Catalysts,
Год журнала:
2024,
Номер
15(1), С. 19 - 19
Опубликована: Дек. 29, 2024
The
photocatalytic
N2
fixation
reaction
still
faces
high
activation
energy
barriers
and
inefficient
electron
transfer
efficiency,
limiting
the
overall
ammonia
yield
of
semiconductors.
This
communication
reports
on
construction
an
organic/inorganic
g-C3N4/oxygen
vacancy-enriched
TiO2
(g-C3N4/TiO2-OV)
composite
system
via
annealing
treatment
in
H2/Ar
mixed
atmosphere
for
enhanced
activity.
After
illumination
4
h,
g-C3N4/TiO2-OV
with
1
wt%
g-C3N4
loading
demonstrates
optimal
31.6
μmol
L−1.
study
existence
oxygen
vacancies
surface
through
EPR
while
also
investigating
carrier
separation
transport
efficiency
material
using
photoelectric
characterization.
experimental
results
indicate
that
introduction
OVs
into
serves
as
Lewis
acid
sites,
facilitating
adsorption.
Moreover,
lower
onset
potential
higher
current
density
composites
heterojunction
significantly
decreases
interfacial
charge
recombination
barrier,
effectively
improving
towards
photo-reduction.
work
emphasizes
importance
rational
tailoring
TiO2-based
photocatalysts
field
fixation.
Materials Horizons,
Год журнала:
2024,
Номер
unknown
Опубликована: Янв. 1, 2024
The
processing
of
conjugated
organic
materials
into
films,
nanoparticles,
and
nanofibers,
presents
significant
opportunities
to
increase
their
activity
for
photocatalytic
hydrogen
evolution
scaled-up
systems
real
world
applications.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 19, 2024
Abstract
Covalent
triazine
frameworks
(CTFs),
noted
for
their
rich
nitrogen
content,
have
attracted
significant
attention
as
promising
photocatalysts.
However,
the
structural
complexity
introduced
by
diversity
of
atoms
in
nitrogen‐rich
CTFs
poses
a
substantial
challenge
discovering
high‐performance
CTFs.
To
address
this
challenge,
machine‐learning
approach
is
developed
to
rationally
design
CTFs,
which
subsequently
validated
through
experimental
methods.
A
framework
employed
based
on
special
orthogonal
group
three
dimensions
(SO(3))‐invariant
graph
neural
networks
predict
photocatalytic
properties
structures.
This
achieves
exceptionally
high
accuracies
with
R
2
scores
exceeding
0.98.
From
dataset
14920
structures,
identifies
45
candidates.
Guided
these
predictions,
novel
CTF
structure,
pyridine‐2,5‐dicarbaldehyde
(CTF‐DCPD)
selected
and
successfully
synthesized,
exhibits
an
ultrahigh
hydrogen
evolution
rate
17.70
mmol
g
−1
h
.
significantly
surpasses
that
widely
studied
CTF‐1,4‐dicyanobenzene
(CTF‐DCB,
10.41
).
work
provides
new
paradigm
machine
learning
accelerate
materials
development,
can
be
generalized
development
other
functional
materials.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 18, 2024
Abstract
The
ability
to
generate
heterostructures
with
a
desirable
charge
transfer
pathway
is
essential
for
achieving
semiconductor
photocatalysts
super
photocatalytic
activity.
Herein,
it
proposed
realize
robust
tailoring
of
effective
in
semiconductor‐based
via
work
function
regulation,
and
elucidate
the
influence
on
mechanism
at
heterostructure
interface.
Specifically,
taking
type‐II
SrTiO
3
/Mn
O
4
as
an
example,
introducing
BiFeO
into
effectively
regulate
(BiFeO
)
x
(SrTiO
1−
(B
T
solid
solution
through
optimizing
value.
Combined
situ
testing,
results
show
that
original
heterojunction
converted
S‐scheme
0.3
0.7
when
introduced.
This
increases
semiconductor,
inducing
light‐generated
carriers
be
guided
separated
by
generated
built‐in
electric
field.
Therefore,
implementation
this
strategy
can
achieve
efficient
CO
2
reduction.
In
contrast
pristine
,
exhibits
28‐fold
enhancement
electron
consumption
rate
during
reduction,
reaction
suggested.
study,
converting
interfacial
pathways
developed
enhance
photoconversion
kinetics
H
O.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 13, 2025
Abstract
Developing
organic
semiconductor
photocatalysts
with
alterable
optical
properties
and
excitonic
behaviors
for
photocatalytic
hydrogen
evolution
has
received
significant
attention
recently.
Herein,
three
polymerized
small‐molecule
acceptors
(PSMAs)
different
linker
lengths,
namely
PY‐1T,
PY‐2T
PY‐3T,
are
designed
synthesized
to
construct
nano‐photocatalysts.
In
comparison
YDT,
these
PSMAs
exhibit
broader
absorption
in
both
visible
near‐infrared
(NIR)
light
region
as
well
enlarged
exciton
diffusion
length.
the
meanwhile,
intramolecular
charge
transfer
separation
is
promoted
by
varying
length,
leading
enhanced
harvesting
utilization.
As
a
result,
single‐component
nano‐photocatalyst
based
on
PY‐3T
achieves
an
impressive
average
rate
(HER)
of
400.3
mmol
h
−1
g
under
AM
1.5G
sunlight
(100
mW
cm
−2
),
which
≈48
times
greater
than
that
YDT
NPs
(8.3
).
These
results
not
only
prove
potential
developing
extended
chain
length
efficient
photocatalysts,
but
also
elucidate
importance
regulating
designing
high‐performance
photocatalysts.
Although
the
design
of
photocatalysts
incorporating
donor-acceptor
units
has
garnered
significant
attention
for
its
potential
to
enhance
efficiency
photocatalysis
process,
primary
bottleneck
lies
in
challenge
generating
long-lived
charge
separation
states
during
exciton
separation.
Therefore,
a
novel
Janus-nanomicelles
photocatalyst
is
developed
using
carbazole
(Cz)
as
donor
unit,
perylene-3,4,9,10-tetracarboxydiimide
(PDI)
with
long-excited
state
acceptor
unit
and
polyethylene
glycol
(PEG)
hydrophilic
segment
through
ROMP
polymerization.
After
optimizing
ratio,
Cz19-PDI18-PEG10
rapidly
adsorbs
bisphenol
A
(BPA)
within
10
s
π-π
interaction,
hydrogen-bonding
hydrophobic
interaction
between
BPA
blocks
when
exposed
aqueous
humor
efficiently
photodegrades
(50
ppm)
120
min
water
purification
purposes
due
achieving
highest
reported
so
far.
Mechanistic
studies
have
shown
that
this
excellent
performance
can
be
attributed
synergistic
interactions
highly
efficient
adsorption
capacity
photocatalysis.
This
strategy
holds
promise
an
effective
candidate
purification.
Inorganic Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 10, 2025
Constructing
a
hollow
porous
ZnO–ZnS
sphere
is
still
big
challenge
due
to
the
difficulty
in
controlling
morphology
and
distribution
of
ZnO
shell
originating
from
fact
that
prefers
grow
along
particular
crystal
planes.
Here,
we
demonstrate
novel
synthetic
strategy
for
preparation
oxygen-vacancy-enriched
(Ov-ZOS
(HP))
spheres
by
combining
concepts
adopting
template-directed
method,
selecting
sulfidation
precursor,
tuning
calcination
process
template.
Structural
characterization
density
functional
theory
(DFT)
calculations
reveal
nanostructures
oxygen
vacancies
heterojunction
are
beneficial
promoting
efficient
charge
transfer
separation.
The
optimized
Ov-ZOS
(HP)
exhibits
enhanced
rates
hydrogen
evolution
reaction
(71.86
mmol
h–1
g–1),
which
1.48,
2.08,
3.0
times
higher
than
those
spheres,
vacancy-enriched
nanosheets,
respectively.
Moreover,
presents
excellent
cyclability
photocatalytic
evolution.
Therefore,
this
study
provides
physical
insights
into
various
semiconductor
heterojunctions
hard
form
through
other
existing
strategies
solar
energy
utilization.
