Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(18)
Published: March 7, 2024
Abstract
Constructing
stable
and
efficient
photocatalysts
for
H
2
O
production
is
of
great
importance
challenging.
In
this
study,
the
synthesis
three
photoactive
cyclooctatetrathiophene
(COTh)‐based
porous
aromatic
frameworks
(COTh‐PAFs)
in
an
alternating
donor‐acceptor
(D−A)
fashion
presented.
combination
with
a
triazine‐derived
electron
acceptor,
PAF‐363
exhibits
high
efficiency
photosynthesis
rates
11733
μmol
g
−1
h
(with
sacrificial
agent)
3930
(without
from
water
oxygen
under
visible
light
irradiation.
Experimental
results
theoretical
calculations
reveal
that
charge
transfer
positions
adsorption
sites
are
both
concentrated
on
COTh
fragments,
which
facilitate
through
reduction
reaction
(ORR)
pathway.
This
work
highlights
rational
design
COTh‐PAFs
consideration
D−A
direction,
positions,
provides
feasible
access
to
photocatalysts.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: March 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
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(7), P. 4822 - 4829
Published: Feb. 8, 2024
The
construction
of
function-oriented
covalent
organic
frameworks
(COFs)
remains
a
challenge
as
it
requires
simultaneous
consideration
diversified
structures,
robust
linkage,
and
tailorable
functionalities.
Herein,
we
report
the
rational
synthesis
functionalized
COFs
via
four-component
reaction
strategy.
Through
Debus–Radziszewski
reaction,
11
N-substituted
imidazole-based
with
structures
were
facilely
constructed
from
readily
available
building
blocks.
By
forming
imidazole
these
synthesized
displayed
ultrastability
toward
strong
acids
base.
Moreover,
four
components
allows
As
an
example,
phosphonate-functionalized
COF
(LZU-530)
was
rationally
for
efficient
adsorption
uranium(VI).
uranium(VI)
uptake
LZU-530
reaches
up
to
95
mg·g–1
in
2
M
HNO3,
which
is
highest
existing
porous
materials
under
such
harsh
conditions.
Our
results
highlight
use
multicomponent
targeted
applications.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(25)
Published: April 16, 2024
Covalent
organic
frameworks
(COFs)
have
recently
shown
great
potential
for
photocatalytic
hydrogen
production.
Currently
almost
all
reports
are
focused
on
two-dimensional
(2D)
COFs,
while
the
3D
counterparts
rarely
explored
due
to
their
non-conjugated
derived
from
sp
ACS Materials Letters,
Journal Year:
2024,
Volume and Issue:
6(5), P. 2007 - 2049
Published: April 17, 2024
Hydrogen
peroxide
(H2O2),
a
valuable
chemical,
is
widely
used
as
powerful
oxidizing
agent
in
chemical
synthesis,
pharmaceuticals,
medical
disinfection,
and
environmental
treatment
industries.
Currently,
over
95%
of
H2O2
produced
industrially
using
the
anthraquinone
process,
which
associated
with
its
high
energy
consumption
hazardous
byproducts.
Therefore,
photochemical
synthesis
from
water
oxygen
covalent
organic
framework
based
photocatalysts
have
attracted
considerable
attention.
This
review
aims
to
outline
recent
achievements,
challenges
future
prospects
COFs
heterogeneous
for
sustainable
generation.
We
summarize
chronological
development
COFs,
different
mechanisms
involved,
detailed
experiments
quantification
methods
photocatalytic
The
puts
forward
an
outlook,
highlighting
advantages
limitations
anticipate
that
this
will
provide
insight
into
current
progress
inspire
next-generation
production.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(15)
Published: Feb. 9, 2024
Developing
high
connectivity
(>8)
three-dimensional
(3D)
covalent
organic
frameworks
(COFs)
towards
new
topologies
and
functions
remains
a
great
challenge
owing
to
the
difficulty
in
getting
building
blocks.
This
however
represents
most
important
step
promoting
diversity
of
COFs
due
still
limited
dynamic
bonds
available
for
constructing
at
this
stage.
Herein,
highly
connected
phthalocyanine-based
(Pc-based)
3D
MPc-THHI-COFs
(M=H
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(37)
Published: June 25, 2024
Abstract
The
electrochemical
production
of
hydrogen
peroxide
(H
2
O
)
using
metal‐free
catalysts
has
emerged
as
a
viable
and
sustainable
alternative
to
the
conventional
anthraquinone
process.
However,
precise
architectural
design
these
electrocatalysts
poses
significant
challenge,
requiring
intricate
structural
engineering
optimize
electron
transfer
during
oxygen
reduction
reaction
(ORR).
Herein,
we
introduce
novel
covalent
organic
frameworks
(COFs)
that
effectively
shift
ORR
from
four‐electron
more
advantageous
two‐electron
pathway.
Notably,
JUC‐660
COF,
with
strategically
charge‐modified
benzyl
moieties,
achieved
continuous
high
H
yield
over
1200
mmol
g
−1
h
for
an
impressive
duration
85
hours
in
flow
cell
setting,
marking
it
one
most
efficient
non‐pyrolyzed
reported
date.
Theoretical
computations
alongside
situ
infrared
spectroscopy
indicate
markedly
diminishes
adsorption
OOH*
intermediate,
thereby
steering
towards
desired
Furthermore,
versatility
was
demonstrated
through
its
application
electro‐Fenton
reaction,
where
efficiently
rapidly
removed
aqueous
contaminants.
This
work
delineates
pioneering
approach
altering
pathway,
ultimately
paving
way
development
highly
effective
electrocatalysts.
ACS Materials Letters,
Journal Year:
2024,
Volume and Issue:
6(6), P. 2276 - 2294
Published: May 10, 2024
Solar-driven
water
splitting
into
hydrogen
and
oxygen
fuels
represents
a
promising
way
for
clean
energy
production
to
achieve
carbon-neutral
future.
The
efficiency
of
photocatalytic
strongly
relies
on
the
development
high-performance
catalysts.
Noteworthily,
covalent
organic
frameworks
(COFs)
offer
distinctive
platform
designing
photo-to-chemical
conversion,
benefiting
from
their
tailorable
structure,
ultrahigh
porosity,
robust
framework,
sufficient
light
absorption,
rich
active
sites.
Herein
we
highlight
systematic
overview
recent
research
progress
using
COFs
half-reactions
overall
splitting.
With
an
aim
shed
understanding
structural
design
COF
photocatalysts
splitting,
various
functional
strategies
are
discussed.
Finally,
major
challenges
future
perspectives
proposed
with
hope
achieving
ongoing
this
emerging
field.
