Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(34)
Published: June 18, 2022
Single-atom
active-site
catalysts
have
attracted
significant
attention
in
the
field
of
photocatalytic
CO2
conversion.
However,
designing
active
sites
for
reduction
and
H2
O
oxidation
simultaneously
on
a
photocatalyst
combining
corresponding
half-reaction
system
is
still
difficult.
Here,
we
synthesized
bimetallic
single-atom
with
two
compatible
centers
Mn
Co
carbon
nitride
(Mn1
Co1
/CN).
Our
experimental
results
density
functional
theory
calculations
showed
that
center
promotes
by
accumulating
photogenerated
holes.
In
addition,
activation
increasing
bond
length
angle
molecules.
Benefiting
from
synergistic
effect
atomic
centers,
Mn1
/CN
exhibited
CO
production
rate
47
μmol
g-1
h-1
,
which
significantly
higher
than
single-metal
photocatalyst.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
33(34)
Published: July 8, 2021
Atomically
dispersed
metal-based
electrocatalysts
have
attracted
increasing
attention
due
to
their
nearly
100%
atomic
utilization
and
excellent
catalytic
performance.
However,
current
fundamental
comprehension
summaries
reveal
the
underlying
relationship
between
single-atom
site
(SACs)
corresponding
application
are
rarely
reported.
Herein,
understandings
intrinsic
mechanisms
SACs
electrocatalytic
applications
systemically
summarized.
Different
preparation
strategies
presented
synthetic
with
engineering
well-defined
on
basis
of
theoretical
principle
(size
effect,
metal-support
interactions,
electronic
structure
coordination
environment
effect).
Then,
an
overview
is
presented,
including
oxygen
reduction
reaction,
hydrogen
evolution
oxidation
small
organic
molecules,
carbon
dioxide
nitrogen
reaction.
The
structure-performance
reactions
also
discussed
in
depth
expound
enhancement
mechanisms.
Finally,
a
summary
provided
perspective
supplied
demonstrate
challenges
opportunities
for
rational
designing,
synthesizing,
modulating
advanced
toward
reactions.
Energy & Environmental Science,
Journal Year:
2021,
Volume and Issue:
14(5), P. 2809 - 2858
Published: Jan. 1, 2021
Non-carbon
supported
SACs
were
classified
into
eight
categories
based
on
the
nature
of
their
substrates
for
first
time,
and
corresponding
anchoring
stabilization
mechanisms
have
been
systematically
summarized
discussed.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(15)
Published: Jan. 23, 2023
Abstract
Photocatalytic
water
splitting
and
carbon
dioxide
(CO
2
)
reduction
provide
promising
solutions
to
global
energy
environmental
issues.
In
recent
years,
metal‐organic
frameworks
(MOFs),
a
class
of
crystalline
porous
solids
featuring
well‐defined
tailorable
structures
as
well
high
surface
areas,
have
captured
great
interest
toward
photocatalytic
CO
reduction.
this
review,
the
semiconductor‐like
behavior
MOFs
is
first
discussed.
We
then
summarize
advances
in
over
MOF‐based
materials
focus
on
unique
advantage
for
clarifying
structure‐property
relationship
photocatalysis.
addition,
some
representative
characterization
techniques
been
presented
unveil
kinetics
reaction
intermediates
systems.
Finally,
challenges,
perspectives
future
directions
are
proposed.
Nature Communications,
Journal Year:
2022,
Volume and Issue:
13(1)
Published: March 17, 2022
Abstract
Direct
photocatalytic
CO
2
reduction
from
primary
sources,
such
as
flue
gas
and
air,
into
fuels,
is
highly
desired,
but
the
thermodynamically
favored
O
almost
completely
impedes
this
process.
Herein,
we
report
on
efficacy
of
a
composite
photocatalyst
prepared
by
hyper-crosslinking
porphyrin-based
polymers
hollow
TiO
surface
subsequent
coordinating
with
Pd(II).
Such
exhibits
high
resistance
against
inhibition,
leading
to
12%
conversion
yield
air
after
2-h
UV-visible
light
irradiation.
In
contrast,
over
Pd/TiO
without
polymer
severely
inhibited
presence
(
≥
0.2
%).
This
study
presents
feasible
strategy,
building
Pd(II)
sites
-adsorptive
surface,
for
realizing
H
in
an
aerobic
environment
/O
adsorption
selectivity
efficient
charge
separation
oxidation
,
respectively.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(40)
Published: Aug. 15, 2022
The
light-driven
CO2
reduction
to
multi-carbon
products
is
especially
meaningful,
while
the
low
efficiency
of
multi-electron
transfer
and
sluggish
C-C
coupling
greatly
hinder
its
development.
Herein,
we
report
a
photocatalyst
comprising
P
Cu
dual
sites
anchored
on
graphitic
carbon
nitride
(P/Cu
SAs@CN),
which
achieves
high
C2
H6
evolution
rate
616.6
μmol
g-1
h-1
in
reducing
hydrocarbons.
detailed
spectroscopic
characterizations
identify
formation
charge-enriched
sites,
where
isolated
atoms
serve
as
hole
capture
during
photocatalysis.
Theoretical
simulations
combined
with
situ
FTIR
measurement
reveal
kinetically
feasible
process
for
intermediate
(*OC-COH)
confirm
favorable
production
P/Cu
SAs@CN
photocatalyst.
This
work
offers
new
insights
into
design
atomic
precision
toward
highly
efficient
photocatalytic
conversion
value-added
products.
Advanced Materials,
Journal Year:
2021,
Volume and Issue:
33(32)
Published: May 29, 2021
With
the
capability
of
inducing
intense
electromagnetic
field,
energetic
charge
carriers,
and
photothermal
effect,
plasmonic
metals
provide
a
unique
opportunity
for
efficient
light
utilization
chemical
transformation.
Earth-abundant
low-cost
Cu
possesses
tunable
localized
surface
plasmon
resonance
from
ultraviolet-visible
to
near
infrared
region.
Moreover,
essentially
exhibits
remarkable
catalytic
performance
toward
various
reactions
owing
its
intriguing
physical
properties.
Coupling
with
light-harvesting
ability
function,
serves
as
promising
platform
light-driven
reaction.
Herein,
recent
advancements
Cu-based
photocatalysis
are
systematically
summarized,
including
designing
synthetic
strategies
catalysts,
performance,
mechanistic
understanding
over
catalysts.
What's
more,
approaches
enhancement
efficiency
construction
active
centers
on
catalysts
highlighted
discussed
in
detail,
such
morphology
size
control,
regulation
electronic
structure,
defect
strain
engineering,
etc.
Remaining
challenges
future
perspectives
further
development
catalysis
also
proposed.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(40)
Published: Aug. 10, 2022
Photoreduction
of
CO2
to
C2+
solar
fuel
is
a
promising
carbon-neutral
technology
for
renewable
energy.
This
strategy
challenged
by
its
low
productivity
due
efficiency
in
multielectron
utilization
and
slow
C-C
coupling
kinetics.
work
reports
dual-metal
photocatalyst
consisting
atomically
dispersed
indium
copper
anchored
on
polymeric
carbon
nitride
(InCu/PCN),
which
the
photoreduction
delivered
an
excellent
ethanol
production
rate
28.5
μmol
g-1
h-1
with
high
selectivity
92
%.
Coupled
experimental
investigation
DFT
calculations
reveal
following
mechanisms
underpinning
performance
this
catalyst.
Essentially,
In-Cu
interaction
enhances
charge
separation
accelerating
transfer
from
PCN
metal
sites.
Indium
also
transfers
electrons
neighboring
via
Cu-N-In
bridges,
increasing
electron
density
active
Furthermore,
sites
promote
adsorption
*CO
intermediates
lower
energy
barrier
coupling.