Analytical Chemistry,
Journal Year:
2023,
Volume and Issue:
95(5), P. 2865 - 2873
Published: Jan. 24, 2023
Nanozymes
can
imitate
the
catalytic
properties
of
natural
enzymes
while
overcoming
limitations
such
as
high
cost,
poor
robustness,
and
difficulty
in
recycling.
However,
rational
design
facile
preparation
nanozymes
are
still
demand.
Inspired
by
chemical
structure
laccase,
we
report
an
amorphous
metal-organic
coordination
nanocomposite
named
CuNAD,
which
is
composed
copper
ions
nicotinamide
adenine
dinucleotide
(NAD+)
via
a
simple
coordinating
coassembly
process.
As
single-site
nanozyme,
CuNAD
exhibits
excellent
robustness
under
extreme
conditions,
significantly
stronger
activity
for
phenolic
compounds,
4.02-fold
higher
sensitivity
epinephrine
detection
than
laccase.
Furthermore,
breaking
through
functional
constraints
also
able
to
activate
H2O2
at
neutral
pH,
benefiting
one-step
chromogenic
platform
cholesterol.
This
approach
demonstrates
potential
develop
biomimicking
may
boost
more
insights
into
structure-function
relationship
nanozymes.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(31), P. 16824 - 16855
Published: Jan. 16, 2021
Enzyme
catalysis
is
gaining
increasing
importance
in
synthetic
chemistry.
Nowadays,
the
growing
number
of
biocatalysts
accessible
by
means
bioinformatics
and
enzyme
engineering
opens
up
an
immense
variety
selective
reactions.
Biocatalysis
especially
provides
excellent
opportunities
for
late-stage
modification
often
superior
to
conventional
de
novo
synthesis.
Enzymes
have
proven
be
useful
direct
introduction
functional
groups
into
complex
scaffolds,
as
well
rapid
diversification
compound
libraries.
Particularly
important
highly
topical
are
enzyme-catalysed
oxyfunctionalisations,
halogenations,
methylations,
reductions,
amide
bond
formations
due
high
prevalence
these
motifs
pharmaceuticals.
This
Review
gives
overview
strengths
limitations
enzymatic
modifications
using
native
engineered
enzymes
synthesis
while
focusing
on
examples
drug
development.
Asian Journal of Organic Chemistry,
Journal Year:
2021,
Volume and Issue:
10(4), P. 711 - 748
Published: Feb. 11, 2021
Abstract
Photocatalyzed
organic
synthesis
transformation
is
a
remarkable
green
synthetic
strategy
because
of
the
advantages
operational
simplicity,
high
chemoselectivities,
cheap,
and
environmental
benignancy,
along
with
extensive
applications
in
fields
organic,
pharmaceutical
functional
material
chemistry.
Generally,
photoredox
catalysts
or
photosensitizers
are
necessary
for
generation
their
excited
states
to
perform
successive
oxidative
reductive
reactions
through
single
electron
transfer
(SET)
energy
(ET)
process.
Furthermore,
exploration
colored
donor‐acceptor
(EDA)
complex
charge
(CT)
between
an
electron‐rich
electron‐poor
substrate
provides
chance
deliver
intermediate
under
irradiation
light,
resulting
formation
radical
activate
species
induce
various
reactions.
These
were
performed
without
need
any
external
photocatalysts
mild
reaction
conditions.
Herein,
this
review
focuses
on
recent
progress
photoinduced
addition
reactions,
borylations,
radical‐radical
cross‐coupling
degradation
cascade
cyclization
via
EDA
complexes.
We
highlight
these
novel
methodologies
applications,
as
well
mechanisms.
This
will
help
provide
references
medicinal
chemists
who
charmed
by
photochemical
transformations
based
The Journal of Organic Chemistry,
Journal Year:
2022,
Volume and Issue:
87(16), P. 10555 - 10563
Published: July 29, 2022
Electron
donor–acceptor
(EDA)
complexes
provide
a
means
to
initiate
radical
reactions
under
visible
light
irradiation
using
substrates
that
do
not
absorb
individually.
Catalytic
approaches
complex
formation
are
vital
for
advancing
this
synthetic
strategy
as
it
decouples
the
complexation
and
photogeneration
of
radicals
from
substrate
functionalization,
limitation
inherent
stoichiometric
restricts
structural
diversity.
This
Synopsis
highlights
recent
developments
in
EDA
photochemistry
which
either
donor
or
acceptor
employed
catalytically.
Science,
Journal Year:
2022,
Volume and Issue:
376(6595), P. 869 - 874
Published: May 19, 2022
We
report
the
reprogramming
of
nonheme
iron
enzymes
to
catalyze
an
abiological
C(sp3)‒H
azidation
reaction
through
iron-catalyzed
radical
relay.
This
biocatalytic
transformation
uses
amidyl
radicals
as
hydrogen
atom
abstractors
and
Fe(III)‒N3
intermediates
trapping
agents.
established
a
high-throughput
screening
platform
based
on
click
chemistry
for
rapid
evolution
catalytic
performance
identified
enzymes.
The
final
optimized
variants
deliver
range
products
with
up
10,600
total
turnovers
93%
enantiomeric
excess.
Given
prevalence
relay
reactions
in
organic
synthesis
diversity
enzymes,
we
envision
that
this
discovery
will
stimulate
future
development
metalloenzyme
catalysts
synthetically
useful
transformations
unexplored
by
natural
evolution.
Science,
Journal Year:
2023,
Volume and Issue:
381(6656), P. 444 - 451
Published: July 27, 2023
Developing
synthetically
useful
enzymatic
reactions
that
are
not
known
in
biochemistry
and
organic
chemistry
is
an
important
challenge
biocatalysis.
Through
the
synergistic
merger
of
photoredox
catalysis
pyridoxal
5'-phosphate
(PLP)
biocatalysis,
we
developed
a
radical
biocatalysis
approach
to
prepare
valuable
noncanonical
amino
acids,
including
those
bearing
stereochemical
dyad
or
triad,
without
need
for
protecting
groups.
Using
engineered
PLP
enzymes,
either
enantiomeric
product
could
be
produced
biocatalyst-controlled
fashion.
Synergistic
