ACS Sustainable Chemistry & Engineering,
Год журнала:
2024,
Номер
12(27), С. 10221 - 10228
Опубликована: Июнь 24, 2024
Transforming
gaseous
waste
CO2
as
a
C1
feedstock
into
fine
chemicals
is
significant
for
green
chemistry
and
sustainable
development.
Herein,
the
novel
Ag(I)-functionalized
polyoxoniobate-based
coordination
polymer
{[Ag(tpy)]5[Nb10O28]}[Ag(H2O)]·5H2O
(1,
tpy
=
2,2′:6′,2″-terpyridine)
successfully
fabricated
fully
characterized.
Compound
1
not
only
displays
excellent
thermal
solvent
stabilities
but
can
also
efficiently
selectively
catalyze
solvent-free
carboxylative
cyclization
of
terminal
propargylic
alcohols
with
different
substituents
to
high-value-added
α-alkylidene
cyclic
carbonates
at
room
temperature.
The
prominent
performance
attributed
synergistic
operation
Ag(I)
[Nb10O28]
in
its
structure,
which
responsible
activating
C≡C
bond
hydroxyl
group
alcohols,
respectively.
catalyst
exhibits
outstanding
sustainability;
no
obvious
decrease
catalytic
activity
observed
during
five
successive
cycles,
yield
carbonate
gram-scale
(100
mmol,
8.4
g)
experiment
up
61.7%
(turnover
number
value
5144).
To
best
our
knowledge,
this
represents
first
example
polyoxometalate-based
catalyzing
conversion
value-added
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(5), С. 2888 - 2894
Опубликована: Янв. 26, 2024
Catalytic
asymmetric
carboxylation
of
readily
available
alkenes
with
CO2,
an
abundant
and
sustainable
one-carbon
building
block,
that
gives
access
to
value-added
α-stereogenic
carboxylic
acids
in
atom-
step-economic
manner
is
highly
attractive.
However,
it
has
remained
a
formidable
challenge
for
the
synthetic
community.
Here,
first
example
Cu-catalyzed
regio-
enantioselective
boracarboxylation
reaction
on
various
arylalkenes
diboron
under
atmospheric
pressure
CO2
described,
which
afforded
variety
chiral
β-boron-functionalized
α-aryl
up
87%
yield
97%
ee
mild
conditions.
Importantly,
α-substituted
could
also
be
subject
this
protocol
excellent
enantiopurities,
thereby
rendering
efficient
approach
generation
enantioenriched
α-chiral
all-carbon
quaternary
center.
Moreover,
high
functional
group
tolerance,
scalable
synthesis,
facile
bioactive
compounds,
like
(−)-scopolamine,
(−)-anisodamine,
(−)-tropicamide,
further
demonstrated
utility
strategy.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(21), С. 14835 - 14843
Опубликована: Май 10, 2024
The
transformation
of
carbon
dioxide
(CO2)
into
functional
materials
has
garnered
considerable
worldwide
interest.
Metal–organic
frameworks
(MOFs),
as
a
distinctive
class
materials,
have
made
great
contributions
to
CO2
capture
and
conversion.
However,
facile
conversion
stable
porous
MOFs
for
utilization
remains
unexplored.
Herein,
we
present
methodology
using
synthesize
zirconium-based
MOFs.
Two
CO2–Zr-DEP
CO2–Zr-DEDP
with
face-centered
cubic
topology
were
obtained
via
sequential
desilylation–carboxylation–coordination
reaction.
exhibit
excellent
crystallinity,
verified
through
powder
X-ray
diffraction
high-resolution
transmission
electron
microscopy
analyses.
They
also
notable
porosity
high
surface
area
(SBET
up
3688
m2
g–1)
good
adsorption
capacity
(up
12.5
wt
%).
resulting
abundant
alkyne
moieties,
confirmed
13C
cross-polarization/magic
angle
spinning
nuclear
magnetic
resonance
Fourier
transform
infrared
spectra.
Leveraging
the
catalytic
prowess
Ag(I)
in
diverse
CO2-involved
reactions,
incorporated
MOFs,
capitalizing
on
their
interactions
carbon–carbon
π-bonds
alkynes,
thereby
forming
heterogeneous
catalyst.
This
catalyst
demonstrates
outstanding
efficiency
catalyzing
propargylic
alcohols
cyclic
carbonates,
achieving
>99%
yield
at
room
temperature
atmospheric
pressure
conditions.
Thus,
this
work
provides
dual
strategy,
encompassing
synthesis
CO2-based
(20–24
%
from
CO2)
subsequent
application
processes.
approach
significantly
enhances
overall
utilization.
Energy & Fuels,
Год журнала:
2024,
Номер
38(6), С. 4836 - 4880
Опубликована: Март 12, 2024
The
survival
and
sustainable
development
of
humanity
are
gravely
threatened
by
climate
change,
which
has
recently
been
elevated
to
the
status
one
greatest
threats
humanity's
security
on
a
worldwide
scale.
In
response
global
how
obtain
renewable
clean
fuels
is
an
important
challenge
for
human
society.
order
reach
carbon
peak
attain
neutrality,
using
CO2
as
resource
become
crucial
aim
civilization.
Converting
into
chemical
products
with
higher
added
value,
that
is,
utilization
technology
can
not
only
achieve
emission
reduction
but
also
have
certain
economic
benefits.
technologies
primarily
include
photocatalytic
reduction,
electrocatalytic
thermal
catalytic
relay
catalysis.
This
paper
mainly
summarizes
mechanism
conversion
research
related
catalysts,
discusses
prospects
system
(catalyst
modification,
product
selectivity
improvement,
etc.).
ideas
guidance
provided
efficient
stable
catalysts
application
in
areas
environment
energy.
Organic Letters,
Год журнала:
2024,
Номер
26(2), С. 467 - 472
Опубликована: Янв. 5, 2024
Disclosed
here
is
a
visible-light
photoredox-catalyzed
intermolecular
sequential
α-aminomethyl/carboxylative
dearomatization
of
indoles
with
CO2
and
α-aminoalkyl
radical
precursors,
affording
series
functionalized
indoline-3-carboxylic
acids
lactams
in
good
yields
high
regioselectivity.
This
multicomponent
reaction
provides
green
facile
method
for
the
synthesis
diverse
indolines
by
using
as
carboxylic
carbonyl
source.
Journal of CO2 Utilization,
Год журнала:
2024,
Номер
82, С. 102753 - 102753
Опубликована: Март 30, 2024
To
address
the
CO2
accumulation
in
atmosphere,
various
initiatives
have
been
proposed,
among
which
capture
and
utilization
(CCU)
is
regarded
as
an
appealing
strategy
to
reconcile
carbon
emission
resource
utilization.
Especially,
integrated
(ICCU),
i.e.
performing
in-situ
conversion
can
circumvent
energy-intensive
desorption
step
thus
facilitate
establishing
step-
energy-efficient
process,
rendering
at
mild
conditions
particularly
low
pressure
due
substantial
activation
upon
uptake.
However,
not
simple
add-up
of
these
two
processes.
Its
successful
implementation
relies
on
harmonization
reagents,
substrates
corresponding
catalysts.
By
far,
tremendous
efforts
made
this
field
a
plethora
reagents
including
inorganic
bases,
organic
ionic
liquids
carbonaceous
materials
utilized
protocols
such
hydrogenation,
cycloaddition,
carboxylative
cyclization
etc.
explored
for
captured
CO2.
As
result,
valuable
products
containing
methanol,
methane,
carbonates,
carbamates,
oxazolidinones,
ureas,
quinazolinone
obtained
from
more
importantly,
chemistry
theory
also
enriched
via
investigating
structure
reactivity
reactions.
In
review,
we
summarize
progress
based
reaction
types
absorbents.
It's
hoped
that
review
shed
light
design
inspire
further
development
field.
ACS Applied Materials & Interfaces,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 17, 2025
The
carbon
dioxide
(CO2)
capture
and
utilization
strategy
has
emerged
as
an
innovative
multifaceted
approach
to
counteract
emissions.
In
this
study,
a
highly
porous
muffin
polyhedral
barium
(Ba)
̵
organic
framework
(BaTATB;
H3TATB
=
4,4',4″-s-triazine-2,4,6-triyl-tribenzoic
acid)
was
synthesized
solvothermally.
three-dimensional
honeycomb
pore
architectures
were
densely
populated
with
Lewis
acidic
Ba(II)
metal
sites
basic
nitrogen-rich
triazines.
BaTATB
demonstrated
selective
CO2
adsorption
high
heat
of
adsorption.
Its
abundance
(Ba
clusters)
(triazine)
makes
ideal
catalyst
for
the
cycloaddition
epoxides
in
two-
three-component
reactions.
Furthermore,
is
exceptional
recyclable
aromatic
amines,
enabling
high-yield
synthesis
cyclic
carbonates
oxazolidinone
at
1
bar
under
moderate,
solvent-free,
cocatalyst-free
conditions.
Additionally,
recycled
nine
seven
consecutive
cycles
carbonate
no
substantial
decrease
catalytic
activity.
Using
density
functional
theory,
we
rational
design
metal-organic
frameworks
that
exhibit
excellent
conversion.
Nature Communications,
Год журнала:
2025,
Номер
16(1)
Опубликована: Фев. 21, 2025
Carboxylation
with
CO2
offers
an
attractive
and
sustainable
access
to
valuable
carboxylic
acids.
Among
these
methods,
direct
C−H
carboxylation
of
terminal
alkynes
has
attracted
much
attention
for
one-carbon
homologation
alkynes,
enabling
rapid
synthesis
propiolic
In
contrast,
the
multi-carbons
construct
important
non-conjugated
alkynyl-containing
acids
not
been
reported.
Herein,
we
present
alkynylcarboxylation
alkenes
via
photoredox
copper
dual
catalysis.
This
protocol
provides
a
practical
method
form
alkynyl
from
readily
available
CO2.
Additionally,
this
approach
also
features
mild
(room
temperature,
1
atm
CO2)
redox-neutral
conditions,
high
atom
step
economy,
good
functional
group
tolerance,
selectivities.
Moreover,
diverse
transformations
β-alkynyl
acid
products
bioactive
molecule
(GPR40/FFA1
agonist)
further
illustrate
synthetic
utility
methodology.
The
report
multi-carbon
is
rare.
authors
catalysis,
affording
Chemical Communications,
Год журнала:
2024,
Номер
60(12), С. 1599 - 1602
Опубликована: Янв. 1, 2024
Cobalt
porphyrin-based
hypercrosslinked
ionic
polymers
act
as
bifunctional
catalysts
for
the
conversion
of
CO
2
into
cyclic
carbonates
due
to
high
surface
areas,
densely
located
groups
and
highly
dispersed
cobalt
sites.