Chemistry - An Asian Journal,
Год журнала:
2022,
Номер
17(19)
Опубликована: Авг. 8, 2022
Herein,
we
developed
two
distinct
pyridine
N-oxide
directed
C-H
activation
protocols
to
achieve
[4+1]
annulation
and
alkoxylation
of
benzamide
derivatives
by
merging
Co-catalysis
with
visible-light
photoredox
catalysis.
The
deliver
the
respective
products
in
good
yields
under
facile
conditions
at
room
temperature.
use
an
inexpensive
photocatalyst
coupled
molecular
oxygen
bypassing
need
stoichiometric
oxidants
forms
chief
highlight
work.
are
scalable
could
be
further
modified.
Additionally,
preliminary
studies
were
carried
out
probe
reaction
mechanism.
Chemical Reviews,
Год журнала:
2023,
Номер
123(8), С. 4237 - 4352
Опубликована: Янв. 24, 2023
The
emergence
of
modern
photocatalysis,
characterized
by
mildness
and
selectivity,
has
significantly
spurred
innovative
late-stage
C–H
functionalization
approaches
that
make
use
low
energy
photons
as
a
controllable
source.
Compared
to
traditional
strategies,
photocatalysis
paves
the
way
toward
complementary
and/or
previously
unattainable
regio-
chemoselectivities.
Merging
compelling
benefits
with
workflow
offers
potentially
unmatched
arsenal
tackle
drug
development
campaigns
beyond.
This
Review
highlights
photocatalytic
strategies
small-molecule
drugs,
agrochemicals,
natural
products,
classified
according
targeted
bond
newly
formed
one.
Emphasis
is
devoted
identifying,
describing,
comparing
main
mechanistic
scenarios.
draws
critical
comparison
between
established
ionic
chemistry
photocatalyzed
radical-based
manifolds.
aims
establish
current
state-of-the-art
illustrate
key
unsolved
challenges
be
addressed
in
future.
authors
aim
introduce
general
readership
functionalization,
specialist
practitioners
evaluation
methodologies,
potential
for
improvement,
future
uncharted
directions.
Abstract
Despite
the
rich
photochemistry
of
3d‐metal
complexes,
utilization
excited‐state
reactivity
these
compounds
in
organic
synthesis
has
been
historically
overlooked.
The
advent
photoredox
catalysis
changed
perception
synthetic
chemists
towards
photochemistry,
and
nowadays
potential
photoinduced,
outer‐sphere
single‐electron
transfer
events
is
widely
recognized.
More
recently,
an
emerging
new
mode
photoactivation
taken
spotlight,
based
on
inner‐sphere
triggered
by
population
ligand‐to‐metal
charge‐transfer
(LMCT)
excited
states.
Contrarily
to
photoredox,
LMCT‐activation
does
not
rely
matching
redox
potentials,
offers
unique
profiles
particularly
well
suited
Earth‐abundant
metal
complexes.
Those
appealing
features
are
propelling
development
methods
using
this
blueprint
generate
highly
reactive
open‐shell
species
under
mild
conditions.
aim
contribution
provide
a
didactical
tool
for
comprehension
concept
facilitate
methodologies
achieve
sustainable
chemical
transformations.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(19), С. 10480 - 10485
Опубликована: Май 8, 2023
We
establish
a
synthetically
convenient
method
to
degrade
polyacrylate
homopolymers.
Carboxylic
acids
are
installed
along
the
polymer
backbone
by
partial
hydrolysis
of
ester
side
chains,
and
then,
in
one-pot
sequential
procedure,
carboxylic
converted
into
alkenes
oxidatively
cleaved.
This
process
enables
robustness
properties
polyacrylates
be
maintained
during
their
usable
lifetime.
The
ability
tune
degree
degradation
was
demonstrated
varying
acid
content
polymers.
is
compatible
with
wide
range
polymers
prepared
from
vinyl
monomers
through
copolymerization
acrylic
different
including
acrylates,
acrylamides,
styrenics.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(7), С. 4375 - 4379
Опубликована: Фев. 1, 2024
We
demonstrate
hydrohalogenation
of
aliphatic
alkenes
with
collidine·HX
salts
through
dual
photoredox/cobalt
catalysis.
The
catalysis
enables
conversion
a
proton
and
halide
anion
from
salt
to
nucleophilic
hydrogen
radical
equivalent
an
electrophilic
halogen
delivery
them
alkene
moiety.
This
protocol
allows
for
introduction
fluorine,
chlorine,
bromine,
or
iodine
atom
alkene,
producing
highly
functionalized
alkyl
halides.
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
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(19)
Опубликована: Фев. 28, 2024
Abstract
We
report
a
general,
intramolecular
cycloisomerization
of
unactivated
olefins
with
pendant
nucleophiles.
The
reaction
proceeds
under
mild
conditions
and
tolerates
ethers,
esters,
protected
amines,
acetals,
pyrazoles,
carbamates,
arenes.
It
is
amenable
to
N
‐,
O
as
well
C
‐nucleophiles,
yielding
number
different
heterocycles
including,
but
not
limited
to,
pyrrolidines,
piperidines,
oxazolidinones,
lactones.
Use
both
benzothiazinoquinoxaline
organophotocatalyst
Co‐salen
catalyst
obviates
the
need
for
stoichiometric
oxidant
or
reductant.
showcase
utility
protocol
in
late‐stage
drug
diversification
synthesis
several
small
natural
products.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(50), С. 23001 - 23009
Опубликована: Дек. 8, 2022
A
new
regio-
and
stereoselective
reductive
coupling
of
alkynes
crotononitrile
has
been
developed
via
visible
light
organophotoredox
cobalt
dual
catalysis.
variety
enantioenriched
homoallylic
nitriles
bearing
a
stereodefined
trisubstituted
alkene
have
easily
synthesized
with
good
to
excellent
(up
>20:1
rr),
stereo-
(>20:1
E/Z),
enantioselectivity
98%
ee)
control
under
mild
conditions.
The
corresponding
nitrile
products
were
smoothly
converted
into
various
chiral
building
blocks.
Remarkably,
simple
organic
base
together
water
utilized
as
hydrogen
sources
in
this
photoinduced
reaction.
Chemical Communications,
Год журнала:
2024,
Номер
60(50), С. 6340 - 6361
Опубликована: Янв. 1, 2024
In
this
review,
the
state-of-the-art
advances
in
radical-involved
C(sp
3
)–N
bond
formation
via
metallaphotoredox
catalysis
have
been
highlighted,
which
are
organized
according
to
different
catalytic
modes,
reaction
types,
and
substrate
classes.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(33)
Опубликована: Май 22, 2024
Abstract
Drawing
inspiration
from
nature
has
long
been
a
cornerstone
of
chemical
innovation,
with
natural
systems
offering
wealth
untapped
potential
for
discovery.
In
this
minireview,
we
delve
into
the
burgeoning
field
cobaloxime
catalysis
in
organic
synthesis,
which
mimics
catalytic
activity
organometallic
alkylcobalamine
enzymes.
Our
focus
lies
on
elucidating
latest
advancements
area,
as
well
delineating
primary
mechanistic
pathways
at
play.
By
describing,
and
comparing
these
mechanisms,
provide
comprehensive
overview
current
state‐of‐the‐art,
while
also
shedding
light
key
unresolved
challenges
that
await
further
exploration.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(3)
Опубликована: Ноя. 17, 2022
Abstract
Due
to
its
mild
reaction
conditions
and
unique
chemoselectivity,
hydrogen
atom
transfer
(HAT)
hydrogenation
represents
an
indispensable
method
for
the
synthesis
of
complex
molecules.
Its
analog
using
deuterium,
deuterium
(DAT)
deuteration,
is
expected
enable
access
deuterium‐labeled
compounds.
However,
DAT
deuteration
has
been
scarcely
studied
synthetic
purposes,
a
that
possesses
favorable
characteristics
HAT
hydrogenations
remained
elusive.
Herein,
we
report
protocol
photocatalytic
electron‐deficient
alkenes.
In
contrast
previous
this
tolerates
variety
synthetically
useful
functional
groups
including
haloarenes.
The
late‐stage
also
allows
deuterated
amino
acids
as
well
donepezil‐
d
2
.
Thus,
work
demonstrates
potential
chemistry
become
alternative
choice
preparing
deuterium‐containing
