Inorganic Chemistry Frontiers,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 18, 2024
ZnCdS
2
/NiMoO
4
@Cu
Z-scheme
heterojunctions
exhibit
outstanding
activity
and
nearly
100%
selectivity
for
photocatalytic
CO
reduction
to
CH
under
the
combined
effects
of
surface
defects,
heterojunction
photothermal
properties.
Advanced Materials,
Год журнала:
2024,
Номер
36(30)
Опубликована: Июнь 14, 2024
Abstract
Urea
electrosynthesis
from
co–electrolysis
of
NO
3
−
and
CO
2
(UENC)
offers
a
promising
technology
for
achieving
sustainable
efficient
urea
production.
Herein,
diatomic
alloy
catalyst
(CuPd
1
Rh
–DAA),
with
mutually
isolated
Pd
atoms
alloyed
on
Cu
substrate,
is
theoretically
designed
experimentally
confirmed
to
be
highly
active
selective
UENC
catalyst.
Combining
theoretical
computations
operando
spectroscopic
characterizations
reveals
the
synergistic
effect
–Cu
sites
promote
via
tandem
catalysis
mechanism,
where
site
triggers
early
C–N
coupling
promotes
*CO
–to–*CO
NH
steps,
while
facilitates
subsequent
protonation
step
*COOHNH
toward
formation.
Impressively,
CuPd
–DAA
assembled
in
flow
cell
presents
highest
Faradaic
efficiency
72.1%
yield
rate
53.2
mmol
h
−1
g
cat
at
−0.5
V
versus
RHE,
representing
nearly
performance
among
all
reported
catalysts.
Electrocatalytic
CO2
reduction
into
high-value
multicarbon
products
offers
a
sustainable
approach
to
closing
the
anthropogenic
carbon
cycle
and
contributing
neutrality,
particularly
when
renewable
electricity
is
used
power
reaction.
However,
lack
of
efficient
durable
electrocatalysts
with
high
selectivity
for
multicarbons
severely
hinders
practical
application
this
promising
technology.
Herein,
nanoporous
defective
Au1Cu
single-atom
alloy
(De-Au1Cu
SAA)
catalyst
developed
through
facile
low-temperature
thermal
in
hydrogen
subsequent
dealloying
process,
which
shows
toward
ethylene
(C2H4),
Faradaic
efficiency
52%
at
current
density
252
mA
cm–2
under
potential
−1.1
V
versus
reversible
electrode
(RHE).
In
situ
spectroscopy
measurements
functional
theory
(DFT)
calculations
reveal
that
C2H4
product
results
from
synergistic
effect
between
Au
single
atoms
Cu
sites
on
surface
catalysts,
where
promote
*CO
generation
defects
stabilize
key
intermediate
*OCCO,
altogether
enhances
C–C
coupling
kinetics.
This
work
provides
important
insights
design
electrochemical
products.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 26, 2025
Abstract
Electrochemical
oxidation
of
small
molecules
shows
great
promise
to
substitute
oxygen
evolution
reaction
(OER)
or
hydrogen
(HOR)
enhance
kinetics
and
reduce
energy
consumption,
as
well
produce
high‐valued
chemicals
serve
fuels.
For
these
reactions,
high‐valence
metal
sites
generated
at
oxidative
potentials
are
typically
considered
active
trigger
the
process
molecules.
Isolated
atom
site
catalysts
(IASCs)
have
been
developed
an
ideal
system
precisely
regulate
state
coordination
environment
single‐metal
centers,
thus
optimize
their
catalytic
property.
The
isolated
in
IASCs
inherently
possess
a
positive
state,
can
be
more
readily
homogeneous
under
than
nanoparticle
counterparts.
Meanwhile,
merely
centers
but
lack
ensemble
sites,
which
alter
adsorption
configurations
compared
with
counterparts,
induce
various
pathways
mechanisms
change
product
selectivity.
More
importantly,
construction
is
discovered
limit
d‐electron
back
donation
CO
2p
*
orbital
overly
strong
on
resolve
poisoning
problems
most
electro‐oxidation
reactions
improve
stability.
Based
advantages
fields
electrochemical
molecules,
this
review
summarizes
recent
developments
advancements
focusing
anodic
HOR
fuel
cells
OER
electrolytic
alternative
such
formic
acid/methanol/ethanol/glycerol/urea/5‐hydroxymethylfurfural
(HMF)
key
reactions.
merits
different
decoding
structure–activity
relationships
specifically
discussed
guide
precise
design
structural
regulation
from
perspective
comprehensive
mechanism.
Finally,
future
prospects
challenges
put
forward,
aiming
motivate
application
possibilities
for
diverse
functional
IASCs.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(44)
Опубликована: Июль 26, 2024
Abstract
The
C−C
coupling
of
methane
(CH
4
)
and
carbon
dioxide
(CO
2
to
generate
acetic
acid
3
COOH)
represents
a
highly
atom‐efficient
chemical
conversion,
fostering
the
comprehensive
utilization
greenhouse
gases.
However,
inherent
thermodynamic
stability
kinetic
inertness
CH
CO
present
obstacles
achieving
efficient
selective
conversion
at
room
temperature.
Our
study
reveals
that
hydroxyl
radicals
(⋅OH)
hydrated
electrons
(e
aq
−
produced
by
water
radiolysis
can
effectively
activate
,
yielding
methyl
(⋅CH
radical
anions(⋅CO
facilitate
production
COOH
ambient
introduction
radiation‐synthesized
CuO‐anchored
TiO
bifunctional
catalyst
could
further
enhance
reaction
efficiency
selectivity
remarkably
boosting
radiation
absorption
stability,
resulting
in
concentration
7.1
mmol
⋅
L
−1
with
near‐unity
(>95
%).
These
findings
offer
valuable
insights
for
design
implementation
radiation‐induced
conversion.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
unknown
Опубликована: Янв. 1, 2024
This
manuscript
comprehensively
reviews
the
recent
advancements
in
Cu-based
atomic
site
catalysts
NO
3
RR,
following
a
sequential
order
with
six
sections:
Introduction,
Mechanism,
SACs,
SAAs,
DACs,
and
Perspectives.
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.
Industrial Chemistry and Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
Building
a
sustainable
energy
system
is
currently
major
challenge.
In
this
review,
we
introduce
catalysis
of
promising
systems,
aiming
to
draw
attention
development
in
energy.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 20, 2025
Abstract
Recently,
dual‐atom
alloy
(DAA,
also
named
diatomic
alloy)
catalysts
with
active
metal
dimers
supported
by
a
less
host
have
attracted
considerable
interest
owing
to
their
distinctive
geometric
and
electrical
configurations.
Despite
developing
many
ways
for
synthesizing
DAA
catalysts,
most
contemporary
methods
depend
on
high‐temperature
pyrolysis,
costly
apparatus,
intricate
procedures.
This
study
presents,
the
first
time,
one‐step
laser
solid‐phase
synthesis
of
(PtRu)
1
Co
DAAs
low‐defect
graphene
support
via
ultraviolet
(UV)
irradiation
mixed
precursors
ZIF‐67@PBI
composite
support.
The
special
structure
enhances
catalytic
performance
hydrogen
evolution
reaction
(HER)
in
an
alkaline
solution.
An
overpotential
27
mV
is
reached
at
current
density
‐10
mA
cm⁻
2
.
mass
activity
200
19.6
times
more
than
that
commercial
Pt/C
catalyst.
Moreover,
sustained
stability
over
100
h
‐200
cm
−2
results
demonstrated
potential
as
viable
method
precise
controlling
defect
formations
nanoparticles
carbon
technique
rapid
cost‐effective
opens
up
new
avenue
toward
large‐scale
catalysts.