Advanced Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 27, 2025
Abstract
The
electrocatalytic
conversion
of
CO
2
into
valuable
multi‐carbon
(C
2+
)
products
using
Cu‐based
catalysts
has
attracted
significant
attention.
This
review
provides
a
comprehensive
overview
recent
advances
in
catalyst
design
to
improve
C
selectivity
and
operational
stability.
It
begins
with
an
analysis
the
fundamental
reaction
pathways
for
formation,
encompassing
both
established
emerging
mechanisms,
which
offer
critical
insights
design.
In
situ
techniques,
essential
validating
these
by
real‐time
observation
intermediates
material
evolution,
are
also
introduced.
A
key
focus
this
is
placed
on
how
enhance
through
manipulation,
particularly
emphasizing
catalytic
site
construction
promote
C─C
coupling
via
increasing
*
coverage
optimizing
protonation.
Additionally,
challenge
maintaining
activity
under
conditions
discussed,
highlighting
reduction
active
charged
Cu
species
materials
reconstruction
as
major
obstacles.
To
address
these,
describes
strategies
preserve
sites
control
including
novel
utilization
mitigation
reconstruction.
By
presenting
developments
challenges
ahead,
aims
guide
future
conversion.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 5, 2025
Multi-proton-coupled
electron
transfer,
multitudinous
intermediates,
and
unavoidable
competing
hydrogen
evolution
reaction
during
CO2
electroreduction
make
it
tricky
to
control
high
selectivity
for
specific
products.
Here,
we
present
spatial
confinement
of
Fe
single
atoms
(FeN2S2)
by
adjacent
FeS
clusters
(Fe4S4)
orientate
the
transition
adsorption
configuration
from
C,O-side
O-end,
which
triggers
a
shift
activated
first-step
protonation
C–C
coupling,
thus
switching
target
product
HCOOH
in
Faraday
efficiency
(FE:
90.6%)
on
FeN2S2
CH3COOH
82.3%)
Fe4S4/FeN2S2.
The
strength
*OCHO
upon
solitary
site
is
linearly
related
coordination
number
Fe–S,
with
predominantly
produced
over
single-atom
(ortho-substituted
S
atoms).
Fe4S4
cluster
functions
as
switch
reduction
product,
can
not
only
optimize
electronic
structure
neighboring
but
also
impel
complete
hydrocarbon
intermediate
*CH3,
followed
coupling
CO2*
*CH3
via
synergistic
catalysis
This
strategy
provides
new
avenue
modulate
reactant
model
desirable
pathways,
potential
applications
diverse
multistep
electrochemical
processes
controlled
selectivity.
Growing
global
population,
escalating
energy
consumption,
and
climate
change
threaten
future
security.
Fossil
fuel
combustion,
primarily
coal,
oil,
natural
gas,
exacerbates
the
greenhouse
effect
driving
warming
through
CO
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(39)
Опубликована: Июль 29, 2024
Abstract
Electrocatalytic
CO
2
reduction
(ECR)
powered
by
renewable
electricity
is
a
promising
technology
to
mitigate
carbon
emissions
and
lessen
the
dependence
on
fossil
fuels
toward
carbon‐neutral
energy
cycle.
Metal–organic
frameworks
(MOFs)
their
derivatives,
due
excellent
intrinsic
activity,
have
emerged
as
materials
for
ECR
high‐demand
products.
However,
challenges
such
unsatisfactory
efficiency,
selectivity,
relatively
low
production
rates
hinder
industrial
scalability.
Here,
comprehensive
critical
review
presented
that
summarizes
state‐of‐the‐art
progress
in
MOF‐based
MOF‐derived
electroreduction
catalysts
from
design
functionality
perspectives.
The
fundamentals
of
reaction
(CO
RR)
over
heterogeneous
catalysts,
mechanisms,
key
faced
are
described
first
establish
solid
foundation
forthcoming
in‐depth
analyses.
MOF's
building
blocks,
properties,
shortcomings
pertinent
including
conductivity
stability,
systematically
discussed.
Moreover,
discussions
provided
design,
fabrication,
characterization,
RR
activity
pinpoint
intricate
structure‐property‐performance
relationship.
Finally,
recommendations
put
forward
enhancing
MOF
electrocatalysts
durability.
This
work
may
serve
guideline
developing
high‐performance
MOF‐related
RR,
benefiting
researchers
working
this
growing
potentially
game‐changing
area.
Electrochemical
CO2
reduction
(CO2RR)
in
membrane
electrode
assembly
(MEA)
represents
a
viable
strategy
for
converting
into
value-added
multi-carbon
(C2+)
compounds.
Therefore,
the
microstructure
of
catalyst
layer
(CL)
affects
local
gas
transport,
charge
conduction,
and
proton
supply
at
three-phase
interfaces,
which
is
significantly
determined
by
solvent
environment.
However,
microenvironment
CLs
mechanism
effect
on
C2+
selectivity
remains
elusive.
Herein,
tailored
interfacial
structure
designed
introducing
solvent-mediated
catalyst-ionomer-solvent
microenvironment.
The
acetone
surface
promotion
beneficial
unfolded
ionomers
to
uniformly
coat
catalysts,
contributes
enhancing
hydrophobicity
inhibiting
hydrogen
evolution.
Furthermore,
molecular
dynamics
(MD)
simulation
situ
ATR-SEIRAS
are
employed
elucidate
appropriate
network
with
balanced
distribution
H2O.
uniform
continuous
advantageous
CO2-to-C2+.
optimized
favors
production
products
Cu-based
MEA,
exhibiting
high
faradaic
efficiency
(FE)
80.27%
400
mA
cm-2.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 25, 2025
Abstract
Carbon
capture
and
utilization
(CCU)
is
pivotal
for
low‐carbon
industry.
Among
varied
techniques,
coupling
of
carbon
dioxide
(CO
2
)
with
small
molecules
to
generate
valuable‐added
chemicals
using
renewable
electricity
stands
out
thanks
its
cost‐effectiveness
sustainability.
This
review
first
highlights
recent
strategies
in
catalyst
preparation
improving
the
efficiency
selectivity
electrochemical
reactions,
including
heterostructure
catalysts,
bimetallic
defect
engineering,
coordination
complexes.
The
progresses
on
mechanism
investigation
C─N,
C─O,
C─C
situ
spectroscopies
online
mass
spectrometry
are
subsequently
summarized.
In
addition,
electrolyzer
design
techno–economic
analysis
about
process
optimization
integration
energy
stressed.
Finally,
future
challenges
optimization,
reaction
elucidation,
scale‐up
implementation
discussed.
Science China Materials,
Год журнала:
2024,
Номер
68(1), С. 21 - 38
Опубликована: Ноя. 8, 2024
Abstract
The
conversion
of
carbon
dioxide
(CO
2
)
to
the
reduced
chemical
compounds
offers
substantial
environmental
benefits
through
minimizing
emission
greenhouse
gas
and
fostering
sustainable
practices.
Recently,
unique
properties
metal-organic
frameworks
(MOFs)
make
them
attractive
candidates
for
electrocatalytic
CO
reduction
reaction
RR),
providing
many
opportunities
develop
efficient,
selective,
environmentally
processes
mitigating
emissions
utilizing
as
a
valuable
raw
material
synthesis
fuels
chemicals.
Here,
recent
advances
in
MOFs
efficient
catalysts
RR
are
summarized.
detailed
characteristics,
mechanisms,
practical
approaches
improving
efficiency,
selectivity,
durability
under
realistic
conditions
also
clarified.
Furthermore,
outlooks
on
prospects
MOF-based
electrocatalysts
provided.
Journal of CO2 Utilization,
Год журнала:
2024,
Номер
83, С. 102819 - 102819
Опубликована: Май 1, 2024
Converting
waste
or
hazardous
chemicals
into
valuable
products
is
a
paramount
consideration
from
economic,
environmental,
and
sustainability
standpoints.
Diverse
strategies
are
under
exploration
to
convert
CO₂
fine
chemicals,
encompassing
electrocatalysis,
thermo-
photo-catalysis,
chemical
fixation.
Amid
these
avenues,
the
electrochemical
reduction
reaction
(CO₂RR)
emerges
as
exceptionally
promising,
driven
by
its
manifold
advantages
growing
accessibility
of
renewable
electricity
sources.
While
CO₂RR
has
witnessed
substantial
advancements,
most
endeavors
remain
in
proof-of-concept
phase,
necessitating
improved
catalytic
efficiency
stability
enable
industrialization.
Realizing
industrial
viability
technology
mandates
meticulous
myriad
electrocatalyst-related
factors.
This
review
delves
critical
criteria
recent
materials
with
potential
drive
at
an
scale.
These
factors,
akin
other
processes,
closely
relate
activity,
product
selectivity,
catalyst/system
stability,
catalyst
cost.
In
this
context,
we
investigated
that
define
electrocatalysts
industrially
feasible,
considering
factors
such
Faradaic
efficiency,
current
density,
energy
overpotential,
choice
materials.
Furthermore,
highlight
prime
examples
demonstrating
high
for
process
categorize
them
based
on
products.
To
offer
comprehensive
perspective,
also
discusses
fundamental
principles
CO₂RR,
covering
physicochemical
properties
CO₂,
cell
configurations,
electrolyte
compositions,
role
electrocatalysts.
We
address
economic
significance
various
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 2, 2025
Abstract
Atomically
dispersed
materials
have
been
a
thriving
research
field
due
to
their
maximum
atomic
utilization
and
remarkable
performance
in
energy
conversion
storage
systems.
Owing
the
large
radius,
strong
oxophilicity,
unique
electronic
properties,
rare‐earth
(RE)
elements
widely
investigated
as
oxide
carriers
promoters
atomically
manipulate
regulate
structure
of
active
species.
Single‐atom
state
with
an
adjustable
coordination
environment
on
N‐doped
carbon
endows
RE
metals
special
states
outstanding
catalytic
performances.
A
thorough
comprehension
modulation
mechanism
paves
way
for
construction
advanced
RE‐based
electrocatalysts
high
activity,
stability,
selectivity.
This
review
provides
widespread
insight
into
roles
modulating
properties
combined
structure–performance
relationship
electrocatalysis
processes.
The
characteristic
physical
chemical
are
highlighted,
synthetic
strategy
is
discussed.
Finally,
summary
perspectives
rational
design
development
highly
efficient
catalysts
proposed.
aims
provide
guideline
promoting
effective
functional
materials.
Inorganic Chemistry Frontiers,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
This
paper
reviews
the
progress
of
defective
Cu-based
materials
for
eCO
2
RR,
highlights
design
strategy
defect
structure
and
emphasizes
mechanism
site
on
catalytic
behaviors.