Crystal Growth & Design,
Год журнала:
2025,
Номер
25(5), С. 1636 - 1643
Опубликована: Фев. 19, 2025
Developing
a
mechanochemical,
solvent-free
approach
for
forming
C–C
bonds
in
place
of
traditional
solvent-based
synthesis
is
significant
green
chemistry.
Herein,
novel
Cu-complex-functionalized
polyoxoniobate-based
hybrid
material
[Cu(tpy)2]{[Cu(tpy)(H2O)]2[Nb10O28]}·5.5H2O
(1,
tpy
=
2,2′:6′,2″-terpyridine)
successfully
synthesized
and
thoroughly
characterized.
1
displays
excellent
thermal
solvent
stability
highly
mechanical
force
tolerant.
Catalytic
studies
reveal
that
can
catalyze
the
Knoevenagel
condensations
series
aromatic
aldehydes
with
malononitrile
to
build
bond
compounds
under
mechanochemical
ball
milling
conditions.
The
catalytic
system
conducted
no
additional
heating,
lower
oscillating
frequency,
without
solvent.
remarkable
performance
catalyst
be
attributed
two
factors:
one
sufficient
contact
between
reagents
facilitated
by
force,
as
well
preactivated
it;
other
synergistic
effect
Lewis
acid–base
sites
(Cu2+
[Nb10O28]6–)
within
catalyst.
exhibits
outstanding
recyclability
applied
gram-scale
reactions.
To
best
our
knowledge,
this
work
represents
first
example
mechanochemically
driven
organic
transformation
using
polyoxometalate-based
Chemical Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
In
this
study,
we
present
the
first
general
mechanochemical
protocol
for
catalytic
[2+2+2]
cycloaddition
of
alkynes
via
a
simple
and
inexpensive
cobalt(
ii
)-based
system
in
combination
with
piezoelectric
BaTiO
3
.
Herein,
we
report
the
development
of
first
general
mechanochemical
protocol
for
Buchwald-Hartwig
cross-coupling
using
aromatic
primary
amines
as
nucleophiles.
The
arylamination
reactions
were
rapid
and
completed
within
30
min
most
substrates,
all
synthetic
operations
carried
out
in
air.
Notably,
this
approach
effectively
facilitated
poorly
soluble
aryl
halides,
which
are
barely
reactive
solution.
In
addition,
demonstrated
that
a
two-step
one-pot
sequence
enables
rapid,
efficient,
solvent-free,
time-economical,
modular
synthesis
various
unsymmetrical
triarylamines.
Advanced Synthesis & Catalysis,
Год журнала:
2024,
Номер
366(9), С. 2035 - 2043
Опубликована: Фев. 8, 2024
Abstract
Our
research
has
demonstrated
that
mechanochemical
activation
is
more
effective
with
solid
reagents.
We
have
showcased
the
practicality
of
Bertagnini's
salts,
also
called
aldehyde‐bisulfite
adducts,
which
are
crystalline,
simplifying
preparation
and
storage.
These
salts
stable
substitutes
for
liquid
aldehydes
ketones
been
employed
in
reductive
amination,
synthesizing
aza‐heterocycles
hydrazones
within
mechanochemistry.
The
technique‘s
effectiveness
broadens
substrate
scopes,
simplifies
purification,
reduces
reaction
times,
yields
desired
products
ranging
from
38–91%.
Additionally,
thermal
stability
bisulfite
adducts
confirmed
through
TGA
(Thermogravimetric
analysis)
analysis.
