
compartmentalization
strategies,
flow
chemistry,
etc.
A
comprehensive
review
presented
focusing
on
period
2015
early
2022,
which
has
divided
into
two
main
sections
that
comprise
first
use
metals
independent
catalysts
but
working
in
an
orchestral
sequential
manner,
later
their
application
bionanohybrid
materials
coimmobilization
adequate
supports.
Each
part
classified
different
subheadings,
based
catalyzed
catalyst,
while
development
nonasymmetric
stereoselective
processes
was
considered
section.