The
scalable
artificial
photosynthesis
composed
of
photovoltaic
electrolysis
and
photothermal
catalysis
is
limited
by
inefficient
CO
2
hydrogenation
under
weak
sunlight
irradiation.
Herein,
NiO
nanosheets
supported
with
Ag
single
atoms
[two-dimensional
(2D)
Ni
1
0.02
O
]
are
synthesized
for
to
achieve
1065
mmol
g
−1
hour
production
rate
1-sun
This
performance
attributed
the
coupling
effect
Ag-O-Ni
sites
enhance
weaken
adsorption,
resulting
in
1434
yield
at
300°C.
Furthermore,
we
integrate
2D
-supported
reverse
water-gas
shift
reaction
commercial
electrolytic
water
splitting
construct
a
103-m
scale
system
(CO
+
H
→
),
which
achieves
more
than
22
m
3
/day
green
syngas
an
adjustable
/CO
ratio
(0.4-3)
photochemical
energy
conversion
efficiency
>17%.
research
charts
promising
course
designing
practical,
natural
sunlight–driven
systems.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
146(2), С. 1701 - 1709
Опубликована: Дек. 29, 2023
Mesoporous
materials
with
crystalline
frameworks
have
been
widely
explored
in
many
fields
due
to
their
unique
structure
and
feature,
but
accurate
manipulations
over
scaffolds,
mainly
composed
of
uncontrolled
polymorphs,
are
still
lacking.
Herein,
we
a
controlled
crystallization-driven
monomicelle
assembly
approach
construct
type
uniform
mesoporous
TiO2
particles
atomically
aligned
single-crystal
frameworks.
The
resultant
possess
an
angular
shape
∼80
nm
diameter,
good
mesoporosity
(a
high
surface
area
112
m2
g–1
mean
pore
size
at
8.3
nm),
highly
oriented
anatase
By
adjusting
the
evaporation
rate
during
assembly,
such
facile
solution-processed
strategy
further
enables
regulation
particle
mesopore
without
destruction
crystallites.
Such
combination
ordered
orientation
provides
both
effective
mass
charge
transportation,
leading
significant
increase
hydrogen
generation
rate.
A
maximum
evolution
12.5
mmol
h–1
can
be
realized,
along
great
stability
under
solar
light.
Our
study
is
envisaged
extend
possibility
single
crystal
growth
range
functional
ceramics
semiconductors
toward
advanced
applications.
How
to
collaboratively
reduce
Cr(VI)
and
break
Cr(III)
complexes
is
a
technical
challenge
solve
chromium-containing
wastewater
(CCW)
pollution.
Solar
photovoltaic
(SPV)
technology
based
on
semiconductor
materials
potential
strategy
this
issue.
Sb2
S3
typical
material
with
total
visible-light
harvesting
capacity,
but
its
large-sized
structure
highly
aggravates
disordered
photoexciton
migration,
accelerating
the
recombination
kinetics
resulting
low-efficient
photon
utilization.
Herein,
uniform
mesoporous
CdS
shell
in
situ
formed
surface
of
nanorods
(NRs)
construct
core-shell
@CdS
heterojunction
high
BET
area
excellent
near-infrared
light
capacity
via
cationic
displacement
strategy,
density
functional
theory
thermodynamically
explains
breaking
SbS
bonds
formation
CdS
according
bond
energy
calculation.
The
SbSCd
bonding
interaction
van
der
Waals
force
significantly
enhance
stability
synergy
/CdS
heterointerface
throughout
entire
NRs,
promoting
-to-CdS
electron
transfer
due
built-in
electric
field.
Therefore,
optimized
catalyst
achieves
enhanced
simulated
sunlight-driven
reduction
(0.154
min-1
)
decomplexation
complexed
weakly
acidic
condition,
effective
CCW
treatment
under
co-action
photoexcited
electrons
active
radicals.
This
study
provides
high-performance
heterostructured
for
by
SPV
technology.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(37)
Опубликована: Авг. 6, 2023
Abstract
Atomically
precise
composite
site‐based
catalysts
with
new
electrocatalytic
synergistic
mechanisms
and
enhanced
activities
have
emerged
as
a
frontier
in
the
electrocatalysis
community.
This
topical
review
focuses
on
recent
research
advances
of
atomically
metal
sites‐based
electrocatalysts.
work
first
demonstrates
an
overview
configurations
sites,
including
discussion
advanced
methods
employed
for
understanding
sites.
The
then
provides
comprehensive
organization
previously
reported
methodologies
synthesizing
electrocatalysts
Representative
case
studies
are
provided,
starting
from
simple
one‐step
pyrolysis
strategy
to
species‐by‐species
multi‐step
strategy.
Based
preceding
discussions
catalyst
materials,
further
discusses
unique
raised
by
that
different
routine
single
species
systems
mainly
involve
oxygen
reduction
reaction,
evolution
hydrogen
nitrogen
carbon
dioxide
reaction.
themes
this
section
include
true
active
center
determination
sites
various
types
synergy
mechanisms.
Finally,
critical
unanswered
questions
remaining
challenges,
well
promising
underexplored
directions
identified.
The
scalable
artificial
photosynthesis
composed
of
photovoltaic
electrolysis
and
photothermal
catalysis
is
limited
by
inefficient
CO
2
hydrogenation
under
weak
sunlight
irradiation.
Herein,
NiO
nanosheets
supported
with
Ag
single
atoms
[two-dimensional
(2D)
Ni
1
0.02
O
]
are
synthesized
for
to
achieve
1065
mmol
g
−1
hour
production
rate
1-sun
This
performance
attributed
the
coupling
effect
Ag-O-Ni
sites
enhance
weaken
adsorption,
resulting
in
1434
yield
at
300°C.
Furthermore,
we
integrate
2D
-supported
reverse
water-gas
shift
reaction
commercial
electrolytic
water
splitting
construct
a
103-m
scale
system
(CO
+
H
→
),
which
achieves
more
than
22
m
3
/day
green
syngas
an
adjustable
/CO
ratio
(0.4-3)
photochemical
energy
conversion
efficiency
>17%.
research
charts
promising
course
designing
practical,
natural
sunlight–driven
systems.