Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Июнь 4, 2025
Fully
π-conjugated
organic
frameworks
(π-COFs)
have
attracted
considerable
attention
due
to
their
enhanced
stability
and
conductivity
compared
conventional
covalent
(COFs).
Here,
we
report
the
synthesis
of
a
crystalline
stable
hierarchical
porous
π-COF
(polyphthalocyanine,
HPPc)
demonstrate
its
potential
as
an
ideal
electrosynthesis
platform.
The
as-synthesized
HPPc
possesses
high
surface
area
(∼324
m2
g-1),
plentiful
inherent
micropores
(1.4
nm),
along
with
hard-template-induced,
uniform,
interconnected
mesopores
(35
nm).
This
dual-porosity
design
can
lead
improved
active
site
dispersion
mass
diffusion.
Moreover,
long-range
ordering
brought
by
crystallinity
enables
precise
customization
sites
needed.
Anchored
nickel
cobalt
atoms,
optimized
catalyst
exhibits
outstanding
oxygen
evolution
reaction
performance,
including
competitive
overpotential
305
mV
at
10
mA
cm-2
low
Tafel
slope
40
dec-1,
significantly
surpassing
commercial
RuO2.
work
opens
new
avenue
for
rational
chemically
π-COFs
various
applications.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 2, 2025
Furthering
the
field
of
synthetic
organic
chemistry
from
discrete
molecules
regime
to
extended
structure
regime,
covalent
frameworks
(COFs)
represent
a
new
genre
crystalline
porous
materials
featuring
designability
with
molecular-level
precision,
well-defined
porosity,
and
exceptional
stability
imparted
by
robust
linkages
reticulating
molecules.
The
topology
COFs
is
principal
feature
that
regulates
their
functionality
usability
for
emerging
technologies.
Profound
comprehension
network
topologies
maneuvering
them
toward
targeted
applications
are
crucial
advancing
realm
COF
research
developing
novel
functional
exciting
breakthroughs.
In
this
Perspective,
we
discuss
recent
pursuits
contributing
discovery
highly
connected
nets
having
topologies,
assess
key
challenges
achieving
such
offer
insights
into
current
scenario
future
directions.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 12, 2025
Abstract
Adsorbed
natural
gas
(ANG)
storage
is
emerging
as
a
promising
alternative
to
traditional
compressed
and
liquefied
methods.
However,
its
onboard
application
restricted
by
low
volumetric
methane
capacity.
Flexible
porous
adsorbents
offer
potential
solution,
their
dense
structures
unique
gate‐opening
effects
are
well‐suited
enhance
capacity
under
high
pressures.
This
study
developes
series
of
hyper‐cross‐linked
polymers
(HCPs)
with
tunable
flexibility
modifying
the
aliphatic
chain
length
in
double‐benzene‐ring
building
blocks,
employing
cost‐effective
external
crosslinking
approach.
The
resulting
flexible
polymer,
HCP‐DPP,
exhibits
pore
expansion
specific
pressures,
producing
high‐pressure
adsorption
isotherm
behavior.
Combined
intrinsic
skeleton,
this
feature
leads
superior
performance
over
rigid
counterparts.
Notably,
HCP‐DPP
achieves
record‐high
total
uptake
333
cm
3
STP
−3
working
291
at
273
K
100
bar,
exceeding
U.S.
Department
Energy
(DOE)
target
263
.
These
findings
lay
foundation
for
developing
advanced
practical
ANG
applications.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 30, 2024
Dynamic
3D
covalent
organic
frameworks
(COFs)
have
shown
a
concerted
structural
transformation
upon
adaptive
guest
inclusion.
However,
the
origin
of
conformational
mobility
and
host–guest
adaptivity
remain
conjecture
pedal
motions
revolving
imine
linkages,
often
without
considering
steric
hindrance
from
interwoven
frameworks.
Here,
we
present
atomic-level
observation
rotational
translational
dynamics
in
single-crystal
COF-300
inclusion
various
molecules,
featuring
multiple
rotamers
linkages
switchable
interframework
noncovalent
interactions.
Specifically,
developed
diffusion
gradient
transimination
protocol
to
facilitate
growth
COF
single
crystals,
enabling
high-resolution
X-ray
diffraction
analysis.
We
uncovered
metastable
low-symmetry
intermediate
phases
contracted
expanded
during
evolution.
identified
torsion
angles
terephthalaldehyde
diimine
motifs
that
switch
anti-periplanar
syn-periplanar/anticlinal
conformations.
Moreover,
linkage
were
concurrent
with
tetraphenylmethane
units,
which
tend
form
quadruple
phenyl
embrace.
Such
allows
adapt
such
as
alcohols,
esters,
phenols,
diols,
double
linear,
herringbone,
zigzag
chains,
triple
helix,
tubular
alignments.
Quantitative
energy
analyses
revealed
dynamic
structure
transformations
are
not
arbitrary
but
follow
specific
pathways
resemble
protein
folding.
The
work
is
paving
way
developing
robust,
dynamic,
crystalline
molecular
sponges
for
studying
condensed
liquids
need
further
crystallization.
Abstract
The
catalytic
conversion
of
CO
2
into
valuable
chemicals
using
metalized
covalent
organic
frameworks
(COFs)
as
catalysts
is
a
promising
method
for
reducing
atmospheric
levels.
Herein,
aldehyde‐amine
COF
(TAPT‐Tp)
at
room
temperature
and
pressure
their
metallized
results
synthesized,
Ni‐TAPT‐Tp
Ti‐TAPT‐Tp.
photocatalytic
indicate
that
the
to
reduction
rate
6182.5
µmol
g
−1
h
Ni‐TAPT‐Tp,
but
only
1615.4
Density
functional
theory
(DFT)
simulations
further
demonstrate
intermediates
*
,
COOH,
CO,
energy
consistently
lower
than
Ti‐TAPT‐Tp,
indicating
exhibits
superior
performance
RR.
This
work
provides
reference
optimizing
coordination
structure
M‐COFs
obtain
highly
active
selective
Catalysts,
Год журнала:
2025,
Номер
15(3), С. 237 - 237
Опубликована: Март 1, 2025
In
recent
years,
the
electrochemical
conversion
of
CO2
gasses
into
renewable
fuels
(e.g.,
ethylene,
ethanol,
and
propanol)
has
attracted
much
attention.
this
process,
electrocatalysts
play
a
crucial
role
in
accelerating
reduction
reaction
(CO2RR)
process.
review,
synthesis
C2+
products
from
was
investigated.
To
end,
various
classifications
such
as
metals,
metal
oxides,
alloys,
covalent
organic
frameworks
(COFs),
carbon-based
electrocatalysts,
metal–organic
(MOFs)
their
utilization
chemicals
were
fully
Also,
impact
factors
catalyst
stability,
temperature,
membrane
type,
pressure,
current
density,
pH,
type
electrolyte
on
CO2RR
process
to
generate
valuable
Moreover,
mechanism
for
producing
Furthermore,
limitations
future
perspective
surveyed.
Finally,
industrial
application
value-added
Based
our
investigation,
Cu
Cu2O-based
are
suitable
catalysts
products,
particularly
ethylene
ethanol.
Abstract
Cucurbit[
n
]urils
(abbreviated
as
Q[
]s
or
CB[
]s)
are
synthesized
through
the
condensation
of
formaldehyde
and
glycoluril
in
a
hydrochloric
acid
environment.
These
molecules
exhibit
three
distinctive
properties
concerning
their
charge
distribution:
neutral
internal
cavity,
positively
charged
outer
surface,
negatively
portal
carbonyl
oxygen
atoms.
unique
characteristics
facilitate
formation
supramolecular
frameworks
with
range
anions
metal
polyanions.
The
primary
focus
this
review
is
on
creation
anion‐induced
]‐based
self‐assemblies
exploring
potential
applications
ion
sequestration
release,
gas
adsorption,
well
development
fluorescence
probes.
Additionally,
concise
current
research
compounds
provided,
aiming
to
stimulate
future
advancements
field
innovative
framework
materials.
