Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 5, 2024
Abstract
Direct
and
selective
catalytic
oxidative
coupling
of
methane
(OCM)
into
high‐carbon
products
is
a
great
challenge
in
C1
chemistry.
Herein,
the
successful
fabrication
series
Au
clusters
loaded
on
different
MgO
facets
(111),
(110),
(100)
reported.
This
work
demonstrates
Au‐loaded
MgO(111)
(denoted
as
Au/MgO(111))
shows
highest
C
2
H
6
yield
12733.4
µmol
g
−1
h
selectivity
90.4%,
which
2.46
times
higher
than
that
Au/MgO(110)
(5171.4
)
25.14
Au/MgO(100)
(506.4
).
Moreover,
high
activity
Au/MgO(111)
can
be
well
maintained
over
100
h.
Detailed
situ
experiments
theoretical
calculation
reveal
such
performance
attributed
to
1)
strong
electronic
affinity
surface
oxygen
species
polar
CH
4
with
lowest
adsorption
energy
−0.82
eV;
2)
ΔE
RDS
0.53
eV
rate‐deterime
step
OCM
comes
activating
second
molecule;
3)
act
hole
acceptor
under
light
irradiation
adsorb
*CH
3
d‐σ
hybridization,
resulting
an
increased
selectivity.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 2, 2025
Abstract
Catalysis
remains
a
cornerstone
of
chemical
research,
with
the
active
sites
catalysts
being
crucial
for
their
functionality.
Identifying
sites,
particularly
during
reaction
process,
is
elucidating
relationship
between
catalyst's
structure
and
its
catalytic
property.
However,
dynamic
evolution
within
heterogeneous
metal
presents
substantial
challenge
accurately
pinpointing
real
sites.
The
advent
in
situ
operando
characterization
techniques
has
illuminated
path
toward
understanding
changes
offering
robust
scientific
evidence
to
support
rational
design
catalysts.
There
pressing
need
comprehensive
review
that
systematically
explores
among
single
atoms,
clusters,
nanoparticles
as
utilizing
techniques.
This
aims
delineate
effects
various
factors
on
nanoparticles.
Moreover,
several
are
elaborated
emphases
tracking
linking
them
properties.
Finally,
it
discusses
challenges
future
perspectives
identifying
process
advancing
Abstract
Single‐atom
catalysts
(SACs)
are
a
class
of
with
low
dosage,
cost,
and
the
presence
metal
atom‐carrier
interactions
high
catalytic
activity,
which
considered
to
possess
significant
potential
in
field
electrocatalysis.
The
most
important
aspect
synthesis
SACs
is
selection
suitable
carriers.
Metal
carbides,
nitrides,
or
carbon‐nitrides
(MXenes)
widely
used
as
new
type
2D
materials
good
electrical
conductivity
tunable
surface
properties.
abundance
functional
groups
vacancy
defects
on
MXenes
an
ideal
anchoring
site
for
single
atoms
therefore
regarded
carrier
single‐atom
loading.
In
this
work,
preparation
method
MXenes,
loading
mode
SACs,
characterization
catalysts,
electrochemical
performance
described
detail,
some
hot
issues
current
research
future
directions
also
summarized.
aim
work
promote
development
MXene‐based
within
realm
With
ongoing
innovation,
these
expected
be
crucial
energy
conversion
storage
solutions.
Environmental Science & Technology,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 6, 2025
As
primary
air
pollutants
from
fossil
fuel
combustion,
the
excess
emission
of
nitric
oxides
(NOx)
results
in
a
series
atmospheric
environmental
issues.
Although
selective
catalytic
reduction
technology
has
been
confirmed
to
be
effective
for
NOx
removal,
green
purification
and
value-added
conversion
under
ambient
conditions
are
still
facing
great
challenges,
especially
nitrogen
resource
recovery.
To
address
that,
photo-/electrocatalysis
offers
sustainable
routes
efficient
upcycling
temperature
pressure,
which
received
considerable
attention
scientific
communities.
In
this
review,
recent
advances
critically
summarized.
The
target
products
reaction
mechanisms
systems,
together
with
responsible
active
sites,
discussed,
respectively.
Then,
realistic
practicability
is
proposed,
including
strict
performance
evaluation
criteria
application
by
photo-/electrocatalysis.
Finally,
current
challenges
future
opportunities
proposed
terms
catalyst
design,
enhancement,
mechanism
understanding,
practical
conditions,
product
separation
techniques.
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.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 18, 2024
Abstract
For
traditional
metal
complexes,
intricate
chemistry
is
required
to
acquire
appropriate
ligands
for
controlling
the
electron
and
steric
hindrance
of
active
centers.
Comparatively,
preparation
single‐atom
catalysts
much
easier
with
more
straightforward
effective
accesses
arrangement
control
The
presence
coordination
atoms
or
neighboring
functional
on
supports'
surface
ensures
stability
single‐atoms
their
interactions
individual
substantially
regulate
performance
Therefore,
collaborative
interaction
between
surrounding
environment
enhances
initiation
reaction
substrates
formation
transformation
crucial
intermediate
compounds,
which
imparts
significant
catalytic
efficacy,
rendering
them
a
valuable
framework
investigating
correlation
structure
activity,
as
well
mechanism
in
organic
reactions.
Herein,
comprehensive
overviews
both
homogeneous
complexes
reactions
are
provided.
Additionally,
reflective
conjectures
about
advancement
synthesis
also
proposed
present
reference
later
development.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 4, 2024
Abstract
Photoelectrochemical
(PEC)
water
splitting
for
hydrogen
generation
holds
immense
potential
addressing
environmental
and
energy
crises.
Tailoring
non‐covalent
interaction
via
a
single
atom
is
anticipated
to
realize
prominent
hole
extracting
facilitating
PEC
performance,
but
it
has
never
been
reported.
In
this
study,
Co‐N
4
coordinated
with
5‐fluoroanthranilic
acid
(FAA)
molecules,
then
used
as
hole‐extracting
layer
on
BiVO
substrate.
Experiments
including
X‐ray
absorption
fine
spectra,
Kelvin
probe
force
microscopy,
transient
absorption,
theoretical
calculation
demonstrate
the
FAA
coordination
alters
local
configuration
of
central
Co
atom,
adjusting
interfacial
interaction,
thereby
reducing
barrier
charge
transfer
between
layer.
Consequently,
photogenerated
carriers
are
more
effectively
separated,
oxidation
performance
significantly
enhanced
photocurrent
density
5.47
mA
cm
−2
at
1.23
V
versus
RHE,
much
higher
than
those
previously
reported
photoanodes
composited
porphyrin‐based
compounds.
simulation
confirm
that
boosted
originates
from
exceptional
rather
surface
catalysis
dynamic.
This
study
provides
an
efficient
strategy
tailoring
by
regulating
single‐atom
promoting
extract
boost
activity.
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.
Nature Communications,
Год журнала:
2025,
Номер
16(1)
Опубликована: Янв. 28, 2025
Abstract
Artificial
photosynthesis
of
urea
from
NH
3
and
CO
2
seems
to
remain
still
essentially
unexplored.
Herein,
three
isomorphic
three-dimensional
covalent
organic
frameworks
with
twofold
interpenetrated
ffc
topology
are
functionalized
by
benzene,
pyrazine,
tetrazine
active
moieties,
respectively.
A
series
experiment
results
disclose
the
gradually
enhanced
conductivity,
light-harvesting
capacity,
photogenerated
carrier
separation
efficiency,
co-adsorption
capacity
towards
in
order
benzene-,
pyrazine-,
tetrazine-containing
framework.
This
turn
endows
framework
superior
photocatalytic
activity
production
yield
523
μmol
g
−1
h
,
40
4
times
higher
than
that
for
benzene-
pyrazine-containing
framework,
respectively,
indicating
heterocyclic
N
microenvironment-dependent
catalytic
performance
these
photocatalysts.
is
further
confirmed
in-situ
spectroscopic
characterization
density
functional
theory
calculations.
work
lays
a
way
sustainable
urea.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 14, 2025
Abstract
Single‐atom
site
electrocatalysts
(SACs),
with
maximum
atom
efficiency,
fine‐tuned
coordination
structure,
and
exceptional
reactivity
toward
catalysis,
energy,
environmental
purification,
have
become
the
emerging
frontier
in
recent
decade.
Along
significant
breakthroughs
activity
selectivity,
limited
stability
durability
of
SACs
are
often
underemphasized,
posing
a
grand
challenge
meeting
practical
requirements.
One
pivotal
obstacle
to
construction
highly
stable
is
heavy
reliance
on
empirical
rather
than
rational
design
methods.
A
comprehensive
review
urgently
needed
offer
concise
overview
progress
stability/durability,
encompassing
both
deactivation
mechanism
mitigation
strategies.
Herein,
this
first
critically
summarizes
degradation
induction
factors
at
atomic‐,
meso‐
nanoscale,
mainly
based
but
not
oxygen
reduction
reaction.
Subsequently,
potential
stability/durability
improvement
strategies
by
tuning
catalyst
composition,
morphology
surface
delineated,
including
robust
substrate
metal‐support
interaction,
optimization
active
stability,
fabrication
porosity
modification.
Finally,
challenges
prospects
for
discussed.
This
facilitates
fundamental
understanding
provides
efficient
principles
aimed
overcoming
difficulties
beyond.
