Inorganic Chemistry,
Год журнала:
2022,
Номер
61(5), С. 2695 - 2705
Опубликована: Янв. 24, 2022
We
report
herein
an
exploration
of
the
straightforward
one-pot
dual-catalysis
strategy,
i.e.,
direct
combination
a
photoactive
coordination
polymer
(CP)
with
another
metal
catalyst,
for
carrying
out
desirable
photoinduced
organic
transformation.
The
strategy
overcomes
necessity
presynthesis
metal/CP
composite
that
has
been
demonstrated
to
be
invalid
in
our
case.
A
new
two-dimensional
CP
showing
properties
wide-range
visible-light
absorption
and
efficient
charge
generation
was
synthesized
via
solvothermal
reaction.
successfully
applied
photocatalytic
C-C
cross-coupling
reaction
method,
simple
ligand-free
palladium
salt
Pd(OAc)2
as
catalyst.
features
short
time,
mild
conditions,
good
recyclability,
high
yield
Heck
products
from
broad
variety
substrates.
comparative
experiment
showed
presynthesized
Pd/CP
reaction,
demonstrating
significance
strategy.
Mechanistic
studies
suggest
depends
on
synergy
between
photocatalysis
generate
reactive
aryl
radicals
Pd
catalysis
target
products,
which
interfacial
electron
transfer
vital
producing
transient
catalytically
active
Pd(0)
species
near
surface
CP.
study
shows
photocatalyst
catalyst
is
highly
feasible
method
photochemical
enhances
prospects
application
CPs.
Organic Process Research & Development,
Год журнала:
2023,
Номер
27(2), С. 322 - 330
Опубликована: Янв. 16, 2023
A
proof-of-concept
study
for
the
synthesis
of
1,2-difluorobenzene
from
2-fluoroaniline
via
Balz–Schiemann
reaction
using
HF/pyridine
as
fluorinating
reagent
is
reported.
Key
to
success
a
fast
reaction,
clean
profile─and
thus
high
product
selectivity─was
photochemically
induced
fluorodediazoniation
in
situ-generated
diazonium
salt
performed
continuous
flow
mode.
high-power
365
nm
light-emitting
diode
provided
more
robust
and
efficient
irradiation
system
compared
medium-pressure
Hg
lamp
with
respect
performance
on
scale-out
runs
time,
allowing
generation
within
10
min
residence
time
selectivity
≥95%
at
full
conversion.
Organic Letters,
Год журнала:
2020,
Номер
22(24), С. 9490 - 9494
Опубликована: Ноя. 24, 2020
The
first
coupling
of
α-allenols,
sulfur
dioxide,
and
arenediazonium
salts
is
presented.
three-component
reaction
which
promoted
by
visible
light
can
be
easily
accomplished
using
DABSO
as
a
dioxide
surrogate
in
the
presence
photoredox
catalyst.
In
this
manner,
broad
range
electron-rich
electron-deficient
aryl
substituents
are
well
accommodated
sulfonylation–rearrangement
cascade
to
afford
2,2-disubstituted
3-(arylsulfonyl)but-3-enals
reasonable
yields.
Based
on
control
experiments,
radical
mechanism
does
imply
1,2-aryl
migration
has
been
proposed.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(2)
Опубликована: Ноя. 22, 2022
Abstract
Among
the
tools
available
to
chemists
for
drug
design
of
bioactive
compounds,
bioisosteric
replacement
atoms
or
groups
is
cornerstone
modern
strategies.
Despite
undeniable
interest
in
amino‐to‐hydroxyl
interchange,
enzymatic
deaminative
hydroxylation
remains
unmatched.
Herein,
we
report
a
user
friendly
and
safe
procedure
selectively
convert
aminoheterocycles
their
hydroxylated
analogues
by
means
simple
pyrylium
tetrafluoroborate
salt.
The
step
relies
on
Lossen‐type
rearrangement
under
mild
conditions
thus
avoiding
use
strong
hydroxide
bases.
In
addition
biorelevant
heterocycles,
electron‐deficient
anilines
was
also
demonstrated.
Finally,
mechanistic
experiments
allowed
identification
key
intermediates,
unveiling
rather
unusual
mechanism
this
formal
aromatic
substitution.
Inorganic Chemistry,
Год журнала:
2022,
Номер
61(5), С. 2695 - 2705
Опубликована: Янв. 24, 2022
We
report
herein
an
exploration
of
the
straightforward
one-pot
dual-catalysis
strategy,
i.e.,
direct
combination
a
photoactive
coordination
polymer
(CP)
with
another
metal
catalyst,
for
carrying
out
desirable
photoinduced
organic
transformation.
The
strategy
overcomes
necessity
presynthesis
metal/CP
composite
that
has
been
demonstrated
to
be
invalid
in
our
case.
A
new
two-dimensional
CP
showing
properties
wide-range
visible-light
absorption
and
efficient
charge
generation
was
synthesized
via
solvothermal
reaction.
successfully
applied
photocatalytic
C-C
cross-coupling
reaction
method,
simple
ligand-free
palladium
salt
Pd(OAc)2
as
catalyst.
features
short
time,
mild
conditions,
good
recyclability,
high
yield
Heck
products
from
broad
variety
substrates.
comparative
experiment
showed
presynthesized
Pd/CP
reaction,
demonstrating
significance
strategy.
Mechanistic
studies
suggest
depends
on
synergy
between
photocatalysis
generate
reactive
aryl
radicals
Pd
catalysis
target
products,
which
interfacial
electron
transfer
vital
producing
transient
catalytically
active
Pd(0)
species
near
surface
CP.
study
shows
photocatalyst
catalyst
is
highly
feasible
method
photochemical
enhances
prospects
application
CPs.
