The
activation
of
lattice
oxygen
at
low
temperatures
is
essential
for
heterogeneous
catalytic
oxidation,
but
exactly
how
this
achieved
by
adjusting
the
coordination
structure
atomic
sites
still
elusive.
Herein,
Cu1O3-CeO2
catalyst
with
highly
dispersed
unsaturated
Cu1-O3
was
creatively
engineered,
which
remarkably
enhanced
low-temperature
oxidation
CO
(a
typical
model
reaction)
from
12%
to
90%
66
°C
compared
conventional
CuCeO
x
catalyst.
preservation
coordination-deficient
Cu
enables
transfer
electron
cloud
density
atoms
O
atoms,
hence,
facilitating
oxygen.
Further
atom
species
results
in
charge
back-donation
form
sufficient
Cu+
and
metal
per-oxy
species,
contributing
weaken
O-O
bonds.
We
determined
that
increasing
number
donors
induced
an
efficient
strategy
develop
active
stable
catalysts
activation.
synthesis
strategies
mechanism
demonstrated
work
provide
a
generalizable
platform
future
design
well-defined
functional
reactions.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(46)
Опубликована: Авг. 9, 2024
Abstract
Carbon
materials
are
of
great
significance
in
state‐of‐the‐art
electrochemical
CO
2
reduction
(ECR)
as
key
components
such
electrocatalysts,
gas
diffusion
electrodes,
and
current
collectors.
Notably,
dimensionalities
carbons
related
manipulations
play
vital
roles
boosting
ECR
performance,
e.g.,
mass/charge
transfer
dynamics,
exposure
active
sites,
reaction
space,
product's
Faradaic
efficiency/selectivity,
durability.
Here,
recent
endeavors
dimensionality
engineering
toward
advanced
carbon‐based
for
is
first
summarized,
including
pure
(e.g.,
carbon
nanotube
graphene)
composites,
highlight
the
dimensionality‐dependent
properties
performance.
Various
strategies
referring
to
modulation
integration
have
been
top‐down,
bottom‐up,
soft
chemical
approaches.
Design
principles
dimensionality‐varied
elaborated,
impacts
surface
chemistry
functional
group,
wettability,
electronic
structure)
on
kinetics
product‐targeted
mechanisms
also
scrutinized.
Some
insights
into
how
manipulation
elevates
performance
acceleration,
kinetics,
product
selectivity
provided.
At
last,
a
perspective
challenges
future
development
discussed.
This
review
aims
at
providing
guidance
customizable
construction
with
dependence
green
energy‐saving
electrosynthesis
systems.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(48)
Опубликована: Окт. 15, 2024
Abstract
The
electrochemical
reduction
of
nitrate
to
ammonia
(NO
3
RR)
is
an
effective
route
synthesis
with
the
characteristics
low
energy
input.
However,
complex
multi‐electron/proton
transfer
pathways
associated
this
reaction
may
trigger
accumulation
competitive
by‐products.
Herein,
boron
(B)‐doped
Cu
electrode
(denoted
as
B–Cu
2
O/Cu/CP)
“all‐in‐one”
catalyst
prepared
by
one‐step
electrodeposition
strategy.
Caused
B
doping,
charge
redistribution
and
local
coordination
environment
O/Cu
species
are
modulated,
resulting
in
exposure
active
sites
on
O/Cu/CP
catalyst.
In‐situ
Fourier
transform
infrared
spectroscopy
theoretical
investigations
demonstrate
that
both
O
modulated
can
effectively
enhance
adsorption
NO
−
facilitate
conversion
intermediate
by‐products,
thus
promoting
direct
NH
.
Consequently,
a
remarkable
Faradaic
efficiency
92.74%
be
obtained
minimal
It
expected
work,
based
heterogeneous
will
open
maneuverable
versatile
way
for
design
catalysts.
Advanced Materials,
Год журнала:
2024,
Номер
36(52)
Опубликована: Ноя. 26, 2024
Abstract
Electrocatalytic
carbon
dioxide
(CO
2
)
conversion
into
valuable
chemicals
paves
the
way
for
realization
of
recycling.
Downsizing
catalysts
to
single‐atom
(SACs),
dual‐atom
(DACs),
and
sub‐nanocluster
(SNCCs)
has
generated
highly
active
selective
CO
transformation
reduced
products.
This
is
due
introduction
numerous
sites,
unsaturated
coordination
environments,
efficient
atom
utilization,
confinement
effect
compared
their
nanoparticle
counterparts.
Herein,
recent
Cu‐based
SACs
are
first
reviewed
newly
emerged
DACs
SNCCs
expanding
catalysis
electrocatalytic
reduction
RR)
high‐value
products
discussed.
Tandem
SAC–nanocatalysts
(NCs)
(SAC–NCs)
also
discussed
RR
Then,
non‐Cu‐based
SACs,
DACs,
SAC–NCs,
theoretical
calculations
various
transition‐metal
summarized.
Compared
previous
achievements
less‐reduced
products,
this
review
focuses
on
double
objective
achieving
full
increasing
selectivity
formation
rate
toward
C–C
coupled
with
additional
emphasis
stability
catalysts.
Finally,
through
combined
experimental
research,
future
outlooks
offered
further
develop
over
isolated
atoms
sub‐nanometal
clusters.
Industrial & Engineering Chemistry Research,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 4, 2025
Electrocatalytic
CO2
Reduction
Reaction
(ECO2RR)
driven
by
renewable
energy,
which
could
convert
into
fuels
or
value-added
chemicals,
has
become
an
effective
approach
to
address
environmental
issues
and
the
energy
crisis.
However,
due
low
selectivity,
inferior
activity,
unmanageable
reconstruction
of
catalysts,
path
ECO2RR
remains
a
significant
challenge.
In
this
study,
series
electrocatalysts
composed
copper–lanthanum
nanoparticles
dispersed
within
nitrogen-doped
carbon
framework
(LaCu@NCF-x,
where
x
represents
abbreviation
calcination
temperatures)
were
synthesized
calcining
mixture
polymers
metal
ions,
in
thermal
control
is
key
catalyst
preparation
process.
Phase
morphological
characterizations
reveal
that
degree
carbonization
accessibility
active
sites
modulated
temperature
calcination.
The
study
highlights
importance
synergistic
confinement
effects
encapsulating
layer,
not
only
provides
favorable
matrix
for
but
also
mitigates
electrocatalysts,
thereby
significantly
enhancing
its
performance
CH4
production
during
ECO2RR.
particular,
LaCu@NCF-3
demonstrates
maximum
Faraday
efficiency
(FE)
up
64.6%
at
−1.177
V
vs
RHE
superior
stability.
Moreover,
it
maintains
high
selectivity
(FECH4
≥
60%)
over
wide
potential
range
from
−0.977
−1.577
RHE.
This
novel
fabrication
efficient
stable
Cu-based
electrocatalyst
CH4.
