Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 9, 2024
Abstract
Despite
the
significant
milestones
in
half‐reduction
process
of
photocatalysis,
challenges
remain
fully
utilizing
electron–hole
pairs
simultaneous
redox
reactions.
Herein,
a
Z‐scheme
ZnIn
2
S
4
/W
18
O
49
(ZW)
hybrid
with
complementary
band
edge
potential
is
situ
constructed.
The
resultant
fuzzy
1D‐assembled
sea‐urchin
photocatalyst
demonstrates
an
optimal
H
and
benzaldehyde
yield
122
106
µmol
h
−1
under
λ
>
420
nm
light
irradiation.
This
sacrificial‐agent‐free
system
entails
solar‐to‐hydrogen
(STH)
apparent
quantum
efficiency
(AQE)
values
0.466%
2.48%
(420
nm),
respectively,
surpassing
most
recently
reported
photocatalytic
systems
without
aid
noble
metal
cocatalysts.
outstanding
performance
mainly
attributed
to
synergistic
formation
intimate
heterojunction
induction
localized
surface
plasmon
resonances.
Comprehensive
characterization
studies
prove
direct
injection
energetic
hot
electrons
promote
number
long‐lived
active
electrons.
Besides,
electron
paramagnetic
resonance
scavenger
tests
clarify
complicated
mechanistic
puzzle
dual‐redox
reaction,
where
formed
dominantly
via
O─H
activation
followed
by
C─H
cleavage
benzyl
alcohol
over
ZW
hybrid.
Lastly,
universal
use
composites
testified
various
systems.
study
offers
novel
outlook
for
designing
dual‐functioning
heterojunctions
toward
feasible
photoredox
application.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(37)
Published: April 15, 2024
Abstract
The
sustainable
production
of
hydrogen
utilizing
solar
energy
is
a
pivotal
strategy
for
reducing
reliance
on
fossil
fuels.
ZnIn
2
S
4
(ZIS),
as
typical
metal
sulfide
semiconductor,
has
received
extensive
attention
in
photocatalysis.
Although
the
introduction
sulfur
(S)
vacancies
ZIS
to
enhance
photocatalytic
by
creating
defect
levels
been
explored,
detailed
studies
control
and
modulation
S‐vacancies
are
sparce.
This
study
demonstrates
that
while
moderate
can
evolution,
excessive
may
hinder
process,
underscoring
importance
S‐vacancy
modulation.
Guided
theoretical
calculations,
We
have
designed
synthesized
with
modulated
realize
favorable
adsorption‐free
integrated
Schottky‐heterojunction
MXene
co‐catalysts
enhanced
evolution.
optimized
evolution
performance
/MXene
(ZMX)
reaches
14.82
mmol
g
−1
h
under
visible
light
irradiation,
surpassing
many
reported
‐based
photocatalysts.
ascribed
widened
absorption
carrier
transportation
realized
co‐catalytic
effect.
Femtosecond
ultrafast
(fs‐TA)
spectra
other
in‐situ/ex‐situ
characterizations
further
prove
an
efficient
separation
transfer
as‐prepared
ZMX
catalyst.
These
findings
open
up
new
perspectives
designing
catalysts
vacancy
Results in Surfaces and Interfaces,
Journal Year:
2024,
Volume and Issue:
14, P. 100188 - 100188
Published: Jan. 23, 2024
The
photocatalytic
hydrogen
evolution
technology
converts
solar
energy
into
clean
and
environmentally
friendly
energy,
which
is
considered
an
effective
means
to
solve
environmental
pollution
crisis.
unique
sp
sp2
hybrid
carbon
network
structure
of
graphdiyne
endows
it
with
excellent
carrier
mobility,
high
porosity,
making
a
promising
material
for
conversion.
This
article
provides
detailed
description
the
structural
properties
adjustable
bandgap
graphdiyne.
In
addition,
review
was
provided
on
modification
strategies
based
catalysts
evolution,
including
titanium
photocatalysts,
metal
oxide
double
hydroxide
catalysts,
organic
framework
photocatalysts
other
typical
semiconductors.
Finally,
challenges
opportunities
developing
semiconductors
water
splitting
were
proposed.
Timely
expected
contribute
rapid
development
in
field
evolution.
The
construction
of
S-scheme
heterojunction
is
an
effective
approach
to
accelerate
photocarrier
transfer
and
improve
charge
utilization,
thus
promoting
photocatalytic
hydrogen
evolution.
Herein,
we
report,
for
the
first
time,
a
based
on
sulfur-vacancy-modified
ZnIn2S4
(Sv-ZIS)
covalent
organic
frameworks
(COFs),
by
in-situ
growth
Sv-ZIS
COF
TpPa-1
(composed
1,3,5-triformylphloroglucinol
p-phenylenediamine).
Under
visible-light
irradiation,
in
absence
cocatalyst,
optimal
Sv-ZIS/TpPa-1
(5:1)
(with
Sv-ZIS:
mass
ratio
5:1)
achieved
enhanced
production
rate
2745
μmol
g−1
h−1
than
parent
ZIS/TpPa-1
(5:1),
with
AQE
4.67%
at
420
nm.
Theoretical
calculations
confirmed
that
sulfur-vacancy
enlarged
internal
electric
field
(IEF)
Sv-ZIS/TpPa-1,
leading
greater
interfacial
from
ZIS
TpPa-1.
IEF
rapid
separation
photocarriers
following
mechanism
synergistically
guaranteed
improved
performance.
Journal of Materiomics,
Journal Year:
2024,
Volume and Issue:
11(3), P. 100918 - 100918
Published: July 27, 2024
The
construction
of
heterojunction
is
an
effective
way
to
promote
the
photoinduced
charge
carrier
separation
in
spatial,
thus
accelerating
photocatalytic
reaction.
However,
regulation
interface
properties,
as
a
crucial
factor
affecting
diffusion
process,
still
remains
significant
challenge.
In
this
work,
BiOBr/TpBD-COF
was
successfully
constructed
via
novel
phase
transformation
strategy.
Specifically,
perovskite
Cs3Bi2Br9
first
synthesized
and
then
in-situ
transformed
into
BiOBr
during
preparation
TpBD-COF
procedure,
obtaining
with
favorable
interface.
According
X-ray
photoelectron
spectroscopy
(XPS)
characterization
electron
paramagnetic
resonance
(EPR)
analysis,
photogenerated
electrons
weak
reduction
power
transfer
from
driven
by
internal
electric
field
under
irradiation,
conforming
S-scheme
mode.
As
result,
holes
strong
redox
abilities
are
spatially
located
on
surface,
respectively,
endowing
driving
force
toward
water
splitting
optimized
10%BiOBr/TpBD-COF
displayed
remarkably
enhanced
hydrogen
evolution
rate
(16.17
mmol·g−1·h−1)
comparison
(5.18
mmol·g−1·h−1).
This
study
will
provide
some
inspirations
for
developing
efficient
COF-based
photocatalysts.