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 Functional Materials,
Journal Year:
2021,
Volume and Issue:
31(37)
Published: June 26, 2021
Abstract
Photocatalysis
is
considered
to
be
a
green
and
environment‐friendly
technology
since
it
can
convert
solar
energy
into
other
types
of
chemical
energies.
Over
the
past
several
years,
metal‐organic
frameworks
(MOFs)‐based
photocatalysts
have
received
remarkable
research
interest
due
their
unique
morphology,
high
photocatalytic
performance,
good
stability,
easy
synthesis,
low
cost.
In
this
review,
synthetic
strategies
developing
MOFs‐based
are
first
introduced.
Second,
recent
progress
in
fabrication
various
MOFs
composites
summarized.
Third,
different
applications
including
hydrogen
evolution
reaction,
oxygen
overall
water
splitting,
nitrogen
reduction
carbon
dioxide
reaction
as
well
photodegradation
organic
pollutants
summed
up.
Finally,
challenges
some
suggestions
for
future
development
MOFs‐
composites‐based
also
highlighted.
It
expected
that
report
will
help
researchers
systematically
devise
develop
highly
efficient
based
on
composites.
Joule,
Journal Year:
2022,
Volume and Issue:
6(1), P. 92 - 133
Published: Jan. 1, 2022
Artificial
photocatalytic
energy
conversion
represents
a
highly
intriguing
strategy
for
solving
the
crisis
and
environmental
problems
by
directly
harvesting
solar
energy.
The
development
of
efficient
photocatalysts
is
central
task
pushing
real-world
application
reactions.
Due
to
maximum
atomic
utilization
efficiency
distinct
advantages
outstanding
catalytic
activity,
single-atom
catalysts
(SACs)
have
emerged
as
promising
candidates
photocatalysts.
In
current
review,
recent
progresses
challenges
on
SACs
systems
are
presented.
Fundamental
principles
focusing
charge
separation/transfer
molecular
adsorption/activation
photocatalysis
systemically
explored.
We
outline
how
isolated
reactive
sites
facilitate
photogenerated
electron–hole
transfer
promote
construction
photoactivation
cycles.
widespread
adoption
in
diverse
reactions
also
comprehensively
introduced.
By
presenting
these
advances
addressing
some
future
with
potential
solutions
related
integral
over
SACs,
we
expect
shed
light
forthcoming
research
conversion.
Advanced Powder Materials,
Journal Year:
2021,
Volume and Issue:
1(1), P. 100013 - 100013
Published: Nov. 15, 2021
Various
metal-based
electrocatalysts
from
nanocrystals,
to
clusters
and
single-atoms,
have
been
well-discovered
towards
high-efficient
power
devices
electrocatalytic
conversion.
To
accelerate
energy
transformation
materials
discovery,
developing
high-throughput
DFT
calculations
machine-learning
techniques
is
of
great
necessity.
This
review
comprehensively
outlines
the
latest
progress
theory-guided
design
advanced
materials.
Especially,
we
focus
on
study
single
atoms
in
various
devices,
such
as
fuel
cell
(oxygen
reduction
reaction,
ORR;
acid
oxidation
reaction;
alcohol
reaction),
other
reactions
for
energy-related
conversion
small
molecules,
H2O2
evolution
(2e−
ORR),
water
splitting
(H2
reaction/O2
HER/OER),
N2
reaction
(NRR),
CO2
(CO2RR).
Firstly,
electronic
structure,
interaction
mechanism,
activation
path
are
discussed
provide
an
overall
blueprint
electrocatalysis
batteries
mentioned
above.
Thereafter,
experimental
synthesis
strategies,
structural
recognition,
performance
figured
out.
Finally,
some
viewpoints
into
current
issues
future
concept
provided.
Journal of the American Chemical Society,
Journal Year:
2021,
Volume and Issue:
143(7), P. 2984 - 2993
Published: Feb. 11, 2021
To
realize
the
evolution
of
C2+
hydrocarbons
like
C2H4
from
CO2
reduction
in
photocatalytic
systems
remains
a
great
challenge,
owing
to
gap
between
relatively
lower
efficiency
multielectron
transfer
photocatalysis
and
sluggish
kinetics
C–C
coupling.
Herein,
with
Cu-doped
zeolitic
imidazolate
framework-8
(ZIF-8)
as
precursor,
hybrid
photocatalyst
(CuOX@p-ZnO)
CuOX
uniformly
dispersed
among
polycrystalline
ZnO
was
synthesized.
Upon
illumination,
catalyst
exhibited
ability
reduce
32.9%
selectivity,
rate
2.7
μmol·g–1·h–1
water
hole
scavenger
high
22.3
presence
triethylamine
sacrificial
agent,
all
which
have
rarely
been
achieved
systems.
The
X-ray
absorption
fine
structure
spectra
coupled
situ
FT-IR
studies
reveal
that,
original
catalyst,
Cu
mainly
existed
form
CuO,
while
unique
Cu+
surface
layer
upon
CuO
matrix
formed
during
reaction,
this
site
is
active
anchor
generated
CO
further
perform
coupling
C2H4.
intermediate
*OC–COH
experimentally
identified
by
for
first
time
reduction.
Moreover,
theoretical
calculations
showed
critical
role
such
sites
strengthening
binding
*CO
stabilizing
intermediate.
This
work
uncovers
new
paradigm
achieve
system.
Nature Communications,
Journal Year:
2022,
Volume and Issue:
13(1)
Published: Jan. 10, 2022
Abstract
Single-atom
catalysts
anchoring
offers
a
desirable
pathway
for
efficiency
maximization
and
cost-saving
photocatalytic
hydrogen
evolution.
However,
the
single-atoms
loading
amount
is
always
within
0.5%
in
most
of
reported
due
to
agglomeration
at
higher
concentrations.
In
this
work,
highly
dispersed
large
(>1
wt%)
copper
were
achieved
on
TiO
2
,
exhibiting
H
evolution
rate
101.7
mmol
g
−1
h
under
simulated
solar
light
irradiation,
which
than
other
photocatalysts
reported,
addition
excellent
stability
as
proved
after
storing
380
days.
More
importantly,
it
exhibits
an
apparent
quantum
56%
365
nm,
significant
breakthrough
field.
The
Cu
incorporation
enables
efficient
electron
transfer
via
2+
-Cu
+
process.
present
approach
paves
way
design
advanced
materials
remarkable
activity
durability.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
34(30)
Published: March 3, 2022
Abstract
Although
lithium–sulfur
(Li–S)
batteries
are
promising
next‐generation
energy‐storage
systems,
their
practical
applications
limited
by
the
growth
of
Li
dendrites
and
lithium
polysulfide
shuttling.
These
problems
can
be
mitigated
through
use
single‐atom
catalysts
(SACs),
which
exhibit
advantages
maximal
atom
utilization
efficiency
(≈100%)
unique
catalytic
properties,
thus
effectively
enhancing
performance
electrode
materials
in
devices.
This
review
systematically
summarizes
recent
progress
SACs
intended
for
Li‐metal
anodes,
S
cathodes,
separators,
briefly
introducing
operating
principles
Li–S
batteries,
action
mechanisms
corresponding
SACs,
fundamentals
activity,
then
comprehensively
describes
main
strategies
synthesis.
Subsequently,
operation
reinforced
as
well
other
metal–S
individually
illustrated,
major
challenges
usage
future
development
directions
presented.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(37), P. 17097 - 17109
Published: Sept. 6, 2022
Solar
carbon
dioxide
(CO2)
conversion
is
an
emerging
solution
to
meet
the
challenges
of
sustainable
energy
systems
and
environmental/climate
concerns.
However,
construction
isolated
active
sites
not
only
influences
catalytic
activity
but
also
limits
understanding
structure-catalyst
relationship
CO2
reduction.
Herein,
we
develop
a
universal
synthetic
protocol
fabricate
different
single-atom
metal
(e.g.,
Fe,
Co,
Ni,
Zn,
Cu,
Mn,
Ru)
anchored
on
triazine-based
covalent
organic
framework
(SAS/Tr-COF)
backbone
with
bridging
structure
metal-nitrogen-chlorine
for
high-performance
Remarkably,
as-synthesized
Fe
SAS/Tr-COF
as
representative
catalyst
achieved
impressive
CO
generation
rate
high
980.3
μmol
g-1
h-1
selectivity
96.4%,
over
approximately
26
times
higher
than
that
pristine
Tr-COF
under
visible
light
irradiation.
From
X-ray
absorption
fine
analysis
density
functional
theory
calculations,
superior
photocatalytic
performance
attributed
synergic
effect
atomically
dispersed
host,
decreasing
reaction
barriers
formation
*COOH
intermediates
promoting
adsorption
activation
well
desorption.
This
work
affords
rational
design
state-of-the-art
catalysts
at
molecular
level
provides
in-depth
insights
efficient
conversion.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
61(15)
Published: Dec. 17, 2021
Green
carbon
science
is
defined
as
the
"study
and
optimization
of
transformation
carbon-containing
compounds
relevant
processes
involved
in
entire
cycle
from
resource
processing,
energy
utilization,
CO2
fixation,
recycling
to
utilize
resources
efficiently
minimize
net
emission."[1]
related
closely
neutrality,
fields
have
developed
quickly
last
decade.
In
this
Minireview,
we
propose
concept
index,
recent
progress
petroleum
refining,
production
liquid
fuels,
chemicals,
materials
using
coal,
methane,
,
biomass,
waste
plastics
highlighted
combination
with
green
science.
An
outlook
for
these
important
provided
final
section.