Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(38)
Published: July 1, 2024
While
plastics
like
polyethylene
terephthalate
can
already
be
degraded
efficiently
by
the
activity
of
hydrolases,
other
synthetic
polymers
polyurethanes
(PUs)
and
polyamides
(PAs)
largely
resist
biodegradation.
In
this
study,
we
solved
first
crystal
structure
metagenomic
urethanase
UMG-SP-1,
identified
highly
flexible
loop
regions
to
comprise
active
site
residues,
targeted
a
total
20
potential
hot
spots
site-saturation
mutagenesis.
Engineering
campaigns
yielded
variants
with
single
mutations,
exhibiting
almost
3-
8-fold
improved
against
stable
N-aryl
urethane
amide
bonds,
respectively.
Furthermore,
demonstrated
release
corresponding
monomers
from
thermoplastic
polyester-PU
PA
(nylon
6)
single,
metagenome-derived
after
short
incubation
times.
Thereby,
expanded
hydrolysis
profile
UMG-SP-1
beyond
reported
low-molecular
weight
carbamates.
Together,
these
findings
promise
advanced
strategies
for
bio-based
degradation
recycling
plastic
materials
waste,
aiding
efforts
establish
circular
economy
polymers.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(18)
Published: Feb. 6, 2023
Abstract
The
combination
of
catalytic
methods
provides
multiple
advantages
in
organic
synthesis,
allowing
access
to
diverse
molecules
a
straightforward
manner.
Merging
metal
and
enzyme
catalysis
is
currently
receiving
great
attention
due
the
possibility
assemble
C−C
coupling,
olefin
metathesis,
hydration
other
reactions
with
exquisite
stereospecificity
displayed
by
enzymes.
Thus,
this
minireview
organized
based
on
action
species
(Pd,
Ru,
Au,
Ir,
Fe…)
different
Special
will
be
paid
design
sequential
processes
concurrent
cascades,
presenting
solutions
such
as
use
surfactants
or
compartmentalization
strategies
for
those
cases
where
incompatibilities
could
hamper
overall
process.
Macromolecules,
Journal Year:
2023,
Volume and Issue:
56(3), P. 751 - 761
Published: Feb. 3, 2023
Reversible
deactivation
radical
polymerization
(RDRP)
is
a
set
of
powerful
and
versatile
methods
for
the
synthesis
well-defined
polymers.
Over
past
two
decades,
engagement
biocatalysts,
namely,
enzymes
bacteria,
has
granted
distinctive
features
to
RDRP
propelled
toward
more
sustainable
future.
In
this
Perspective,
we
highlight
green
conditions,
oxygen
tolerance,
function,
ability
access
difficult
polymers
in
conducted
by
biocatalysis
(bio-RDRP),
discuss
major
considerations
when
conducting
bio-RDRP,
point
out
drawbacks
bottlenecks
that
limit
its
further
development.
The
future
bio-RDRP
may
benefit
from
expanding
biocatalyst
library,
improving
redox
potential
enhancing
robustness,
in-depth
mechanistic
studies.
Organic Process Research & Development,
Journal Year:
2024,
Volume and Issue:
28(5), P. 1308 - 1326
Published: March 8, 2024
Flow
chemistry
as
well
biocatalysis
contribute
to
achieve
green
industries
and
sustainable
development.
Now
there
is
an
approach
that
combines
them,
called
flow
biocatalysis,
which
attracts
more
attention.
In
enzyme
immobilization
plays
a
powerful
role
in
promoting
its
This
review
begins
with
general
introduction
of
then
provides
update
on
the
application
immobilized
enzymes
biocatalysis.
Oxidation–reduction,
hydrolysis–esterification,
transferase
reaction,
condensation,
carboxylation,
multistep
cascade
reactions
continuous-flow
process
are
discussed
detail.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(9), P. 6462 - 6469
Published: April 12, 2024
Protein
engineering
is
essential
for
improving
the
catalytic
performance
of
enzymes
applications
in
biocatalysis,
which
machine
learning
provides
an
emerging
approach
variant
design.
Transaminases
are
powerful
biocatalysts
stereoselective
synthesis
chiral
amines
but
one
major
challenge
their
limited
substrate
scope.
We
present
a
general
and
practical
design
protocol
protein
to
combine
advantages
three
strategies,
including
directed
evolution,
rational
design,
learning,
demonstrate
application
transaminases
with
higher
activity
toward
bulky
substrates.
A
high-quality
data
set
was
obtained
by
selected
key
positions,
then
applied
create
model
transaminase
activity.
This
data-assisted
optimized
variants,
showed
improved
(up
3-fold
over
parent)
substrates,
maintaining
enantioselectivity
starting
enzyme
scaffold
as
well
enantiomeric
excess
>99%ee).
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(38)
Published: July 1, 2024
While
plastics
like
polyethylene
terephthalate
can
already
be
degraded
efficiently
by
the
activity
of
hydrolases,
other
synthetic
polymers
polyurethanes
(PUs)
and
polyamides
(PAs)
largely
resist
biodegradation.
In
this
study,
we
solved
first
crystal
structure
metagenomic
urethanase
UMG-SP-1,
identified
highly
flexible
loop
regions
to
comprise
active
site
residues,
targeted
a
total
20
potential
hot
spots
site-saturation
mutagenesis.
Engineering
campaigns
yielded
variants
with
single
mutations,
exhibiting
almost
3-
8-fold
improved
against
stable
N-aryl
urethane
amide
bonds,
respectively.
Furthermore,
demonstrated
release
corresponding
monomers
from
thermoplastic
polyester-PU
PA
(nylon
6)
single,
metagenome-derived
after
short
incubation
times.
Thereby,
expanded
hydrolysis
profile
UMG-SP-1
beyond
reported
low-molecular
weight
carbamates.
Together,
these
findings
promise
advanced
strategies
for
bio-based
degradation
recycling
plastic
materials
waste,
aiding
efforts
establish
circular
economy
polymers.
