Polymer
gels,
renowned
for
unparalleled
chemical
stability
and
self-sustaining
properties,
have
garnered
significant
attention
in
electrocatalysis.
Notably,
organic
polymer
gels
that
exhibit
temperature
sensitivity
incorporate
suitable
polar
nonvolatile
liquids,
enhance
electronic
conductivity,
impart
distinct
morphological
features,
but
remain
largely
unexplored
as
electrocatalysts
oxygen
reduction
reaction
(ORR).
To
address
this
issue,
an
innovative
strategy
is
proposed
synergistic
modulation
of
the
rigidity
mainchain
molecular
skeleton
length
alkyl
sidechains,
enabling
development
organogel
polymers
with
a
sol-gel
temperature-sensitive
phase
transition
promises
high
selectivity
enhanced
activity
electrocatalytic
processes.
shortening
sidechain
can
significantly
affect
gelation
behavior
internal
microstructure
catalyst,
which
modifies
electron
state,
ultimately
impacting
catalytic
gel
catalysts.
In
particular,
phenyl-containing
Ph-FL1
short
sidechains
demonstrates
outstanding
2e
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Окт. 25, 2024
Supramolecular
polymers
possess
great
potential
in
catalysis
owing
to
their
distinctive
molecular
recognition
and
dynamic
crosslinking
features.
However,
investigating
supramolecular
electrocatalysts
with
high
efficiency
oxygen
reduction
reaction
hydrogen
peroxide
(ORHP)
remains
an
unexplored
frontier.
Herein,
we
present
organic
for
ORHP
by
introducing
cyclodextrin-containing
noncovalent
building
blocks,
affording
these
supramolecules
abundant
bonds.
The
electronic
states
kinetics
are
further
well-modulated
via
a
host-guest
strategy,
resulting
appropriate
regional
electron
binding
force
controllable
chemical
activity.
Notably,
integrating
units
into
phenyl
group-containing
model
covalent
polymer
achieves
production
rate
of
9.14
mol
g
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 19, 2025
Abstract
Embedding
isomer
entities
onto
crystalline
frameworks
with
precisely
defined
spatial
distributions
represents
a
promising
approach
to
enhancing
the
efficiency
of
oxygen
reduction
reaction
(ORR)
in
fuel
cells.
However,
accurately
constructing
covalent
organic
(COFs)
regulate
energy
state
effectively
remains
significant
challenge.
Herein,
an
innovative
geometric
isomerization
strategy
aimed
at
minimizing
rotational
barrier
(ΔE),
average
local
ionization
(ALIE),
and
Gibbs
free
(ΔG)
for
ORR
within
COFs
is
proposed.
Based
on
this
strategy,
isomeric
Py‐COF‐αα
2,2‐substitution,
Py‐COF‐ββ
3,3‐substitution,
Py‐COF‐αβ
2,3‐substitution
mainchain
have
been
obtained.
The
electronic
states
intermediate
adsorption
capabilities
are
finely
tuned
through
modification,
yielding
controllable
chemical
activity.
Notably,
lower
ΔE
between
thiophenes
achieves
remarkable
performance,
evidenced
by
half‐wave
potential
0.77
V
vs
reversible
hydrogen
electrode
(RHE),
surpassing
most
reported
metal‐free
electrocatalysts.
Combined
theoretical
prediction
situ
Raman
spectra,
it
revealed
that
increased
dipole
moment
non‐uniform
charge
distribution
caused
endows
pentacyclic‐carbon
(thiophene
β‐position)
far
from
sulfur
atoms
efficient
catalytic
This
work
has
opened
up
novel
paradigm
underscores
pivotal
role
regulation
facilitating
catalysis.
iScience,
Год журнала:
2025,
Номер
28(3), С. 112007 - 112007
Опубликована: Фев. 12, 2025
Optimizing
molecular
structures
in
oxygen
reduction
reaction
(ORR)
is
crucial
for
enhancing
catalytic
efficiency
and
stability,
particularly
with
respect
to
the
effective
adsorption
conversion
of
intermediates.
Sulfur-containing
heterocyclic
compound
thiophene
can
precisely
modulate
electronic
states
local
charge
densities,
thereby
fine-tuning
reactivity
microporous
polymers,
yet,
it
remains
a
largely
unexplored
area.
Herein,
thiophene-based
building
blocks
featuring
diversified
linkers
into
phenyl-containing
model
Ph-CMP
are
developed,
affording
thiophene-fused
BPT-CMP
thiophene-linked
BCT-CMP.
The
electron
density
capacity
frameworks
well
regulated
through
condensation
connecting
modification,
showing
excellent
half-wave
potentials
compared
reversible
hydrogen
electrode,
surpassing
even
most
metal-free
polymer
electrocatalysts.
Through
theoretical
calculations
experimental
results,
we
have
validated
that
skeleton
(BPT-CMP)
triggers
activation
units,
exposed
pentatomic
carbon
atom
(site-3)
serving
as
active
site.
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.
Research Square (Research Square),
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 20, 2025
Abstract
Covalent
organic
frameworks
(COFs)
are
an
emerging
class
of
porous
materials
with
diverse
applications
across
multiple
fields.
Most
the
ongoing
research
related
to
COFs
predominantly
focuses
on
developing
new
through
novel
linkers
and
innovative
reactions,
as
well
exploring
their
applications.
A
detailed
molecular-level
understanding
COF
synthesis
is
essential
for
advanced
materials.
The
water
structure
adjacent
can
significantly
influence
design
highly
efficient
heterogeneous
catalysis,
photocatalytic
splitting,
purification,
aid
in
charge
storage
mechanism
COF-based
electrodes
at
electrode/electrolyte
interfaces.
To
address
this
issue,
we
synthesized
a
2D
thin
film
via
photon-assisted
imine
condensation
water-air
interface
investigated
process
using
vibrational
sum
frequency
generation
(VSFG)
spectroscopy.
We
examined
role
catalyst,
light,
interfacial
molecules
COF.
VSFG
spectroscopy
utilized
successfully
distinguish
between
amorphous
crystalline
films
surface.
Moreover,
it
was
found
that
exhibits
increased
ordering
stronger
hydrogen
bonding
proximity
ACS Applied Materials & Interfaces,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 26, 2025
The
meticulous
control
of
micromorphology
in
high
power
conversion
efficiency
(PCE)
polymer
solar
cells
(PSCs)
typically
relies
on
halogenated
solvents,
which
pose
serious
threats
to
both
environmental
sustainability
and
human
health.
In
this
work,
a
green
efficient
method
for
fabricating
PCE
PSCs
with
halogen-free
solvents
is
developed.
By
introducing
volatile
solid
additives
1-bromo-2,6-dichlorobenzene
(DIB)
1-bromo-2,3,5-trichlorobenzene
(TIB)
into
toluene
the
aggregation
behaviors
PM6:L8-BO
were
meticulously
regulated,
forming
distinct
fibrous
morphology;
detail,
vertical
direction
exhibited
pattern
acceptor
enrichment
at
top
donor
bottom,
leads
enhanced
exciton
dissociation
efficiency,
improved
charge
transport
performance,
significantly
reducing
recombination,
finally
PCEs,
as
maximum
PCEs
18.56
17.67%,
respectively,
are
notably
higher
than
those
devices
without
additives.
Furthermore,
since
can
be
completely
removed
from
active
layer,
additive-treated
exhibit
superior
morphology
photovoltaic
stability.
This
therefore,
unveils
straightforward
environmentally
friendly
preparing
PSCs,
instrumental
facilitating
large-scale
commercialization
PSC
technology.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 18, 2025
Abstract
The
design
of
bifunctional
and
high‐performance
electrocatalysts
that
can
be
used
as
both
cathodes
anodes
for
the
two‐electron
oxygen
reduction
reaction
(2e
−
ORR)
biomass
valorization
is
attracting
increasing
attention.
Herein,
a
conserved
ligand
replacement
strategy
developed
synthesis
highly
ordered
conductive
metal‐organic
frameworks
(Ni‐HITP,
HITP
=
2,
3,
6,
7,
10,
11‐hexaiminotriphenylene)
with
chemically
confined
phosphotungstic
acid
(PW
12
)
nanoclusters
in
nanopores.
newly
formed
Ni−O−W
bonds
resultant
Ni‐HITP/PW
modulate
electronic
structures
Ni
W
sites,
which
are
favorable
cathodic
2e
ORR
to
H
2
O
production
anodic
5‐hydroxymethylfurfural
oxidation
(HMFOR)
5‐furandicarboxylic
(FDCA),
respectively.
In
combination
deliberately
retained
pores,
dual‐functional
composites
enable
rate
9.51
mol
g
cat
−1
h
an
FDCA
yield
96.8%
at
current
density
100
mA
cm
−2
/cell
voltage
1.38
V
integrated
ORR/HMFOR
system,
significantly
improved
than
traditional
ORR/oxygen
evolution
system.
This
work
has
provided
new
insights
into
rational
advanced
electrocatalytic
systems
green
valuable
chemicals.
Catalysts,
Год журнала:
2025,
Номер
15(5), С. 500 - 500
Опубликована: Май 21, 2025
Hydrogen
peroxide
(H2O2)
is
a
versatile
and
environmentally
friendly
oxidant
with
broad
applications
in
industry,
energy,
environmental
remediation.
Electrocatalytic
H2O2
production
via
the
two-electron
oxygen
reduction
reaction
(2e−
ORR)
has
emerged
as
sustainable
alternative
to
traditional
anthraquinone
processes.
Covalent
organic
frameworks
(COFs),
class
of
crystalline
porous
materials,
exhibit
high
structural
tunability,
large
surface
areas,
chemical
stability,
making
them
promising
electrocatalysts
for
2e−
ORR.
This
review
systematically
summarizes
recent
advances
COF-based
production,
including
both
metal-free
metal-containing
systems.
We
discuss
key
strategies
COF
design—such
dimensional
modulation,
linkage
engineering,
heteroatom
doping,
post-synthetic
modification—and
highlight
their
effects
on
activity,
selectivity,
stability.
Fundamental
insights
into
ORR
mechanism
evaluation
metrics
are
also
provided.
Finally,
we
offer
perspectives
current
challenges
future
directions,
emphasizing
integration
machine
learning,
conductivity
enhancement,
scalable
synthesis
advance
COFs
toward
practical
electrosynthesis.
