Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 26, 2025
Abstract
Optimizing
the
binding
sites
of
substrates
for
small
molecules
activation
plays
a
crucial
role
in
enzyme‐like
catalysts
design.
Herein,
frustrated
Lewis
pairs
(FLPs)
are
successfully
constructed
through
boron
(B)
doping
into
CoO
x
(CoBO
)
with
abundant
oxygen
vacancies
(O
v
).
The
O
optimizes
valence
active
sites,
creates
coordinatively
unsaturated
state,
and
elongates
distance
pairs.
electron‐deficient
acid
(LA)
(Co)
facilitate
adsorption
dissociation
2
,
electron‐rich
base
(LB)
(O)
draw
positively
charged
TMB
closer
to
Co
shorten
reaction
distance,
which
synergistically
improve
oxidase
(OXD)‐like
activity.
Besides,
increase
electron
density
induced
by
FLPs
promotes
electrons
transfer,
intermediates
stabilization,
decreases
energy
barrier
rate‐determining
step
.
Significantly,
proof‐of‐concept
application
colorimetric
biosensing
platform,
as‐developed
CoBO
demonstrate
highly
sensitive
selective
detection
capacity
dopamine
(DA)
targets.
This
work
verifies
possibility
activating
catalysis.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(50), С. 27415 - 27423
Опубликована: Дек. 11, 2023
Synchronized
conversion
of
CO2
and
H2O
into
hydrocarbons
oxygen
via
infrared-ignited
photocatalysis
remains
a
challenge.
Herein,
the
hydroxyl-coordinated
single-site
Ru
is
anchored
precisely
on
metallic
TiN
surface
by
NaBH4/NaOH
reforming
method
to
construct
an
infrared-responsive
HO-Ru/TiN
photocatalyst.
Aberration-corrected
high-angle
annular
dark-field
scanning
transmission
electron
microscopy
(ac-HAADF-STEM)
X-ray
absorption
spectroscopy
(XAS)
confirm
atomic
distribution
species.
XAS
density
functional
theory
(DFT)
calculations
unveil
formation
HO-RuN5-Ti
Lewis
pair
sites,
which
achieves
efficient
polarization/activation
dual
coordination
with
C
O
atoms
HO-Ru/TiN.
Also,
implanting
species
powerfully
boosts
separation
transfer
photoinduced
charges.
Under
infrared
irradiation,
catalyst
shows
superior
CO2-to-CO
transformation
activity
coupled
oxidation
release
O2,
reduction
rate
can
further
be
promoted
about
3-fold
under
simulated
sunlight.
With
key
reaction
intermediates
determined
in
situ
diffuse
reflectance
Fourier
transform
(DRIFTS)
predicted
DFT
simulations,
possible
photoredox
mechanism
system
proposed.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(37)
Опубликована: Апрель 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
ACS Catalysis,
Год журнала:
2023,
Номер
13(19), С. 12700 - 12710
Опубликована: Сен. 14, 2023
The
photocatalytic
reduction
of
CO2
into
high-value-added
fuels
is
an
extremely
desirable
process,
but
its
practical
application
limited
by
the
weak
adsorption
and
activation
inert
molecules.
Herein,
oxygen
vacancies
(VOs)
are
formed
on
SrBi2Ta2O9
(SBT)
annealing
in
Ar
gas
at
400
°C
can
spontaneously
react
with
adsorbed
H2O
to
form
surface
hydroxyls.
Therefore,
frustrated
Lewis
pairs
(FLPs)
fabricated
SBT,
where
VO
proximal
hydroxyl
serve
as
acid
base,
respectively.
Experimental
results
indicate
that
obtained
FLPs
act
catalytic
sites
adsorb,
activate,
convert
under
low-intensity
LED
light
irradiation
(420
nm).
Consequently,
a
CO2-to-CO
conversion
rate
9.9
μmol
g–1
h–1
achieved
pure
water
VO-SBT-OH
without
any
sacrificial
agents
or
cocatalysts,
which
∼4×
higher
than
pristine
SBT.
Moreover,
self-replenish
dissociating
during
reaction,
thereby
achieving
long-term
for
60
h.
Our
study
demonstrates
potential
platform
decrease
barriers
reducing
provides
valuable
insights
underlying
mechanism.
Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июнь 27, 2024
Abstract
Artificial
photosynthesis
emerges
as
a
strategic
pathway
to
produce
hydrogen
peroxide
(H
2
O
),
an
environmentally
benign
oxidant
and
clean
energy
carrier.
Nonetheless,
in
many
heterojunction‐based
artificial
photosynthetic
systems,
the
H
productivity
is
significantly
hindered
by
poor
carrier
transport,
narrow
spectral
light
absorption,
lack
of
adequate
active
sites
for
two‐electron
oxygen
reduction
reaction.
Herein,
catalyst
architecture
with
iso‐elemental
heterojunction
formed
interfacing
Zn
3
In
S
6
nano‐flowers
ZnIn
4
nanosheets
proposed.
This
exhibits
production
rate
high
23.47
µmol
g
−1
min
under
UV–vis
irradiation,
which
attributed
minimized
contact
barrier
enhanced
lattice
match
at
/Zn
interface
thanks
aids
efficient
separation
transfer
photogenerated
carriers.
Theoretical
simulations
alongside
comprehensive
in‐situ
ex‐situ
characterizations
confirm
photo‐redox
generation
effective
dynamics
across
surface.
Moreover,
substituting
one
reduction‐type
other
non‐iso‐elemental
catalysts
like
CdIn
,
TiO
CdS
further
confirms
feasibility
superiority
proposed
configuration.
work
offers
new
perspective
on
designing
.
