Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(13), P. 9163 - 9171
Published: March 22, 2024
It
remains
challenging
to
obtain
a
single
product
in
the
gas–solid
photocatalytic
reduction
of
CO2
because
CO
and
CH4
are
usually
produced
simultaneously.
This
study
presents
design
I-type
nested
heterojunction
TiO2/BiVO4
with
controllable
electron
transport
by
modulating
TiO2
component.
demonstrates
that
slowing
could
enable
TiO2/BiVO4-4
generate
100%
selectivity.
In
addition,
modifying
loading
Cu
atom
further
increased
yield
3.83
times
(17.33
μmol·gcat–1·h–1),
while
maintaining
selectivity
for
CO.
Characterization
density
functional
theory
(DFT)
calculations
revealed
was
mainly
determined
support,
whereas
efficiently
adsorbed
activated
atom.
Such
two-step
regulation
strategy
combining
enhances
possibility
simultaneously
obtaining
high
CO2.
Small,
Journal Year:
2021,
Volume and Issue:
17(41)
Published: Sept. 12, 2021
Reasonable
design
of
efficient
hierarchical
photocatalysts
has
gained
significant
attention.
Herein,
a
step-scheme
(S-scheme)
core-shell
TiO2
@ZnIn2
S4
heterojunction
is
designed
for
photocatalytic
CO2
reduction.
The
optimized
sample
exhibits
much
higher
photoreduction
conversion
rates
(the
sum
yield
CO,
CH3
OH,
and
CH4
)
than
the
blank
control,
i.e.,
ZnIn2
.
improved
performance
can
be
attributed
to
inhibited
recombination
photogenerated
charge
carriers
induced
by
S-scheme
heterojunction.
improvement
also
large
specific
surface
areas
abundant
active
sites.
Meanwhile,
transfer
mechanism
testified
in
situ
irradiated
X-ray
photoelectron
spectroscopy,
work
function
calculation,
electron
paramagnetic
resonance
measurements.
This
provides
an
effective
strategy
designing
highly
solar
fuels.
Energy & Environmental Science,
Journal Year:
2021,
Volume and Issue:
15(3), P. 880 - 937
Published: Nov. 16, 2021
Photocatalytic
CO
2
conversion
is
vital
technology
to
realize
global
carbon
neutrality
and
generate
future
energy
supplies.
This
review
proposes
fundamentals,
challenges,
strategies,
prospects
for
photocatalytic
research.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
34(23)
Published: March 9, 2022
Abstract
2D
materials
show
many
particular
properties,
such
as
high
surface‐to‐volume
ratio,
anisotropic
degree,
and
adjustable
chemical
functionality.
These
unique
properties
in
have
sparked
immense
interest
due
to
their
applications
photocatalytic
systems,
resulting
significantly
enhanced
light
capture,
charge‐transfer
kinetics,
surface
reaction.
Herein,
the
research
progress
photocatalysts
based
on
varied
compositions
functions,
followed
by
specific
modification
strategies,
is
introduced.
Fundamental
principles
focusing
harvesting,
charge
separation,
molecular
adsorption/activation
2D‐material‐based
system
are
systemically
explored.
The
examples
described
here
detail
use
of
various
energy‐conversion
including
water
splitting,
carbon
dioxide
reduction,
nitrogen
fixation,
hydrogen
peroxide
production,
organic
synthesis.
Finally,
elaborating
challenges
possible
solutions
for
developing
these
materials,
review
expected
provide
some
inspiration
future
used
efficient
energy
conversions.
Advanced Energy Materials,
Journal Year:
2022,
Volume and Issue:
12(46)
Published: Oct. 6, 2022
Abstract
The
aggravating
extreme
climate
changes
and
natural
disasters
stimulate
the
exploration
of
low‐carbon/zero‐carbon
alternatives
to
traditional
carbon‐based
fossil
fuels.
Solar‐to‐hydrogen
(STH)
transformation
is
considered
as
appealing
route
convert
renewable
solar
energy
into
carbon‐free
hydrogen.
Restricted
by
low
efficiency
high
cost
noble
metal
cocatalysts,
high‐performance
cost‐effective
photocatalysts
are
required
realize
realistic
STH
transformation.
Herein,
2D
FePS
3
(FPS)
nanosheets
anchored
with
TiO
2
nanoparticles
(TiO
/FePS
)
synthesized
tested
for
photocatalytic
hydrogen
evolution
reaction.
With
integration
FPS,
H
‐evolution
rate
on
radically
increased
≈1686%,
much
faster
than
that
alone.
origin
greatly
raised
activity
revealed
theoretical
calculations
various
advanced
characterizations,
such
transient‐state
photoluminescence
spectroscopy/surface
photovoltage
spectroscopy,
in
situ
atomic
force
microscopy
combined
Kelvin
probe
(AFM‐KPFM),
X‐ray
photoelectron
spectroscopy
(XPS),
synchrotron‐based
absorption
near
edge
structure.
Especially,
AFM‐KPFM
XPS
together
confirm
electron
transport
pathway
light
illumination,
unveiling
efficient
separation/transfer
charge
carrier
step‐scheme
heterojunction.
This
work
sheds
designing
fabricating
novel
material‐based
S‐scheme
heterojunctions
photocatalysis.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(10)
Published: Jan. 2, 2023
The
highly
selective
photoreduction
of
CO2
into
valuable
small-molecule
chemical
feedstocks
such
as
CO
is
an
effective
strategy
for
addressing
the
energy
crisis
and
environmental
problems.
However,
it
remains
a
challenge
because
complex
process
usually
generates
multiple
possible
products
requires
subsequent
separation
step.
In
this
paper,
2D
monolayer
bilayer
porphyrin-based
metal-organic
frameworks
(MOFs)
are
successfully
constructed
by
adjusting
reaction
temperature
solvent
polarity
with
5,10,15,20-tetrakis(4-pyridyl)porphyrin
light-harvesting
ligand.
MOF
low-dimensional
special
structure
in
which
upper
lower
layers
arranged
dislocation
bridged
halogen
ions.
This
exhibits
100%
ultra-high
selectivity
reduction
to
under
simulated
sunlight
without
any
cocatalyst
or
photosensitizer
can
be
recycled
at
least
three
times.
intrinsic
mechanism
photocatalytic
explored
through
experimental
characterization
density
functional
theory
(DFT)
calculations.
work
shows
that
rational
design
number
structures
tune
stability
these
opens
new
avenue
photocatalysts.
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
32(29)
Published: Feb. 23, 2022
Abstract
Sparked
by
natural
photosynthesis,
solar
photocatalysis
using
metal‐free
graphitic
carbon
nitride
(g‐C
3
N
4
)
with
appealing
electronic
structure
has
turned
up
as
the
most
captivating
technique
to
quest
for
sustainable
energy
generation
and
pollution‐free
environment.
Nonetheless,
low‐dimensional
g‐C
is
thwarted
from
sluggish
kinetics
rapid
recombination
of
photogenerated
carriers
upon
light
irradiation.
Among
multifarious
modification
strategies,
engineering
2D
cocatalysts
anticipated
accelerate
redox
kinetics,
augment
active
sites
ameliorate
electron–hole
separation
boosted
activity
thanks
its
face‐to‐face
contact
surface.
It
timely
technological
significance
review
2D/2D
interfaces
state‐of‐the‐art
cocatalysts,
spanning
carbon‐containing
phosphorus‐containing,
metal
dichalcogenide,
other
cocatalysts.
Fundamental
principles
each
photocatalytic
application
will
be
introduced.
Thereafter,
recent
advances
cocatalyst‐mediated
systems
critically
evaluated
based
on
their
interfacial
engineering,
emerging
roles,
impacts
toward
stability
catalytic
efficiency.
Importantly,
mechanistic
insights
into
charge
dynamics
structure–performance
relationship
deciphered.
Last,
noteworthy
research
directions
are
prospected
deliver
insightful
ideas
future
development
.
Overall,
this
serve
a
scaffold
cornerstone
in
designing
dimensionality‐dependent
cocatalyst‐assisted
renewable
ecologically
green
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
61(6)
Published: Nov. 9, 2021
Dual-atom-site
catalysts
(DACs)
have
emerged
as
a
new
frontier
in
heterogeneous
catalysis
because
the
synergistic
effect
between
adjacent
metal
atoms
can
promote
their
catalytic
activity
while
maintaining
advantages
of
single-atom-site
catalysts,
such
almost
100
%
atomic
efficiency
and
excellent
hydrocarbon
selectivity.
In
this
study,
cobalt-based
atom
site
with
Co2
-N
coordination
structure
were
synthesized
used
for
photodriven
CO2
reduction.
The
resulting
CoDAC
containing
3.5
Co
demonstrated
superior
ratio
reduction
performance,
65.0
CH4
selectivity,
which
far
exceeds
that
(CoSACs).
intrinsic
reason
CoDACs
is
adsorption
strength
CO*
intermediates
at
dimeric
active
sites.