ACS Catalysis,
Год журнала:
2023,
Номер
13(9), С. 6214 - 6221
Опубликована: Апрель 21, 2023
Photocatalysis
is
promising
for
the
reduction
of
CO2
into
fuels
and
chemicals
under
mild
conditions
but
still
a
challenge
due
to
inert
nature
CO2.
Herein,
ZnIn2S4/In(OH)3–x
(ZIOS)
heterojunction
was
developed
visible-light-driven
reduction,
where
ZnIn2S4
(ZIS)
harvests
light
In(OH)3–x
with
frustrated
Lewis
pairs
(FLPs)
activates
The
hydroxyl-deficient
vacancies
(OHVs)
act
as
acid,
adjacent
hydroxyl
groups
serve
base
form
FLPs.
ZIOS
composites
are
fabricated
via
partial
sulfurization
Zn–In–O
oxide,
constructing
type
II
that
facilitates
photogenerated
electron
transfer
from
reduce
FLP-activated
on
In(OH)3–x.
as-prepared
exhibit
CO
formation
rate
1945.5
μmol·g–1·h–1,
which
about
2.76-fold
higher
than
over
ZnIn2S4,
suppress
hydrogen
evolution
CO/H2
ratio
increasing
0.436
1.6
ZIOS.
This
work
provides
insight
design
efficient
photocatalysts.
Advanced Energy Materials,
Год журнала:
2022,
Номер
12(27)
Опубликована: Июнь 2, 2022
Abstract
With
rising
CO
2
emissions
caused
by
the
massive
consumption
of
fossil
fuels,
it
is
highly
desirable
to
develop
strategies
that
adopt
renewable
energy
convert
into
value‐added
chemical
feedstocks.
Over
past
decades,
photocatalytic
reduction
using
light
has
attracted
considerable
attention.
However,
advanced
photocatalysis
techniques
cannot
exert
their
action
where
unavailable.
Here,
a
method
for
on
basis
vibration‐driven
piezoelectricity
yield
piezo‐electrocatalysis
effect
which
requires
mechanical
vibration
rather
than
light,
proposed.
Under
mild
and
sacrificial
agent‐free
conditions,
piezoelectric
BaTiO
3
catalyst
provides
suitable
piezo‐potential
overcome
redox
potential
with
maximum
63.3
µmol
g
−1
,
achieving
reactivity
comparable
those
photocatalysts.
The
piezo‐electrocatalytic
reaction
adds
new
avenue
in
addition
existing
expanding
scope
utilization
promote
carbon
neutrality.
Energy & Environmental Science,
Год журнала:
2023,
Номер
17(2), С. 518 - 530
Опубликована: Дек. 7, 2023
A
new
all-in-one
design
concept
of
constructing
photochromic
single
atom
photocatalysts
is
proposed
to
achieve
both
high
activity
and
selectivity
photocatalytic
CO
2
-to-CH
4
conversion.
ACS Nano,
Год журнала:
2023,
Номер
17(20), С. 20560 - 20569
Опубликована: Окт. 4, 2023
Inefficient
charge
separation
and
slow
interfacial
reaction
dynamics
significantly
hamper
the
efficiency
of
photocatalytic
CO2
reduction.
Herein,
a
facile
EDC/NHS-assisted
linking
strategy
was
developed
to
enhance
in
heterojunction
photocatalysts.
Using
this
approach,
we
successfully
synthesized
amide-bonded
carbon
quantum
dot-g-C3N4
(CQD-CN)
The
formation
amide
covalent
bonds
between
CN
CQDs
CN-CQD
facilitates
efficient
carrier
migration,
adsorption,
activation.
Exploiting
these
advantages,
photocatalysts
exhibit
high
selectivity
with
CO
CH4
evolution
rates
79.2
2.7
μmol
g-1
h-1,
respectively.
These
are
about
1.7
3.6
times
higher
than
those
CN@CQD
bulk
CN,
Importantly,
demonstrate
exceptional
stability,
even
after
12
h
continuous
testing.
presence
COOH*
signal
is
identified
as
crucial
intermediate
species
conversion
CO.
This
study
presents
bonding
engineering
for
developing
high-performance
solar-driven
reduction
CO2.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(28)
Опубликована: Апрель 23, 2023
Abstract
Photocatalytic
conversion
of
CO
2
into
fuels
using
pure
water
as
the
proton
source
is
immense
potential
in
simultaneously
addressing
climate‐change
crisis
and
realizing
a
carbon‐neutral
economy.
Single‐atom
photocatalysts
with
tunable
local
atomic
configurations
unique
electronic
properties
have
exhibited
outstanding
catalytic
performance
past
decade.
However,
given
their
single‐site
features
they
are
usually
only
amenable
to
activations
involving
single
molecules.
For
photoreduction
entailing
complex
activation
dissociation
process,
designing
multiple
active
sites
on
photocatalyst
for
both
reduction
H
O
still
daunting
challenge.
Herein,
it
precisely
construct
Cu
single‐atom
centers
two‐coordinated
N
vacancies
dual
CN
(Cu
1
/N
2C
V‐CN).
Experimental
theoretical
results
show
that
promote
chemisorption
via
accumulating
photogenerated
electrons,
V
enhance
O,
thereby
facilitating
from
COO*
COOH*.
Benefiting
dual‐functional
sites,
V‐CN
exhibits
high
selectivity
(98.50%)
decent
production
rate
11.12
µmol
g
−1
h
.
An
ingenious
atomic‐level
design
provides
platform
integrating
modified
catalyst
deterministic
identification
property
during
process.
ACS Nano,
Год журнала:
2023,
Номер
17(5), С. 4922 - 4932
Опубликована: Фев. 17, 2023
Photoreduction
of
CO2
is
a
promising
strategy
to
synthesize
value-added
fuels
or
chemicals
and
realize
carbon
neutralization.
Noncopper
catalysts
are
seldom
reported
generate
C2
products,
the
selectivity
over
these
low.
Here,
we
design
rich-interface,
heterostructured
In2O3/InP
(r-In2O3/InP)
for
highly
competitive
photocatalytic
CO2-to-CH3COOH
conversion
with
productivity
96.7
μmol
g–1
>
96%
along
water
oxidation
O2
in
pure
(no
sacrificial
agent)
under
visible
light
irradiation.
The
hard
X-ray
absorption
near-edge
structure
(XANES)
shows
that
formation
r-In2O3/InP
isogenesis
cation
adjusts
coordination
environment
via
interface
engineering
forms
O–In–P
polarized
sites
at
interface.
In
situ
FT-IR
Raman
spectra
identify
key
intermediates
OCCO*
acetate
production
high
selectivity.
Density
functional
theory
(DFT)
calculations
reveal
rich
promotes
C–C
coupling
form
products
because
imbalanced
adsorption
energies
two
atoms.
This
work
reports
an
interesting
indium-based
photocatalyst
selective
photoreduction
strict
solution
irradiation
conditions
provides
significant
insights
into
fabricating
interfacial
polarization
promote
process.
Chemical Engineering Journal,
Год журнала:
2023,
Номер
466, С. 143287 - 143287
Опубликована: Май 2, 2023
The
creation
of
an
isotype
phase
junction
has
been
recognized
as
effective
means
improving
the
spatial
charge
separation
and
migration
in
g-C3N4
materials.
Nevertheless,
due
to
a
lack
electrostatic
control
internal
electric
field,
heterojunction
alone
is
incapable
providing
sufficient
driving
force
maximize
carrier
transfer.
Herein,
we
present
interface
engineering
strategy
for
co-integrating
p-n
heterojunctions
fabricate
g-C3N4/g-C3N4
nanohybrids
using
facile
ultrasonic-assisted
self-assembly
method.
coherent
boundary
between
two
distinct
phases
demonstrates
that
intimate
2D
interfacial
contact
can
be
easily
established
by
π-π
stacking
interactions
because
their
high
structural
similarities
low
lattice
strain.
Furthermore,
compatible
well-matched
electronic
band
structures
led
staggered
type
II
alignment
lateral
heterojunction,
which
confers
resulting
composite
with
strong
redox
ability,
efficient
exciton
dissociation,
desirable
optoelectronic
characteristics
beyond
those
constituents.
Essentially,
work
tandem
create
robust
built-in
allowing
steering
directional
electron
from
BCN
CNx.
Benefiting
these
merits,
BCN/CNx
nanohybrid
manifested
remarkable
CH4
generation
photocatalytic
CO2
reduction,
outperforming
its
CNx
counterparts
1.91
6.88-fold,
respectively.
midgap
states
induced
nitrogen
defects
also
pose
positive
effect
on
improved
photoactivity
binary
acting
reservoir
mediate
transfer
further
impede
recombination.
This
proof-of-concept
study
highlights
significance
flow
manipulation
utilization
enhancement.
Nano-Micro Letters,
Год журнала:
2023,
Номер
15(1)
Опубликована: Июль 11, 2023
Electrochemical
carbon
dioxide
reduction
reaction
(CO2RR)
provides
a
promising
way
to
convert
CO2
chemicals.
The
multicarbon
(C2+)
products,
especially
ethylene,
are
of
great
interest
due
their
versatile
industrial
applications.
However,
selectively
reducing
ethylene
is
still
challenging
as
the
additional
energy
required
for
C-C
coupling
step
results
in
large
overpotential
and
many
competing
products.
Nonetheless,
mechanistic
understanding
key
steps
preferred
pathways/conditions,
well
rational
design
novel
catalysts
production
have
been
regarded
approaches
achieving
highly
efficient
selective
CO2RR.
In
this
review,
we
first
illustrate
CO2RR
(e.g.,
adsorption/activation,
formation
*CO
intermediate,
step),
offering
conversion
ethylene.
Then
alternative
pathways
conditions
competitive
products
(C1
other
C2+
products)
investigated,
guiding
further
development
generation.
Engineering
strategies
Cu-based
CO2RR-ethylene
summarized,
correlations
mechanism/pathways,
engineering
selectivity
elaborated.
Finally,
major
challenges
perspectives
research
area
proposed
future
practical
Nano-Micro Letters,
Год журнала:
2023,
Номер
16(1)
Опубликована: Ноя. 6, 2023
We
report
a
novel
double-shelled
nanoboxes
photocatalyst
architecture
with
tailored
interfaces
that
accelerate
quantum
efficiency
for
photocatalytic
CO