Journal of the American Chemical Society,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 28, 2024
Traditional
desalination
methods
face
criticism
due
to
high
energy
requirements
and
inadequate
trace
ion
removal,
whereas
natural
light-driven
pumps
offer
superior
efficiency.
Current
synthetic
systems
are
constrained
by
short
exciton
lifetimes,
which
limit
their
ability
generate
sufficient
electric
fields
for
effective
pumping.
We
introduce
an
innovative
approach
utilizing
covalent-organic
framework
membranes
that
enhance
light
absorption
reduce
charge
recombination
through
vertical
gradient
protonation
of
imine
linkages
during
acid-catalyzed
liquid-liquid
interfacial
polymerization.
This
technique
creates
intralayer
interlayer
heterojunctions,
facilitating
hybridization
establishing
a
robust
built-in
field
under
illumination.
These
improvements
enable
the
achieve
remarkable
transport
across
extreme
concentration
gradients
(2000:1),
with
rate
approximately
3.2
×
10
Macromolecular Rapid Communications,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 12, 2025
Abstract
Photocatalytic
production
of
hydrogen
peroxide
(H
2
O
)
represents
a
significant
approach
to
achieving
sustainable
energy
generation
through
solar
energy,
addressing
both
shortages
and
environmental
pollution.
Among
various
photocatalytic
materials,
covalent
organic
frameworks
(COFs)
have
gained
widespread
attention
in‐depth
research
due
their
unique
advantages,
including
high
porosity,
predesignability,
atomic‐level
tunability.
In
recent
years,
progress
has
been
made
in
the
development,
performance
enhancement,
mechanistic
understanding
COF‐based
photocatalysts.
This
review
focuses
on
latest
advancements
H
using
COFs,
particularly
emphasizing
rational
design
COF
structures
regulate
catalytic
exploring
fundamental
processes
involved
photocatalysis.
Based
current
achievements
this
field,
paper
also
discusses
existing
challenges
future
opportunities,
aiming
provide
reference
for
application
COFs
production.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 13, 2025
Abstract
Developing
conductor‐mediated
S‐scheme
heterojunction
photocatalysts
imitating
natural
photosynthetic
systems
emerges
as
a
promising
approach
to
hydrogen
peroxide
(H
2
O
)
production.
However,
achieving
precise
coupling
between
two
semiconductors
with
charge
shuttle
and
modulating
the
interfacial
interactions
still
remain
significant
bottleneck.
Herein,
we
propose
catalyst
architecture
Cd
single
atom
mediated
formed
by
interfacing
CdS
TiO
nanoparticles.
This
exhibits
an
H
production
rate
high
60.33
µmol
g
−1
min
under
UV–vis
light
irradiation,
which
is
attributed
efficient
transport
at
interface
of
thanks
S‐scheme.
In‐situ
X‐ray
photoelectron
spectroscopy
(XPS)
electron
spin
resonance
(ESR)
spin‐trapping
tests
confirm
transfer
route.
Femtosecond
transient
absorption
(fs‐TA)
other
ex‐situ
characterizations
further
corroborate
across
interface.
work
offers
new
perspective
on
constructing
atoms
heterojunctions
enhance
photocatalytic
performance.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 31, 2025
Abstract
The
water
oxidation
reaction
(WOR)
with
sluggish
kinetics
usually
fails
to
adequately
furnish
protons
oxygen
reduction
(ORR),
which
ultimately
constrains
the
overall
efficiency
of
photocatalytic
synthesis
H
2
O
,
particularly
in
absence
sacrificial
agents.
Herein,
a
class
hydroxyl
groups
(─OH)
functionalized
covalent
organic
framework
(COF)
is
reported
as
proton
reservoir
compensate
ORR
for
greatly
improving
photosynthesis.
It
has
been
demonstrated
that
incorporation
─OH
into
TFBP‐DHBD
(TFBP:
1,2,4,5‐tetrakis‐(4‐formylphenyl)benzene,
DHBD:
3,3′‐dihydroxybenzidine)
COF
can
achieve
3.3
times
higher
photosynthetic
activity
than
TFBP‐BD
(BD:
benzidine)
without
groups.
Isotope
labeling
experiments
and
situ
infrared
spectroscopy
analysis
demonstrate
donate
subsequently
regain
released
from
WOR.
Theoretical
calculations
further
confirm
provides
formation
*OOH
intermediate
reduces
its
energy
barrier,
thereby
facilitating
photosynthesis
.
A
novel
loaded
Al
3
spheres‐based
streamlined
microreactor
built
simultaneously
production
elimination
bacteria
over
1.3
×
10
4
CFU
mL
−1
superior
continuous
flow
reactors.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 27, 2024
Abstract
Photocatalysis
leverages
solar
energy
to
overcome
the
thermodynamic
barrier,
enabling
efficient
chemical
reactions
under
mild
conditions.
It
can
greatly
reduce
reliance
on
traditional
sources
and
has
attracted
significant
research
interest.
Reticular
materials,
including
metal‐organic
frameworks
(MOFs)
covalent
organic
(COFs),
represent
a
class
of
crystalline
materials
constructed
from
molecular
building
blocks
linked
by
coordination
bonds,
respectively.
function
as
heterogeneous
catalysts,
combining
well‐defined
structures
high
tailorability
akin
homogeneous
catalysts.
In
this
review,
regulation
light
absorption,
charge
separation,
surface
in
photocatalytic
process
through
precise
molecular‐level
design
based
features
reticular
is
elaborated.
Notably,
for
MOFsmicroenvironment
modulation
around
catalytic
sites
affects
performance
delved,
with
emphasis
their
unique
dynamic
flexible
microenvironments.
For
COFs,
inherent
excitonic
effects
due
fully
nature
discussed
highlight
strategies
regulate
charge‐
and/or
energy‐transfer‐mediated
photocatalysis.
Finally,
current
challenges
future
directions
field,
aiming
provide
comprehensive
understanding
how
be
optimized
enhanced
photocatalysis
discussed.
Graphitic
carbon
nitride
(C3N4)
has
been
identified
as
an
optimal
material
for
hydrogen
peroxide
(H2O2)
photosynthesis,
although
its
utility
is
hampered
by
a
high
photocarrier
recombination
rate.
Herein,
novel
with
giant
built-in
electric
field
(BEF),
Trz-CN,
synthesized
through
hydrothermal-calcination
tandem
strategy.
The
BEF
(4.8-fold)
induced
the
large
dipole
moment
facilitated
efficient
separation
and
directional
migration
of
photogenerated
carriers.
Trz-CN
exhibited
H2O2
production
rate
569.9
µmol·g-1·h-1
using
O2
feedstock
under
visible
light
(λ
>
420
nm),
marking
impressive
11.2-fold
enhancement
compared
to
bulk
C3N4.
Utilizing
air
instead
pure
resulted
in
trivial
1.6%
decrease
generation
while
maintaining
substantial
560.6
µmol·g-1·h-1.
Notably,
showcased
sterilization
99.9%
against
Escherichia
coli
(E.
coli)
natural
seawater.
Density
functional
theory
(DFT)
calculations
revealed
that
incorporating
nitrogen-rich
skeleton
into
C3N4
enhanced
oxygen
adsorption
capacity
lowered
energy
barrier
formation.
This
leads
photocatalytic
performance
ambient
conditions.
provides
new
exploratory
idea
direct
synthesis
ballast
water
treatment.
