Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences,
Год журнала:
2017,
Номер
376(2110), С. 20170063 - 20170063
Опубликована: Ноя. 25, 2017
Biocatalysis
has
undergone
a
tremendous
development
in
the
past
few
years.
A
plethora
of
methods
enable
rather
rapid
tailored-design
an
enzyme
for
targeted
reaction
such
as
asymmetric
synthesis
chiral
building
block
by
combination
information
from
sequence
and
structure
databases
with
modern
molecular
biology
high-throughput
screening
tools.
Moreover,
novel
non-natural
reactions
could
be
implemented
into
protein
scaffolds
new
classes
are
emerging,
both
broadening
repertoire
now
available
organic
synthesis.
Furthermore,
impressive
examples
metabolic
engineering-the
several
newly
introduced
steps
microbial
host-have
been
developed,
paving
way
large-scale
processes
pharmaceuticals
bulk
chemicals.
This
contribution
highlights
recent
developments
this
area
points
out
future
challenges.This
article
is
part
discussion
meeting
issue
'Providing
sustainable
catalytic
solutions
rapidly
changing
world'.
Angewandte Chemie International Edition,
Год журнала:
2020,
Номер
60(1), С. 88 - 119
Опубликована: Июнь 18, 2020
Abstract
Biocatalysis
has
found
numerous
applications
in
various
fields
as
an
alternative
to
chemical
catalysis.
The
use
of
enzymes
organic
synthesis,
especially
make
chiral
compounds
for
pharmaceuticals
well
the
flavors
and
fragrance
industry,
are
most
prominent
examples.
In
addition,
biocatalysts
used
on
a
large
scale
specialty
even
bulk
chemicals.
This
review
intends
give
illustrative
examples
this
field
with
special
focus
scalable
production
using
enzymes.
It
also
discusses
opportunities
limitations
enzymatic
syntheses
distinct
provides
outlook
emerging
enzyme
classes.
Chemical Society Reviews,
Год журнала:
2018,
Номер
47(15), С. 5786 - 5865
Опубликована: Янв. 1, 2018
This
review
provides
an
overview
of
the
use
electrochemistry
as
appealing
platform
for
expediting
carbon–hydrogen
functionalization
and
carbon–nitrogen
bond
formation.
Angewandte Chemie International Edition,
Год журнала:
2018,
Номер
57(30), С. 9238 - 9261
Опубликована: Март 24, 2018
Abstract
Oxidation
chemistry
using
enzymes
is
approaching
maturity
and
practical
applicability
in
organic
synthesis.
Oxidoreductases
(enzymes
catalysing
redox
reactions)
enable
chemists
to
perform
highly
selective
efficient
transformations
ranging
from
simple
alcohol
oxidations
stereoselective
halogenations
of
non‐activated
C−H
bonds.
For
many
these
reactions,
no
“classical”
chemical
counterpart
known.
Hence
oxidoreductases
open
up
shorter
synthesis
routes
based
on
a
more
direct
access
the
target
products.
The
generally
very
mild
reaction
conditions
may
also
reduce
environmental
impact
biocatalytic
reactions
compared
classical
counterparts.
In
this
Review,
we
critically
summarise
most
important
recent
developments
field
oxidation
identify
pressing
bottlenecks
as
well
promising
solutions.
Angewandte Chemie International Edition,
Год журнала:
2019,
Номер
59(32), С. 13204 - 13231
Опубликована: Июль 3, 2019
Directed
evolution
of
stereo-,
regio-,
and
chemoselective
enzymes
constitutes
a
unique
way
to
generate
biocatalysts
for
synthetically
interesting
transformations
in
organic
chemistry
biotechnology.
In
order
this
protein
engineering
technique
be
efficient,
fast,
reliable,
also
relevance
synthetic
chemistry,
methodology
development
was
still
is
necessary.
Following
description
early
key
contributions,
review
focuses
on
recent
developments.
It
includes
optimization
molecular
biological
methods
gene
mutagenesis
the
design
efficient
strategies
their
application,
resulting
notable
reduction
screening
effort
(bottleneck
directed
evolution).
When
aiming
laboratory
selectivity
activity,
second-generation
versions
Combinatorial
Active-Site
Saturation
Test
(CAST)
Iterative
Mutagenesis
(ISM),
both
involving
saturation
(SM)
at
sites
lining
binding
pocket,
have
emerged
as
preferred
approaches,
aided
by
silico
such
machine
learning.
The
recently
proposed
Focused
Rational
Site-specific
(FRISM)
fusion
rational
evolution.
On-chip
solid-phase
chemical
synthesis
rapid
library
construction
enhances
quality
notably
eliminating
undesired
amino
acid
bias,
future
evolution?
ACS Central Science,
Год журнала:
2021,
Номер
7(1), С. 55 - 71
Опубликована: Янв. 14, 2021
Biocatalysis,
using
defined
enzymes
for
organic
transformations,
has
become
a
common
tool
in
synthesis,
which
is
also
frequently
applied
industry.
The
generally
high
activity
and
outstanding
stereo-,
regio-,
chemoselectivity
observed
many
biotransformations
are
the
result
of
precise
control
reaction
active
site
biocatalyst.
This
achieved
by
exact
positioning
reagents
relative
to
each
other
fine-tuned
3D
environment,
specific
activating
interactions
between
protein,
subtle
movements
catalyst.
Enzyme
engineering
enables
one
adapt
catalyst
desired
process.
A
well-filled
biocatalytic
toolbox
ready
be
used
various
reactions.
Providing
nonnatural
conditions
evolving
biocatalysts
play
with
myriad
options
creating
novel
transformations
thereby
opening
new,
short
pathways
target
molecules.
Combining
several
pot
perform
reactions
concurrently
increases
efficiency
biocatalysis
even
further.
Organometallics,
Год журнала:
2018,
Номер
38(1), С. 47 - 65
Опубликована: Дек. 20, 2018
This
is
an
overview
of
successes
in
the
realm
catalytic
homogeneous
asymmetric
hydrogenation
substrates
primarily
interest
synthesis
pharmaceuticals
order
to
identify
important
problems
still
unsolved.
First,
tables
are
provided
that
list
successful
reductions
over
90%
enantiomeric
excess
prochiral
ketones
alcohols,
imines
amines,
and
olefins
saturated
carbon
centers.
Noted
metal
(including
"green"
metals
Mn,
Fe,
Co)
or
enzyme,
class
ligand,
conditions
medium,
scale
reduction,
if
1
kg
product,
as
well
nature
process,
whether
direct
using
H2
gas
(DH),
transfer
(TH),
with
dynamic
kinetic
resolution
(DKR).
Tables
representative
pharmaceutical
fine
chemicals
products
for
each
substrate.
With
this
overview,
opportunities
further
research
development
become
clearer.
