Organic Letters,
Journal Year:
2024,
Volume and Issue:
26(7), P. 1489 - 1494
Published: Feb. 15, 2024
A
novel
approach
using
aromatic
amines
and
chiral
phosphoric
acids
in
a
synergistic
catalytic
cascade
reaction
of
2-alkynylnaphthols
with
aldehydes
has
been
established.
This
method
offers
direct
route
to
preparing
flavanone
analogues
excellent
stereoselectivity.
Mechanistic
studies
reveal
sequential
process
involving
addition,
elimination,
cyclization,
hydrolysis
which
play
key
roles
via
imine-enamine
hydrogen
bonding
models.
Science,
Journal Year:
2024,
Volume and Issue:
383(6678), P. 77 - 81
Published: Jan. 4, 2024
Catalytic
methods
to
couple
alkene
and
amine
feedstocks
are
valuable
in
synthetic
chemistry.
The
direct
carbonylative
coupling
of
alkenes
amines
holds
promise
as
a
perfectly
atom-economical
approach
amide
synthesis,
but
general
remain
underdeveloped.
Herein,
we
report
an
hydroaminocarbonylation
catalyzed
by
unmodified,
inexpensive
cobalt
carbonyl
under
mild
conditions
low
pressure
promoted
light.
Silane
addition
after
the
reaction
enables
sequential
cobalt-catalyzed
reduction,
constituting
formal
hydroaminomethylation.
These
exhibit
exceptional
scope
across
both
components
with
high
chemo-
regioselectivity
proceed
efficiently
even
absence
solvent.
formation
hydridocobalt
through
photodissociation
ligand
is
proposed
enable
catalytic
activity
conditions,
which
addresses
long-standing
challenge
catalysis.
Chemical Communications,
Journal Year:
2024,
Volume and Issue:
60(50), P. 6340 - 6361
Published: Jan. 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.
Organic Chemistry Frontiers,
Journal Year:
2024,
Volume and Issue:
11(10), P. 2762 - 2767
Published: Jan. 1, 2024
A
P(NMe2)3-catalyzed
[4
+
2]
annulation
of
2-amino-β-nitrostyrenes
and
β′-acetoxy
allenoates
followed
by
a
Zn/AcOH-mediated
reduction–hydroamination–isomerization
has
been
developed.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 9, 2025
The
direct
synthesis
of
C(sp3)-rich
architectures
is
a
driving
force
for
innovation
in
synthetic
organic
chemistry.
Such
scaffolds
impart
beneficial
properties
onto
drug
molecules
that
correlate
with
greater
clinical
success.
Consequently,
there
strong
impetus
to
develop
new
methods
by
which
access
sp3-rich
from
commercial
feedstocks,
such
as
alkenes.
Herein,
we
report
three-component
aminoalkylation
reaction
utilizes
the
principles
triple
radical
sorting
regioselectively
add
N-centered
and
C-centered
radicals
across
This
process
relies
upon
photoredox
catalysis
transform
alkyl
bromides
reductively
activated
precursors
into
high-energy
species
redox-neutral
fashion.
A
broad
scope
coupling
partners
demonstrated,
multiple
applications,
including
facile
syntheses
pharmacophoric
substituted
N-heterocycles.
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 20, 2025
Due
to
their
conductive
properties
and
optoelectronic
tunability,
MXenes
have
revolutionized
the
area
of
electrocatalysis
active
materials
in
supercapacitors.
In
comparison,
there
are
only
a
few
reports
on
as
thermal
catalysts
for
general
organic
reactions.
Herein,
unprecedented
catalytic
activity
Ti3C2
MXene
hydroamination
alkynes
is
reported,
overcoming
limitations
poor
activity,
lack
selectivity,
stability,
which
generally
encountered
solid
known
so
far.
case
Ti3C2,
exhibits
almost
complete
selectivity
anti-Markovnikov
regioisomer,
both
aliphatic
amines
less-reactive
aromatic
amines.
also
efficiently
catalyzes
intramolecular
hydroamination,
leading
formation
indol
heterocycles.
The
C-C
multiple
bonds
reaction
with
atom
efficiency
that
may
form
C-N
from
convenient
reagents.
maximum
number
sites
nanosheets
quantified
by
thermoprogrammed
NH3
desorption.
measured
TOF
values
order
102
h-1,
highest
value
being
350
h-1
1-hexyne
n-butylamine.
Therefore,
among
heterogeneous
studied,
its
per
site
comparable
best
reported
Density
functional
theory
calculations
models
indicate
cooperation
neighboring
Ti
atoms
mechanism.
Considering
compositional
structural
versatility
MXenes,
present
findings
open
door
further
application
other
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(40), P. 21738 - 21744
Published: Oct. 3, 2023
We
report
a
light-driven
method
for
the
intermolecular
anti-Markovnikov
hydroamination
of
alkenes
with
primary
heteroaryl
amines.
In
this
protocol,
electron
transfer
between
an
amine
substrate
and
excited-state
iridium
photocatalyst
affords
aminium
radical
cation
(ARC)
intermediate
that
undergoes
C–N
bond
formation
nucleophilic
alkene.
Integral
to
reaction
success
is
electronic
character
amine,
wherein
increasingly
electron-deficient
amines
generate
reactive
ARCs.
Counteranion-dependent
reactivity
observed,
triflate
photocatalysts
are
employed
in
place
conventional
hexafluorophosphate
complexes.
This
exhibits
broad
functional
group
tolerance
across
55
examples
N-alkylated
products
derived
from
pharmaceutically
relevant
Accounts of Chemical Research,
Journal Year:
2024,
Volume and Issue:
57(13), P. 1827 - 1838
Published: June 21, 2024
ConspectusChemists
have
long
been
inspired
by
biological
photosynthesis,
wherein
a
series
of
excited-state
electron
transfer
(ET)
events
facilitate
the
conversion
low
energy
starting
materials
such
as
H
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(6), P. 4053 - 4065
Published: March 1, 2024
Chiral
recognition
for
the
synthesis
of
axially
chiral
biaryl
units
is
a
fundamental
and
challenging
topic
in
organic
synthesis.
Herein,
we
documented
that
an
efficient
O-ligand
exchange
between
catalyst
substrate
enabled
axial
asymmetric
aminopalladation/olefination
2-alkynylanilides
vinyl
trifluoromethanesulfonates,
providing
3-alkenylindoles
with
up
to
97%
ee
98%
yield.
This
protocol
features
mild
conditions,
broad
functional
group
tolerance,
scalability,
late-stage
modification
bioactive
molecules.
Experimental
computational
studies
hinted
(R)-BIDIME/Pd
complex
alkoxy
was
crucial
success
stereoselectivity
control.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(41)
Published: Aug. 23, 2023
An
iridium-catalyzed
remote
site-switchable
hydroarylation
of
alkenes
was
reported,
delivering
the
products
functionalized
at
subterminal
methylene
and
terminal
methyl
positions
on
an
alkyl
chain
controlled
by
two
different
ligands,
respectively,
in
good
yields
with
to
excellent
site-selectivities.
The
catalytic
system
showed
functional
group
tolerance
a
broad
substrate
scope,
including
unactivated
activated
alkenes.
More
importantly,
regioconvergent
transformations
mixtures
isomeric
were
also
successfully
realized.
results
mechanistic
studies
demonstrate
that
reaction
undergoes
chain-walking
process
give
[Ar-Ir-H]
complex
alkene.
subsequent
processes
proceed
through
modified
Chalk-Harrod-type
mechanism
via
migratory
insertion
alkene
into
Ir-C
bond
followed
C-H
reductive
elimination
afford
hydrofunctionalization
site-selectively.
ChemCatChem,
Journal Year:
2024,
Volume and Issue:
16(16)
Published: March 23, 2024
Abstract
The
N‐methylation
reaction
of
amines
with
methanol
via
the
borrowing‐hydrogen
strategy
is
an
important
method
for
construction
C−N
bonds.
Compared
other
C1
sources,
such
as
toxic
formaldehyde
or
expensive
formic
acid,
more
suitable
reactions
due
to
its
eco‐friendliness
and
low
price.
Using
this
strategy,
various
types
N‐methylated
products,
including
biological
pharmaceutical
molecules
have
been
prepared.
Here,
we
present
a
thorough
survey
decades
articles
showing
current
developments
in
methanol.
We
discuss
homogenous,
heterogenous
light‐driven
catalytic
systems
both
N,N‐dimethylation
reactions.
This
review
presents
shortcomings
provides
future
development
progress
