Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(38), С. 25976 - 25985
Опубликована: Авг. 8, 2024
Cerium
photoredox
catalysis
has
emerged
as
a
powerful
strategy
to
activate
molecules
under
mild
conditions.
Radical
intermediates
are
formed
using
visible
light
and
simple
complexes
of
the
earth-abundant
lanthanide.
Here,
we
report
an
artificial
photoenzyme
enabling
this
chemistry
inside
protein.
We
utilize
de
novo
designed
protein
scaffold
that
tightly
binds
lanthanide
ions
in
its
central
cavity.
Upon
visible-light
irradiation,
cerium-dependent
enzyme
catalyzes
radical
C-C
bond
cleavage
1,2-diols
aqueous
solution.
Protein
engineering
led
variants
with
improved
photostability
metal
binding
behavior.
The
cleaves
range
aromatic
aliphatic
substrates,
including
lignin
surrogates.
Surface
display
on
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(3), С. 1068 - 1089
Опубликована: Янв. 1, 2024
Leveraging
light
energy
to
expose
the
‘dark’
reactive
states
describes
whole
essence
of
triplet–triplet
transfer.
This
offers
an
impressive
opportunity
conduct
a
multitude
diverse
reactions
and
access
sought-after
molecular
motifs.
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 5459 - 5520
Опубликована: Апрель 28, 2023
Biocatalysis
has
revolutionized
chemical
synthesis,
providing
sustainable
methods
for
preparing
various
organic
molecules.
In
enzyme-mediated
most
reactions
involve
molecules
operating
from
their
ground
states.
Over
the
past
25
years,
there
been
an
increased
interest
in
enzymatic
processes
that
utilize
electronically
excited
states
accessed
through
photoexcitation.
These
photobiocatalytic
a
diverse
array
of
reaction
mechanisms
are
complementary
to
one
another.
This
comprehensive
review
will
describe
state-of-the-art
strategies
photobiocatalysis
synthesis
until
December
2022.
Apart
reviewing
relevant
literature,
central
goal
this
is
delineate
mechanistic
differences
between
general
employed
field.
We
organize
based
on
relationship
photochemical
step
and
transformations.
The
include
studies,
substrate
scopes,
protein
optimization
strategies.
By
clearly
defining
mechanistically-distinct
chemistry,
we
hope
illuminate
future
synthetic
opportunities
area.
Chemical Reviews,
Год журнала:
2024,
Номер
124(14), С. 8740 - 8786
Опубликована: Июль 3, 2024
In
recent
years,
powerful
genetic
code
reprogramming
methods
have
emerged
that
allow
new
functional
components
to
be
embedded
into
proteins
as
noncanonical
amino
acid
(ncAA)
side
chains.
this
review,
we
will
illustrate
how
the
availability
of
an
expanded
set
building
blocks
has
opened
a
wealth
opportunities
in
enzymology
and
biocatalysis
research.
Genetic
provided
insights
enzyme
mechanisms
by
allowing
introduction
spectroscopic
probes
targeted
replacement
individual
atoms
or
groups.
NcAAs
also
been
used
develop
engineered
biocatalysts
with
improved
activity,
selectivity,
stability,
well
enzymes
artificial
regulatory
elements
are
responsive
external
stimuli.
Perhaps
most
ambitiously,
combination
laboratory
evolution
given
rise
classes
use
ncAAs
key
catalytic
elements.
With
framework
for
developing
ncAA-containing
now
firmly
established,
optimistic
become
progressively
more
tool
armory
designers
engineers
coming
years.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(20), С. 13754 - 13759
Опубликована: Май 13, 2024
a-Tertiary
amino
acids
are
essential
components
of
drugs
and
agrochemicals,
yet
traditional
syntheses
step-intensive
provide
access
to
a
limited
range
structures
with
varying
levels
enantioselectivity.
Here,
we
report
the
α-alkylation
unprotected
alanine
glycine
by
pyridinium
salts
using
pyridoxal
(PLP)-dependent
threonine
aldolases
Rose
Bengal
photoredox
catalyst.
The
strategy
efficiently
prepares
various
a-tertiary
in
single
chemical
step
as
enantiomer.
UV–vis
spectroscopy
studies
reveal
ternary
interaction
between
salt,
protein,
photocatalyst,
which
hypothesize
is
responsible
for
localizing
radical
formation
active
site.
This
method
highlights
opportunity
combining
catalysts
enzymes
new
catalytic
functions
known
enzymes.
JACS Au,
Год журнала:
2024,
Номер
4(8), С. 2746 - 2766
Опубликована: Авг. 8, 2024
Photocatalysis
is
a
versatile
and
rapidly
developing
field
with
applications
spanning
artificial
photosynthesis,
photo-biocatalysis,
photoredox
catalysis
in
solution
or
supramolecular
structures,
utilization
of
abundant
metals
organocatalysts,
sustainable
synthesis,
plastic
degradation.
In
this
Perspective,
we
summarize
conclusions
from
an
interdisciplinary
workshop
young
principal
investigators
held
at
the
Lorentz
Center
Leiden
March
2023.
We
explore
how
diverse
fields
within
photocatalysis
can
benefit
one
another.
delve
into
intricate
interplay
between
these
subdisciplines,
by
highlighting
unique
challenges
opportunities
presented
each
multidisciplinary
approach
drive
innovation
lead
to
solutions
for
future.
Advanced
collaboration
knowledge
exchange
across
domains
further
enhance
potential
photocatalysis.
Artificial
photosynthesis
has
become
promising
technology
solar
fuel
generation,
instance,
via
water
splitting
CO
