Small,
Journal Year:
2024,
Volume and Issue:
20(27)
Published: Jan. 24, 2024
It
is
a
challenge
to
regulate
charge
separation
dynamics
and
redox
reaction
kinetics
at
the
atomic
level
synergistically
boost
photocatalytic
hydrogen
(H
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
32(23)
Published: March 14, 2022
Abstract
Ultrafast
excited‐state
decay
and
intrinsic
charge
carrier
recombination
restrain
the
photoactivity
enhancement
for
solar‐to‐H
2
production.
Here,
a
CdS‐fullerene/graphene
(CdS‐F/G)
photocatalyst
is
synthesized
enhancing
visible‐light‐driven
hydrogen
generation
from
earth‐abundant
water.
The
CdS‐F/G
shows
ultrafast
interfacial
electrons/holes
transfer
holes
self‐trapping
process
in
photocatalysis.
in‐situ
dynamic
study
transient
absorption
spectroscopy
reveals
sub‐microsecond‐lived
excited
states
(≈172.6
ns),
electron
(≈30.3
ps),
hole
trapping
(≈44.0
ps)
photocatalyst.
efficient
active
species
transportation
prolonged
lifetime
significantly
enhance
separation
state
survival,
increasing
photostability.
Consequently,
visible‐light
activity
(>400%)
of
H
evolution
reaction
(HER)
obtained
at
with
high
stability
(>36
h).
127.2
µmol
h
−1
g
performance
corresponding
to
quantum
efficiency
7.24%
420
nm
not
only
higher
than
case
pristine
CdS
(29.2
)
but
also
much
that
CdS‐Pt
(73.8
).
cost‐effective
exhibits
great
potential
sustainable
high‐efficiency
photocatalytic
water
splitting
into
clean
energy
carriers.
Moreover,
optimized
electronic
structure
associated
promotes
overall
O
generation.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(13)
Published: Feb. 15, 2023
Abstract
Covalent
organic
frameworks
(COFs)
as
appealing
platforms
have
received
tremendous
interest
in
the
field
of
photocatalytic
H
2
evolution
owing
to
their
well‐defined
structures
and
tailor‐made
function.
However,
excitonic
effects
resulting
from
Coulomb
interactions
between
electron–hole
pairs
are
key
rate‐determining
processes
hydrogen
evolution,
which
usually
ignored.
Thus,
it
is
profound
significance
highly
desired,
but
still
a
challenge,
explore
new
routes
modulate
dissociation
COFs
for
boosting
photocatalysis.
To
address
this
Ni‐intercalated
fluorenone‐based
(Ni‐COF‐SCAU‐1)
at
imine
linkage,
proposed
first
time,
demonstrated
exhibit
enhanced
polarization
electric
field;
thus,
facilitating
Hall
electron
mobility
singlet
excitons
into
free
charge
carriers
under
photoexcitation
participate
surface
reaction.
Benefiting
these
results,
Ni‐COF‐SCAU‐1
displays
production
rate
197.46
mmol·g
−1
h
visible
light
irradiation
with
an
apparent
quantum
efficiency
(AQE)
up
43.2%
420
nm.
This
work
offers
in‐depth
understanding
crucial
role
interlayer
atomic
interface
improving
paves
way
regulation
COFs.
Journal of Materials Chemistry A,
Journal Year:
2022,
Volume and Issue:
10(13), P. 6835 - 6871
Published: Jan. 1, 2022
A
comprehensive
review
about
the
recent
advances
of
single-atom
catalysts
for
photocatalytic
and
photoelectrochemical
water
splitting
is
presented
by
highlighting
distinctive
roles,
unique
fabrication
methods
specific
design
strategies.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(5), P. 3241 - 3249
Published: Jan. 26, 2024
Photocatalytic
CO2
reduction
holds
great
potential
for
alleviating
global
energy
and
environmental
issues,
where
the
electronic
structure
of
catalytic
center
plays
a
crucial
role.
However,
spin
state,
key
descriptor
properties,
is
largely
overlooked.
Herein,
we
present
simple
strategy
to
regulate
states
Co
centers
by
changing
their
coordination
environment
exchanging
species
into
stable
Zn-based
metal–organic
framework
(MOF)
afford
Co-OAc,
Co-Br,
Co-CN
photoreduction.
Experimental
DFT
calculation
results
suggest
that
distinct
sites
give
rise
different
charge
separation
abilities
barriers
adsorption/activation
in
photocatalysis.
Consequently,
optimized
Co-OAc
with
highest
spin-state
presents
an
excellent
photocatalytic
activity
2325.7
μmol·g–1·h–1
selectivity
99.1%
CO,
which
are
among
best
all
reported
MOF
photocatalysts,
absence
noble
metal
additional
photosensitizer.
This
work
underlines
MOFs
as
ideal
platform
manipulation
toward
improved
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(33)
Published: April 25, 2023
Abstract
Combining
metal
nanoparticles
(NPs)
featured
with
localized
surface
plasmon
resonance
(LSPR)
metal–organic
framework
(MOF)‐based
photocatalysts
is
a
novel
means
for
achieving
efficient
separation
of
electron–hole
pairs.
Herein,
the
Au@NH
2
‐UiO‐66/CdS
composites
are
successfully
synthesized
by
encapsulating
Au
NPs
LSPR
into
NH
‐UiO‐66
nanocage,
further
growing
CdS
on
‐UiO‐66,
which
exhibits
higher
photocatalytic
activity
in
hydrogen
evolution
reaction
under
visible‐light
irradiation
than
that
and
CdS,
respectively.
Transient
absorption
measurements
reveal
MOF
not
only
transit
station
electrons
generated
from
to
Au,
but
also
receiver
hot
plasmonic
Au@MOF/CdS
composites.
Thus,
LSPR‐induced
electron
transfer
an
important
manifestation
prolong
carrier
lifetime
enhance
performance.
This
work
provides
insights
investigating
photoinduced
dynamics
nanomaterials
effects
enhancing
MOF‐based