Angewandte Chemie,
Год журнала:
2022,
Номер
134(44)
Опубликована: Сен. 9, 2022
Abstract
The
use
of
temperature‐controlled
mechanochemistry
to
enable
the
mechanochemical
nickel‐catalyzed
Suzuki–Miyaura
coupling
is
herein
described.
Transitioning
from
a
capricious
room‐temperature
protocol,
through
heated,
PID‐controlled
programmable
jar
heater
manifold
was
required
deliver
an
efficient
method
for
aryl
sulfamates
(derived
ubiquitous
phenols)
and
boronic
acid
species.
Furthermore,
this
process
conducted
using
base‐metal
nickel
catalyst,
in
absence
bulk
solvent,
air/moisture
sensitive
reaction
set‐ups.
This
methodology
showcased
translation
large‐scale
twin‐screw
extrusion
enabling
200‐fold
scale
increase,
producing
decagram
quantities
C−C
coupled
material.
Carbon-carbon
(C─C)
bond
formation
is
a
key
step
in
diverse
chemical
processes
and
requires
high-performance
catalysts
to
enable
energy-efficient
technologies.
Here,
we
present
liquid
Pd
catalysts,
formed
by
dissolving
Ga,
for
high-turnover
C─C
coupling
reactions.
The
catalyst
achieved
turnover
frequency
of
2.5
×
10
8
hour
−1
model
reaction
at
70°C,
surpassing
all
reported
1000-fold.
Our
results
show
that
atoms
the
Ga
matrix
are
liquid-like,
exhibiting
unique
electronic
interfacial
properties
substantially
lower
energy
barrier
enhance
kinetics.
system
retained
full
activity
over
five
cycles
showed
no
leaching,
highlighting
transformative
potential
liquid-phase
metals
advance
high-throughput
sustainable
bond-forming
strategies.
Angewandte Chemie,
Год журнала:
2022,
Номер
134(44)
Опубликована: Сен. 9, 2022
Abstract
The
use
of
temperature‐controlled
mechanochemistry
to
enable
the
mechanochemical
nickel‐catalyzed
Suzuki–Miyaura
coupling
is
herein
described.
Transitioning
from
a
capricious
room‐temperature
protocol,
through
heated,
PID‐controlled
programmable
jar
heater
manifold
was
required
deliver
an
efficient
method
for
aryl
sulfamates
(derived
ubiquitous
phenols)
and
boronic
acid
species.
Furthermore,
this
process
conducted
using
base‐metal
nickel
catalyst,
in
absence
bulk
solvent,
air/moisture
sensitive
reaction
set‐ups.
This
methodology
showcased
translation
large‐scale
twin‐screw
extrusion
enabling
200‐fold
scale
increase,
producing
decagram
quantities
C−C
coupled
material.
