Abstract
Herein,
guided
by
the
results
of
density
functional
theory
prediction,
study
rationally
designs
a
hollow
core–shell
FeNi
2
S
4
@ZnIn
(FNS@ZIS)
Step‐scheme
(S‐scheme)
heterojunction
for
photocatalytic
H
evolution
with
photothermal‐assisted.
The
FNS
spheres
offered
substrate
coating
ZIS
nanosheets,
which
can
inhibit
nanosheets
from
agglomerating
into
pellet,
enrich
active
site,
increase
specific
surfaces,
and
raise
light
absorption.
Notably,
due
to
its
excellent
photothermal
properties,
core
generated
heat
unceasingly
inside
under
visible‐light
irradiation
effectively
prevent
loss
reaction
system,
increased
local
temperature
photocatalysts
thus
accelerated
charge
migration.
In
addition,
S‐scheme
construction
via
in
situ
growth
has
tight
interface,
facilitate
separation
transfer
carriers
achieve
high
redox
potential.
Owning
distinctive
construction,
FNS@ZIS
show
extraordinary
stability
rate
7.7
mmol
h
−1
g
,
is
≈15.2‐fold
than
pristine
ZIS.
Based
on
double
evidence
theoretical
predictions
experimental
confirmations,
effect
electron
mechanism
this
innovative
material
are
investigated
depth
following
infrared
thermography
technology
deep
DFT
calculations.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июнь 3, 2024
Abstract
Artificial
photosynthesis
using
carbon
nitride
(g-C
3
N
4
)
holds
a
great
promise
for
sustainable
and
cost-effective
H
2
O
production,
but
the
high
carrier
recombination
rate
impedes
its
efficiency.
To
tackle
this
challenge,
we
propose
an
innovative
method
involving
multispecies
iodine
mediators
(I
−
/I
intercalation
through
pre-photo-oxidation
process
potassium
iodide
(suspected
deteriorated
“KI”)
within
g-C
framework.
Moreover,
introduce
external
electric
field
by
incorporating
cationic
methyl
viologen
ions
to
establish
auxiliary
electron
transfer
channel.
Such
unique
design
drastically
improves
separation
of
photo-generated
carriers,
achieving
impressive
production
46.40
mmol
g
−1
h
under
visible
light
irradiation,
surpassing
most
visible-light
-producing
systems.
Combining
various
advanced
characterization
techniques
elucidates
inner
photocatalytic
mechanism,
application
potential
system
is
validated
with
simulation
scenarios.
This
work
presents
significative
strategy
preparing
applying
highly
efficient
-based
catalysts
in
photochemical
production.
Abstract
Owing
to
the
improved
charge
separation
and
maximized
redox
capability
of
system,
Step‐scheme
(S‐scheme)
heterojunctions
have
garnered
significant
research
attention
for
efficient
photocatalysis
H
2
evolution.
In
this
work,
an
innovative
linear
donor–acceptor
(D–A)
conjugated
polymer
fluorene‐alt‐(benzo‐thiophene‐dione)
(PFBTD)
is
coupled
with
CdS
nanosheets,
forming
organic–inorganic
S‐scheme
heterojunction.
The
CdS/PFBTD
(CP)
composite
exhibits
impressed
hydrogen
production
rate
7.62
mmol
g
−1
h
without
any
co‐catalysts,
which
≈14
times
higher
than
pristine
CdS.
It
revealed
that
outstanding
photocatalytic
performance
attributed
formation
rapid
electron
transfer
channels
through
interfacial
Cd─O
bonding
as
evidenced
by
density
functional
theory
(DFT)
calculations
in
situ
X‐ray
photoelectron
spectroscopy
(XPS)
analysis.
mechanism
involved
further
investigated
photo‐irradiated
Kelvin
probe
force
microscopy
(KPFM)
This
work
provides
a
new
point
view
on
points
out
direction
designing
superior
heterojunction
photocatalysts.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 20, 2024
Crafting
semiconducting
heterojunctions
represents
an
effective
route
to
enhance
photocatalysis
by
improving
interfacial
charge
separation
and
transport.
However,
lattice
mismatch
(δ)
between
different
semiconductors
can
significantly
hinder
dynamics.
Here,
meticulous
tailoring
is
reported
create
a
covalent
heterointerface
with
built-in
electric
field
(BIEF),
imparting
markedly
improved
hydrogen
peroxide
(H
Abstract
Herein,
guided
by
the
results
of
density
functional
theory
prediction,
study
rationally
designs
a
hollow
core–shell
FeNi
2
S
4
@ZnIn
(FNS@ZIS)
Step‐scheme
(S‐scheme)
heterojunction
for
photocatalytic
H
evolution
with
photothermal‐assisted.
The
FNS
spheres
offered
substrate
coating
ZIS
nanosheets,
which
can
inhibit
nanosheets
from
agglomerating
into
pellet,
enrich
active
site,
increase
specific
surfaces,
and
raise
light
absorption.
Notably,
due
to
its
excellent
photothermal
properties,
core
generated
heat
unceasingly
inside
under
visible‐light
irradiation
effectively
prevent
loss
reaction
system,
increased
local
temperature
photocatalysts
thus
accelerated
charge
migration.
In
addition,
S‐scheme
construction
via
in
situ
growth
has
tight
interface,
facilitate
separation
transfer
carriers
achieve
high
redox
potential.
Owning
distinctive
construction,
FNS@ZIS
show
extraordinary
stability
rate
7.7
mmol
h
−1
g
,
is
≈15.2‐fold
than
pristine
ZIS.
Based
on
double
evidence
theoretical
predictions
experimental
confirmations,
effect
electron
mechanism
this
innovative
material
are
investigated
depth
following
infrared
thermography
technology
deep
DFT
calculations.
