Advanced Energy Materials,
Год журнала:
2024,
Номер
14(27)
Опубликована: Май 11, 2024
Abstract
The
oxygen
evolution
reaction
(OER)
is
central
to
energy
conversion
technologies,
but
the
high
cost
and
scarcity
of
commercial
noble
metal
catalysts
limit
their
widespread
application.
Natural
products
exhibit
great
potential
in
preparing
high‐performance
electrocatalysts
due
cost‐effectiveness
sustainability.
Here,
a
kind
1D
polymers
[M‐EA
(M═Co,
Cu,
Ni)]
for
via
complexation
ellagic
acid
(EA)
with
ions
are
reported.
It
found
that
Ni‐EA
displays
low
overpotential
(190
mV
at
10
mA
cm
−2
)
an
ultralow
Tafel
slope
(28
dec
−1
),
production
only
3.6
×
%
IrO
2
.
Density
functional
theory
investigations
reveal
electrocatalytic
mechanism
OER.
A
rechargeable
Zn‐Air
battery
using
Ni‐EA+Pt/C
as
air
electrode
shows
lower
charging
better
cycling
stability
than
+Pt/C‐based
battery.
This
work
provides
train
development
state‐of‐the‐art
OER
catalysts.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(5)
Опубликована: Дек. 1, 2022
Imine-linked
covalent
organic
frameworks
(COFs)
have
been
extensively
studied
in
photocatalysis
because
of
their
easy
synthesis
and
excellent
crystallinity.
The
effect
imine-bond
orientation
on
the
photocatalytic
properties
COFs,
however,
is
still
rarely
studied.
Herein,
we
report
two
novel
COFs
with
different
orientations
imine
bonds
using
oligo(phenylenevinylene)
moieties.
showed
similar
structures
but
great
differences
photoelectric
properties.
COF-932
demonstrated
a
superior
hydrogen
evolution
performance
compared
to
COF-923
when
triethanolamine
was
used
as
sacrificial
agent.
Interestingly,
use
ascorbic
acid
led
protonation
further
altering
direction
electron
transfer.
performances
were
increased
23.4
0.73
mmol
g-1
h-1
for
protonated
COF-932,
respectively.
This
study
provides
clear
strategy
design
imine-linked
COF-based
photocatalysts
advances
development
COFs.
RSC Advances,
Год журнала:
2024,
Номер
14(29), С. 20609 - 20645
Опубликована: Янв. 1, 2024
The
photocatalytic
field
revolves
around
the
utilization
of
photon
energy
to
initiate
various
chemical
reactions
using
non-adsorbing
substrates,
through
processes
such
as
single
electron
transfer,
or
atom
transfer.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(39), С. 21483 - 21490
Опубликована: Сен. 22, 2023
One-step
adsorptive
purification
of
ethylene
(C2H4)
from
a
ternary
mixture
acetylene
(C2H2),
C2H4,
and
ethane
(C2H6)
by
single
material
is
great
importance
but
challenging
in
the
petrochemical
industry.
Herein,
chemically
robust
olefin-linked
covalent
organic
framework
(COF),
NKCOF-62,
designed
synthesized
melt
polymerization
method
employing
tetramethylpyrazine
terephthalaldehyde
as
cheap
monomers.
This
avoids
most
disadvantages
classical
solvothermal
methods,
which
enable
cost-effective
kilogram
fabrication
COFs
one
pot.
Furthermore,
NKCOF-62
shows
remarkably
selective
adsorption
C2H2
C2H6
over
C2H4
thanks
to
its
unique
pore
environments
suitable
size.
Breakthrough
experiments
demonstrate
that
polymer-grade
can
be
directly
obtained
C2H2/C2H6/C2H4
(1/1/1)
mixtures
through
separation
process.
Notably,
first
demonstration
potential
use
for
separation,
provides
blueprint
design
construction
industrial
gas
separations.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(20), С. 11276 - 11281
Опубликована: Май 11, 2023
Dimensional
isomers,
defined
in
reticular
chemistry
as
frameworks
consisting
of
identical
molecular
building
blocks
but
extended
two
or
three
dimensions
(2D
3D),
are
an
important
type
framework
isomers
that
have
never
been
isolated.
Herein,
we
report
the
crystallization
dimensional
covalent
organic
(COFs)
for
first
time.
By
polymerization
same
at
different
temperatures,
both
2D
and
3D
COFs
were
successfully
constructed
due
to
temperature-induced
conformational
changes
precursors
from
planar
tetrahedral.
In
addition,
non-fluorescent
COF
can
be
gradually
converted
into
fluorescent
by
increasing
temperature
under
solvothermal
conditions.
Therefore,
it
is
reasonable
crystallize
materials
controlling
conformation
blocks,
more
examples
expected.
Since
obtained
show
properties
functions,
this
work
will
definitely
motivate
us
design
target
applications
future.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Март 10, 2024
Abstract
Covalent
organic
frameworks
(COFs)
attract
significant
attention
due
to
their
ordered,
crystalline,
porous,
metal‐free,
and
predictable
structures.
These
unique
characteristics
offer
great
opportunities
for
the
diffusion
transmission
of
photogenerated
charges
during
photocatalysis.
Currently,
a
considerable
number
COFs
are
used
as
metal‐free
semiconductor
photocatalysts.
This
review
aims
understand
relationships
between
structure
photocatalysis
performance
provides
in‐depth
insight
into
synthetic
strategy
improve
performance.
Subsequently,
focuses
on
structural
motif
in
sustainable
photocatalytic
hydrogen
evolution,
carbon
dioxide
reduction,
peroxide
generation,
compound
transformations.
Last,
conjunction
with
progress
achieved
challenges
yet
be
overcome,
candid
discussion
is
undertaken
regarding
field
COF
photocatalysis,
accompanied
by
presentation
potential
research
avenues
future
directions.
seeks
provide
readers
comprehensive
understanding
pivotal
role
robust
guidance
innovative
utilization
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(26)
Опубликована: Май 2, 2023
The
chemical
microenvironment
modulation
of
metal
nanoparticles
(NPs)
holds
promise
for
tackling
the
long-lasting
challenge
trade-off
effect
between
activity
and
selectivity
in
catalysis.
Herein,
ultrafine
PdCu2
NPs
incorporated
into
covalent
organic
frameworks
(COFs)
with
diverse
groups
on
their
pore
walls
have
been
fabricated
semihydrogenation
alkynes.
Cu
species,
as
primary
Pd
active
sites,
greatly
improves
selectivity.
functional
secondary
around
effectively
regulate
activity,
which
encapsulated
COF
bearing
-CH3
exhibit
highest
>99
%
conversion
97
Both
experimental
calculation
results
suggest
that
group
affects
electron-donating
ability
COFs,
successively
impacts
charge
transfer
COFs
giving
rise
to
a
modulated
electronic
state
excellent
catalytic
performance.
Controllable
modulation
of
the
stacking
modes
2D
(two-dimensional)
materials
can
significantly
influence
their
properties
and
functionalities
but
remains
a
formidable
synthetic
challenge.
Here,
an
effective
strategy
is
proposed
to
control
layer
imide-linked
covalent
organic
frameworks
(COFs)
by
altering
methods.
Specifically,
modulator-assisted
method
afford
COF
with
rare
ABC
without
need
for
any
additives,
while
solvothermal
synthesis
leads
AA
stacking.
The
variation
interlayer
influences
chemical
physical
properties,
including
morphology,
porosity,
gas
adsorption
performance.
resultant
shows
much
higher
C2
H2
capacity
selectivity
over
CO2
H4
than
stacking,
which
not
demonstrated
in
field
yet.
Furthermore,
outstanding
practical
separation
ability
confirmed
breakthrough
experiments
/CO2
(50/50,
v/v)
/C2
(1/99,
v/v),
selectively
remove
good
recyclability.
This
work
provides
new
direction
produce
COFs
controllable
modes.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(23), С. 16229 - 16236
Опубликована: Май 30, 2024
Employing
covalent
organic
frameworks
(COFs)
for
the
photocatalytic
CO2
reduction
reaction
(CDRR)
to
generate
high-value
chemical
fuels
and
mitigate
greenhouse
gas
emissions
represents
a
sustainable
catalytic
conversion
approach.
However,
achieving
superior
CDRR
performance
is
hindered
by
challenges
of
low
charge
separation
efficiency,
poor
stability,
high
preparation
costs
associated
with
COFs.
Herein,
in
this
work,
we
utilized
perfluorinated
metallophthalocyanine
(MPcF16)
biomolecule
compound
ellagic
acid
(EA)
as
building
blocks
actualize
functional
named
EPM-COF
(M
=
Co,
Ni,
Cu).
The
designed
EPCo-COF,
featuring
cobalt
metal
active
sites,
demonstrated
an
impressive
CO
production
rate
selectivity
(CDRR).
Moreover,
following
alkaline
treatment
(EPCo-COF-AT),
COF
exposed
carboxylic
anion
(COO–)
hydroxyl
group
(OH),
thereby
enhancing
electron-donating
capability
EA.
This
modification
achieved
heightened
17.7
mmol
g–1
h–1
outstanding
97.8%
efficient
CDRR.
Theoretical
calculations
further
illustrated
that
EPCo-COF-AT
functionalized
COO–
OH
can
effectively
alleviate
energy
barriers
involved
process,
which
facilitates
proton-coupled
electron
transfer
processes
enhances
on
sites
within
EPCo-COF-AT.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Янв. 27, 2024
Abstract
The
synthesis
of
three-dimensional
covalent
organic
frameworks
with
highly
connected
building
blocks
presents
a
significant
challenge.
In
this
study,
we
report
two
3D
COFs
the
nia
topology,
named
JUC-641
and
JUC-642,
by
introducing
planar
hexagonal
triangular
prism
nodes.
Notably,
our
adsorption
studies
breakthrough
experiments
reveal
that
both
exhibit
exceptional
separation
capabilities,
surpassing
previously
reported
most
porous
polymers,
factor
up
to
2.02
for
benzene
cyclohexane.
Additionally,
dispersion-corrected
density
functional
theory
analysis
suggests
good
performance
these
can
be
attributed
incorporation
aromatic
presence
extensive
pore
structures.
Consequently,
research
not
only
expands
diversity
but
also
highlights
potential
COF
materials
as
promising
candidates
environmentally-friendly
applications.