Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 23, 2024
Abstract
Kinetic
factors
frequently
emerge
as
the
primary
constraints
in
photocatalysis,
exerting
a
critical
influence
on
efficacy
of
polymeric
photocatalysts.
The
diverse
conjugation
systems
within
covalent
organic
frameworks
(COFs)
can
significantly
impact
photon
absorption,
energy
level
structures,
charge
separation
and
migration
kinetics.
Consequently,
these
limitations
often
manifest
unsatisfactory
kinetic
behavior,
which
adversely
affects
photocatalytic
activity
COFs.
To
address
challenges,
we
propose
methoxy
(−OMe)
molecular
engineering
strategy
designed
to
enhance
carrier
kinetics
mitigate
mass
transfer
resistance.
Through
strategic
modulation
position
quantity
−OMe
units,
effectively
manipulate
p‐π
conjugation,
thereby
enhancing
migration.
Moreover,
COFs
enriched
with
moieties
exhibit
enhanced
dynamics
due
hydrophilic
nature
groups,
facilitate
diffusion
reactants
products
porous
structure.
This
approach
is
hypothesized
drive
an
efficient
hydrogen
evolution
reaction.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(40)
Published: July 18, 2024
Abstract
The
integration
of
electron
donor
(D)
and
acceptor
(A)
units
into
covalent
organic
frameworks
(COFs)
has
received
increasing
interest
due
to
its
potential
for
efficient
photocatalytic
hydrogen
(H
2
)
evolution
from
water.
Nevertheless,
the
advancement
D–A
COFs
is
still
constrained
by
limited
investigations
on
engineering,
which
enables
highly
effective
charge
transfer
pathways
in
deliver
photoexcited
electrons
a
preferential
orientation
enhance
performance.
Herein,
two
systems
with
D–A–A
configurations
based
molecular
engineering
strategy
are
proposed
construct
three
distinct
COFs.
Specifically,
TAPPy‐DBTDP‐COF
merging
one
pyrene‐based
benzothiadiazole
acceptors
realized
an
average
H
rate
12.7
mmol
h
−1
g
under
visible
light,
among
highest
ever
reported
typical
D–A‐type
COF
systems.
combination
experimental
theoretical
analysis
signifies
crucial
role
dual‐acceptor
arrangement
promoting
exciton
dissociation
carrier
migration.
These
findings
underscore
significant
structural
design,
conducive
separation
holes
resulting
superior
activities.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(29)
Published: May 6, 2024
Abstract
Despite
the
pivotal
role
of
molecular
oxygen
(O
2
)
activation
in
artificial
photosynthesis,
efficiency
is
often
restricted
by
sluggish
exciton
dissociation
and
charge
transfer
kinetics
within
polymer
photocatalysts.
Herein,
we
propose
two
tetrathiafulvalene
(TTF)‐based
imine‐linked
covalent
organic
frameworks
(COFs)
with
tailored
donor‐acceptor
(D–A)
structures,
TTF‐PDI‐COF
TTF‐TFPP‐COF,
to
promote
O
activation.
Because
enhanced
electron
push‐pull
interactions
that
facilitated
separation
behavior,
exhibited
superior
photocatalytic
activity
electron‐induced
reactions
over
TTF‐TFPP‐COF
under
visible
light
irradiation,
including
photosynthesis
(
E
)‐3‐amino‐2‐thiocyano‐
α
,
β
‐unsaturated
compounds
H
.
These
findings
highlight
significant
potential
rational
design
COFs
D–A
configurations
as
suitable
candidates
for
advanced
applications.
Inorganic Chemistry Frontiers,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 1, 2025
Three
water-soluble
organic–inorganic
hybridized
POMs-based
memristor
are
proposed.
The
introduction
of
organic
ligands
improves
its
performance.
mechanism
the
device
during
high
temperature
operation
was
explored
using
2D-COS-IR.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 18, 2025
Abstract
As
the
largest
sensory
organ,
human
skin
generates
ionic
signals
in
response
to
tactile,
thermal,
and
electrical
stimuli,
which
are
then
transmitted
neurons
processed
by
brain,
thereby
enabling
sensing
memory,
ultimately
promoting
conscious
perception
decision‐making.
However,
existing
artificial
skins
face
significant
challenges
including
inability
achieve
multimodal
memory
simultaneously
(i.e.,
stimuli),
difficulty
detecting
ultra‐low
currents,
limitations
rich
synaptic
behaviors
that
essential
for
highly
efficient
in‐sensor
reservoir
computing.
Inspired
electric
eels,
study
here
develops
an
based
on
iontronic
p‐n
junctions
consisting
of
PolyAT
PolyES
bi‐layered
structures.
This
features
broad
detection
ranges
temperature
(−80
120
°C,
well
beyond
reach
hydrogel
counterparties),
pressure
(0.075
Pa
400
kPa,
among
highest
sensitivities
ever
reported),
current
(1–200
nA),
meanwhile
demonstrates
functions.
Additionally,
incorporating
a
robotic
hand
can
grasp
objects
with
different
temperatures
weights
demand.
Further,
fully
memristive
computing
is
implemented
skin,
allowing
sensing,
decoding,
learning
via
stimulation,
achieving
91.3%
accuracy
classifying
MNIST
handwritten
digit
images.
Nano Letters,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 25, 2025
The
rapid
evolution
of
neuromorphic
devices
seeks
to
bridge
biological
neural
networks
and
artificial
systems,
enabling
energy-efficient
scalable
computing
for
next-generation
intelligence.
Herein,
we
introduce
methyl-engineered
one-dimensional
covalent
organic
framework
(1D
COF)-based
memristors
as
a
transformative
platform
reconfigurable
computing.
incorporation
methyl
groups
enhances
localized
polarization
effects
within
the
COF
framework,
effectively
mitigating
random
Ag+
migration/diffusion
stabilizing
conductive
filament
morphology.
This
strategic
modification
yields
with
exceptional
multilevel
storage
capabilities,
exhibiting
superior
stability,
linearity,
reproducibility.
Moreover,
highly
ordered
architecture
customizable
chemical
environment
methyl-functionalized
1D
allows
precise
control
over
resistive
switching
behaviors,
facilitating
emulation
synaptic
functions
development
network
architectures.
Demonstrating
performance
in
tasks
such
high-accuracy
image
recognition,
these
showcase
significant
promise
foundation
energy-efficient,
systems.
Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(29)
Published: May 6, 2024
Abstract
Despite
the
pivotal
role
of
molecular
oxygen
(O
2
)
activation
in
artificial
photosynthesis,
efficiency
is
often
restricted
by
sluggish
exciton
dissociation
and
charge
transfer
kinetics
within
polymer
photocatalysts.
Herein,
we
propose
two
tetrathiafulvalene
(TTF)‐based
imine‐linked
covalent
organic
frameworks
(COFs)
with
tailored
donor‐acceptor
(D–A)
structures,
TTF‐PDI‐COF
TTF‐TFPP‐COF,
to
promote
O
activation.
Because
enhanced
electron
push‐pull
interactions
that
facilitated
separation
behavior,
exhibited
superior
photocatalytic
activity
electron‐induced
reactions
over
TTF‐TFPP‐COF
under
visible
light
irradiation,
including
photosynthesis
(
E
)‐3‐amino‐2‐thiocyano‐
α
,
β
‐unsaturated
compounds
H
.
These
findings
highlight
significant
potential
rational
design
COFs
D–A
configurations
as
suitable
candidates
for
advanced
applications.