Dilute
alloy
(DA)
catalysts,
including
single-atom
alloys
(SAAs),
which
are
comprised
of
trace
amounts
an
active
promoter
metal
dispersed
on
the
surface
a
selective
host
metal,
offer
exceptional
activity
and
selectivity
while
utilizing
precious
metals
more
efficiently.
Although
most
SAA
DA
applications
have
focused
partial
hydrogenation
oxidation
reactions,
their
use
has
steadily
expanded
into
complex
thermo-,
photo-,
electro-catalytic
processes.
This
progress
been
largely
driven
by
mechanistic
insights
derived
from
computational
chemistry
is
expected
to
accelerate
with
advancement
artificial
intelligence.
minireview
discusses
novel
advances
in
simulating
SAAs
DAs
for
catalysis
applications,
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(13)
Опубликована: Янв. 16, 2024
Abstract
Activation
of
ubiquitous
C(sp
3
)−H
bonds
is
extremely
attractive
but
remains
a
great
challenge.
Heterogeneous
photocatalysis
offers
promising
and
sustainable
approach
for
activation
has
been
fast
developing
in
the
past
decade.
This
Minireview
focuses
on
mechanism
strategies
heterogeneous
photocatalytic
activation.
After
introducing
mechanistic
insights,
including
precise
design
active
sites,
regulation
reactive
radical
species,
improving
charge
separation
reactor
innovations
are
discussed.
In
addition,
recent
advances
hydrocarbons,
alcohols,
ethers,
amines
amides
by
summarized.
Lastly,
challenges
opportunities
outlined
to
encourage
more
efforts
development
this
exciting
field.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 10, 2024
In
the
context
of
reshaping
energy
pattern,
designing
and
synthesizing
high-performance
noble
metal-free
photocatalysts
with
ultra-high
atomic
utilization
for
hydrogen
evolution
reaction
(HER)
still
remains
a
challenge.
streamlined
synthesis
process,
in-situ
single
atom
anchoring
is
performed
in
parallel
HER
by
irradiating
precursory
defect-state
CdS/Co
suspension
(Co-DCdS-Ss)
system
under
simulated
sunlight
single-atom
Co
photocatalyst
(Co5:DCdS)
exhibits
further
improved
catalytic
performance
(60.10
mmol
g
Abstract
Carbon
recycling
is
poised
to
emerge
as
a
prominent
trend
for
mitigating
severe
climate
change
and
meeting
the
rising
demand
energy.
Converting
carbon
dioxide
(CO
2
)
into
green
energy
valuable
feedstocks
through
photocatalytic
CO
reduction
(PCCR)
offers
promising
solution
global
warming
needs.
Among
all
semiconductors,
zinc
oxide
(ZnO)
has
garnered
considerable
interest
due
its
ecofriendly
nature,
biocompatibility,
abundance,
exceptional
semiconducting
optical
properties,
cost‐effectiveness,
easy
synthesis,
durability.
This
review
thoroughly
discusses
recent
advances
in
mechanistic
insights,
fundamental
principles,
experimental
parameters,
modulation
of
ZnO
catalysts
direct
PCCR
C
1
products
(methanol).
Various
modification
techniques
are
explored,
including
atomic
size
regulation,
synthesis
strategies,
morphology
manipulation,
doping
with
cocatalysts,
defect
engineering,
incorporation
plasmonic
metals,
single
atom
boost
performance.
Additionally,
highlights
importance
photoreactor
design,
reactor
types,
geometries,
operating
modes,
phases.
Future
research
endeavors
should
prioritize
development
cost‐effective
catalyst
immobilization
methods
solid‐liquid
separation
recycling,
while
emphasizing
use
abundant
non‐toxic
materials
ensure
environmental
sustainability
economic
viability.
Finally,
outlines
key
challenges
proposes
novel
directions
further
enhancing
ZnO‐based
conversion
processes.
Abstract
Photocatalytic
oxidative
coupling
of
CH
4
(OCM)
is
a
promising
conversion
process
that
can
achieve
efficient
methane
with
the
assistance
O
2
.
It
remains
to
be
highly
challenging
improve
photocatalytic
OCM
activity
from
catalyst
design
and
deepen
understanding
reactant
activation
in
process.
In
this
work,
Au‐loaded
ZnAl‐layered
double
hydroxides
(LDHs)
without
oxygen
vacancy
are
constructed
(denoted
as
Au/ZnAl
Au/ZnAl‐v),
respectively.
When
applied
for
OCM,
Au/ZnAl‐v
shows
rate
8.5
mmol
g
−1
h
92%
selectivity
C
H
6
at
40
°C,
outperforming
most
reported
systems
low
temperature
literature.
Furthermore,
catalytic
performance
stable
100
h.
contrast,
An/ZnAl
exhibits
0.8
46%
Detailed
characterizations
DFT
calculation
studies
reveal
introduced
Ov
sites
on
able
activate
,
resulting
superoxide
radical
·
−
greatly
promotes
The
3
groups
Au
cocatalyst
leads
formation
high
activity.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Ноя. 15, 2024
Photocatalytic
oxidative
coupling
of
methane
with
oxygen
is
promising
to
obtain
valuable
muti-carbon
products,
yet
suffering
low
reactivity.
Here,
we
apply
cerium
modifications
on
zinc
oxide-supported
gold
catalysts
based
the
electronic
asymmetry
design
lattice
improve
activity.
The
conversion
rate
exceeds
16000
μmol
g−1
h−1
selectivity
94.9%
and
catalytic
durability
3
days,
it
can
increase
34000
under
more
thermal
assistance,
a
turnover
frequency
507
for
ethane
an
apparent
quantum
efficiency
33.7%
at
350
nm.
According
systematic
characterizations
theoretical
analysis,
dopants
not
only
boost
formation
reactive
species
but
also
intervene
in
vivacity
by
manipulating
metal-oxygen
bond
strength,
thereby
leading
favorable
methyl
desorption
form
quick
water
release.
This
work
provides
insight
into
rational
efficient
photocatalysts
aerobic
methane-to-ethane
conversion.
approach
create
products.
authors
use
Ce
construct
electronically
asymmetric
sites
ZnO
enhance
migration
promote
C-C
coupling.
ACS Catalysis,
Год журнала:
2024,
Номер
14(17), С. 13520 - 13530
Опубликована: Авг. 27, 2024
Valorization
of
nitrous
oxide
(N2O)
as
a
mild
oxygen
source
for
light
alkanes
presents
promising
and
economical
method
mitigating
global
warming.
However,
activating
N2O
alkane
together
often
leads
to
overoxidation
poor
selectivity
the
products.
To
disentangle
trade-off
between
activity
selectivity,
herein,
an
Ir-based
hexagonal
boron
nitride
(hBN)
catalyst
was
synthesized
obtain
reversed
charge
transfer
(RCT)
from
support
metal
centers,
forming
dual
active
sites
on
Ir
clusters
separation
redox
determined
via
operando
near-ambient-pressure
X-ray
photoelectron
spectroscopy
(NAP-XPS)
density
functional
theory
(DFT)
calculations.
Ir/hBN
demonstrated
high
conversion
(99.5%)
syngas
yield
(95.9
mol
CO
kgcat–1
h–1
41.9
H2
h–1)
during
selective
oxidation
propane
(C3H8)
at
450
°C.
The
electron-rich
interfacial
perimeter
(Irδ−)
enhance
adsorption
N–O
bond
dissociation
produce
O*;
however,
facial
metallic
Ir0
effectively
facilitate
C3H8
activation,
including
dehydrogenation
cracking.
H*
O*
intermediates,
along
with
frustrated
H*/O*
spillover,
facilitates
formation
H2.
*CH2
intermediate
breakage
migrates
reacts
bound
sites,
where
it
is
oxidized
CO32–
subsequently
liberates
CO.
This
study
provides
mechanistic
insights
into
O
element
valorization
synergetic
enhancement
in
alkanes.
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(20), С. 7649 - 7680
Опубликована: Янв. 1, 2024
This
review
explores
the
role
of
atomic
metal
site
cocatalysts
in
photocatalysis
for
solar
energy
conversion,
focusing
on
recent
advances
single-atom
and
cluster
cocatalysts,
their
structure–activity
relationships,
key
applications.
Dalton Transactions,
Год журнала:
2024,
Номер
53(8), С. 3797 - 3807
Опубликована: Янв. 1, 2024
A
novel
Ag
coordination
polymer
(Ag-TIPA)
was
rationally
designed,
successfully
prepared
and
used
for
the
photodegradation
of
ciprofloxacin
nitrophenol,
showing
excellent
photocatalytic
performance
high
reusability.
