Chinese Journal of Chemistry,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 28, 2024
Comprehensive
Summary
The
construction
of
luminescent
two‐dimensional
(2D)
imine‐linked
covalent
organic
frameworks
(COFs)
is
a
formidable
challenge
due
to
the
strong
interlayer
stacking
and
bond
rotations
that
typically
suppress
intramolecular
charge
transfer
(ICT),
leading
nonradiative
energy
dissipation.
Herein,
three
COFs
with
tailored
distances
are
designed
modulate
ICT
behaviours.
targeted
COF
(TPAZ‐TPE‐COF)
achieved
significantly
enhanced
photoluminescence
quantum
yield
(PLQY)
21.22%
in
solid
state
by
restricting
rotation
enlarging
layer
distance.
This
represents
3.5‐fold
530.5‐fold
improvement
over
TPAZ‐PYTA‐COF
(6.15%),
which
has
shortened
space,
TPAZ‐PATA‐COF
(0.04%),
exhibits
rotations,
respectively.
Importantly,
TPAZ‐TPE‐COF
also
exceptional
sensing
performance
for
iron
ions,
detection
limit
at
ppb
level.
Both
experimental
theoretical
analyses
reveal
prominent
assigned
effective
suppression
pathways,
especially
those
arising
from
vibrations.
These
findings
pave
way
deliberate
2D
high
PL
intensity,
thereby
expanding
portfolio
potential
applications
optoelectronics.
Advanced Materials,
Год журнала:
2024,
Номер
36(33)
Опубликована: Июнь 25, 2024
Abstract
Double‐atom
catalysts
(DACs)
with
asymmetric
coordination
are
crucial
for
enhancing
the
benefits
of
electrochemical
carbon
dioxide
reduction
and
advancing
sustainable
development,
however,
rational
design
DACs
is
still
challenging.
Herein,
this
work
synthesizes
atomically
dispersed
novel
sulfur‐bridged
Cu‐S‐Ni
sites
(named
Cu‐S‐Ni/SNC),
utilizing
biomass
wool
keratin
as
precursor.
The
plentiful
disulfide
bonds
in
overcome
limitations
traditional
gas‐phase
S
ligand
etching
process
enable
one‐step
formation
S‐bridged
sites.
X‐ray
absorption
spectroscopy
(XAS)
confirms
existence
bimetallic
N
2
Cu‐S‐NiN
moiety.
In
H‐cell,
Cu‐S‐Ni/SNC
shows
high
CO
Faraday
efficiency
98.1%
at
−0.65
V
versus
RHE.
Benefiting
from
charge
tuning
effect
between
metal
site
bridged
sulfur
atoms,
a
large
current
density
550
mA
cm
−2
can
be
achieved
−1.00
flow
cell.
Additionally,
situ
XAS,
attenuated
total
reflection
surface‐enhanced
infrared
(ATR‐SEIRAS),
functional
theory
(DFT)
calculations
show
Cu
main
adsorption
dual‐regulated
by
Ni
which
enhances
activation
accelerates
*COOH
intermediates.
This
kind
atom
may
open
new
pathways
precision
preparation
performance
regulation
atomic
materials
toward
energy
applications.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 13, 2024
Abstract
Modulating
the
electronic
state
of
multicomponent
covalent
organic
framework
(COF)
electrocatalysts
is
crucial
for
enhancing
catalytic
activity.
However,
effect
dimensionality
on
their
physicochemical
functionalities
still
lacking.
Herein,
we
report
an
interlaced
unsaturated
2D
and
saturated
3D
strategy
to
develop
multicomponent‐regulated
COFs
with
tunable
gradient
high
selectivity
activity
electrocatalysis.
Compared
two‐component
model
COFs,
2D/3D
locally
irregular
dimensions
structures
are
more
practical
in
optimizing
intrinsic
electrode
surface
reaction
mass
transfer.
Remarkably,
2D‐inserted
TAE‐COF
regulates
adsorption
mode
OOH*
species
supply
a
favorable
dynamic
pathway
H
2
O
process,
thereby
achieving
excellent
production
rate
8.50
mol
g
cat
−1
h
.
Moreover,
utilizing
theoretical
calculation
situ
ATR‐FTIR
experiment,
found
that
central
carbon
atom
tetraphenyl‐based
unit
(site‐1
site‐6)
potential
active
sites.
This
operating
ability
reactants
dimensionality‐interconnected
building
blocks
provides
idea
designing
durable
efficient
electrocatalysts.
Angewandte Chemie International Edition,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 9, 2025
Photo/electro-catalytic
CO2
reduction
into
high-value
products
are
promising
strategies
for
addressing
both
environmental
problems
and
energy
crisis.
Duo
to
their
advantageous
visible
light
absorption
ability,
adjustable
optic/electronic
properties,
definite
active
center,
post-modification
capability,
excellent
stability,
porphyrin-based
covalent
organic
frameworks
(COFs)
have
emerged
as
attractive
photo/electro-catalysts
towards
reduction.
In
this
review,
the
research
progress
of
COFs
photo/electro-catalytic
is
summarized
including
design
principles,
catalytic
performance,
reaction
mechanism.
addition,
review
also
presents
some
challenges
prospects
application
in
reduction,
laying
base
fundamental
efforts.
Angewandte Chemie,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 9, 2025
Abstract
Photo/electro‐catalytic
CO
2
reduction
into
high‐value
products
are
promising
strategies
for
addressing
both
environmental
problems
and
energy
crisis.
Duo
to
their
advantageous
visible
light
absorption
ability,
adjustable
optic/electronic
properties,
definite
active
center,
post‐modification
capability,
excellent
stability,
porphyrin‐based
covalent
organic
frameworks
(COFs)
have
emerged
as
attractive
photo/electro‐catalysts
towards
reduction.
In
this
review,
the
research
progress
of
COFs
photo/electro‐catalytic
is
summarized
including
design
principles,
catalytic
performance,
reaction
mechanism.
addition,
review
also
presents
some
challenges
prospects
application
in
reduction,
laying
base
fundamental
efforts.
ACS Materials Letters,
Год журнала:
2024,
Номер
7(1), С. 220 - 228
Опубликована: Дек. 13, 2024
Developing
multifunctional
adsorbents
with
exceptional
capture
performance
and
outstanding
antibiofouling
activity
is
of
great
significance
for
the
recovery
gold.
However,
most
reported
materials
only
have
a
single
adsorption
function,
which
restricts
their
practical
application
gold
extraction
from
complex
matrices.
Herein,
we
construct
series
three-component
covalent
organic
frameworks
(COFs)
good
antibacterial
All
obtained
COFs
show
high
capacities
over
1250
mg·g–1
gold,
may
be
attributed
to
specific
surface
area,
regular
pore
structure
abundant
binding
sites.
In
particular,
optimized
COF-TPTD-DHTA-TAB
gives
excellent
capacity
(2884
mg·g–1),
ultrafast
kinetics
(60
min)
distribution
coefficient
(Kd
>
4
×
105
mL·g–1).
More
importantly,
sterilization
observed
on
both
COF-TPTD-DHTA
under
visible
light
irradiation.
This
work
provides
paradigm
develop
ionic
recovery.
Efficient
sacrificial-agent-free
photosynthesis
of
H2O2
from
air
and
water
represents
the
greenest,
lowest-cost,
most
real-time
avenue
for
production
but
remains
a
challenging
issue.
Here,
we
show
general
effective
approach
through
structural
design
on
covalent
organic
frameworks
(COFs)
with
asymmetric
dual-function
hybrid
linkages
boosting
COFs.
Through
such
can
equip
COF
not
only
catalytic
active
center
also
special
function
isolating
D–A
motif,
which
consequently
endows
(CI-COF)
built
significantly
enhanced
efficiency
in
generation,
transmission,
separation
photogenerated
carriers,
relative
to
(II-COF
CC-COF)
symmetric
single-function
single
linkages.
Correspondingly,
performance
is
by
three
or
five
times.
Accompanied
largely
promoted
O2
utilization
conversion
36.6%
99.9%.
A
rare
dual-channel
suggested
CI-COF.
