Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 24, 2025
The
electrocatalytic
conversion
of
carbon
dioxide
(CO2)
to
ethylene
(C2H4)
holds
great
promise
for
sustainable
chemical
synthesis,
yet
achieving
industrially
relevant
production
rates
remains
a
significant
challenge.
Through
computational
screening,
we
have
identified
praseodymium
(Pr)
single-atom
alloy
embedded
in
copper
(Cu)
catalyst
(Pr@Cu)
that
exhibits
superior
CO2
activation
and
remarkably
low
energy
barrier
asymmetric
*CO-*CHO
coupling,
primarily
by
facilitating
the
*CHO
intermediate
formation.
Our
optimized
catalyst,
Pr@Cu-2
(6
wt
%
Pr),
achieves
C2H4
Faradaic
efficiency
(FE)
64.2%
at
-1.6
V
versus
reversible
hydrogen
electrode
(RHE)
under
high
current
density
1200
mA
cm-2
reduction
reaction
(CO2RR).
Furthermore,
when
integrated
into
100
cm2
membrane
assembly
(MEA)
electrolyzer,
demonstrates
robust
performance,
maintaining
continuous
rate
21.3
mL
min-1
20
A
over
200
h.
This
work
provides
fundamental
insights
role
Pr
alloys
CO2RR
highlights
their
potential
scalable
electrosynthesis.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(10), С. 5149 - 5189
Опубликована: Янв. 1, 2024
This
review
summarizes
promising
strategies
including
the
design
of
catalysts
and
construction
coupled
electrocatalytic
reaction
systems,
aimed
at
achieving
selective
production
various
products
from
CO
2
electroreduction.
ACS Nano,
Год журнала:
2024,
Номер
18(23), С. 15303 - 15311
Опубликована: Май 28, 2024
Electroreduction
of
CO2
in
highly
acidic
environments
holds
promise
for
enhancing
utilization
efficiency.
Due
to
the
HER
interference
and
structural
instability,
however,
challenges
improving
selectivity
stability
toward
multicarbon
(C2+)
products
remain.
In
this
study,
we
proposed
an
"armor
protection"
strategy
involving
deposition
ultrathin,
hydrophobic
SiO2
onto
Cu
surface
(Cu/SiO2)
through
a
simple
one-step
hydrolysis.
Our
results
confirmed
effective
inhibition
by
layer,
leading
high
Faradaic
efficiency
(FE)
up
76.9%
C2+
at
current
density
900
mA
cm–2
under
strongly
condition
with
pH
1.
The
observed
performance
surpassed
reported
most
previously
studied
Cu-based
catalysts
CO2RR
systems.
Furthermore,
ultrathin
shell
was
demonstrated
effectively
prevent
reconstruction
preserve
oxidation
state
Cuδ+
active
sites
during
CO2RR.
Additionally,
it
hindered
accumulation
K+
ions
on
catalyst
diffusion
situ
generated
OH–
away
from
electrode,
thereby
favoring
product
generation.
Raman
analyses
coupled
DFT
simulations
further
elucidated
that
proficiently
modulated
*CO
adsorption
behavior
Cu/SiO2
reducing
energy,
facilitating
C–C
coupling.
This
work
offers
compelling
rationally
designing
exploiting
stable
environments.
Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 22, 2024
Abstract
Reconstruction
of
catalysts
is
now
well
recognized
as
a
common
phenomenon
in
electrocatalysis.
As
the
reconstructed
structure
may
promote
or
hamper
electrochemical
performance,
how
to
achieve
designed
active
surface
for
highly
enhanced
catalytic
activity
through
reconstruction
needs
be
carefully
investigated.
In
this
review,
genesis
and
effects
various
processes,
such
hydrogen
evolution
reaction
(HER),
oxygen
(OER),
carbon
dioxide
reduction
(CO
2
RR),
nitrate
(NO
3
RR)
are
first
described.
Then,
strategies
optimizing
reconstruction,
valence
states
control,
phase
retention,
engineering,
poisoning
prevention
comprehensively
discussed.
Finally,
general
rules
optimization
summarized
give
perspectives
future
study.
It
believed
that
review
shall
provide
deep
insights
into
electrocatalytic
mechanisms
guide
design
pre‐catalysts
with
improved
activity.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 1, 2025
Abstract
The
synergistic
effects
in
electrocatalysis
can
significantly
enhance
catalyst
performance
by
improving
catalytic
activity,
selectivity,
and
stability,
optimizing
reaction
mechanisms
electron
transfer
processes.
This
review
summarizes
recent
advancements
the
of
electrochemical
reduction
CO
2
(eCO
RR)
to
multi‐carbon
(C
2+
)
products.
Starting
with
fundamental
principles
eCO
RR
for
C
product
formation,
paper
outlines
producing
,
3
4
5
A
comprehensive
discussion
is
provided
on
critical
impact
structure–performance
relationship
production
Subsequently,
observed
are
classified
various
electrocatalysts
different
properties,
including
single/dual‐atom
catalysts,
multi‐centric
single‐atom
alloys,
metal‐organic
frameworks,
heterojunction
catalysts.
Finally,
challenges
achieving
selective
formation
through
discussed,
along
corresponding
strategies
overcome
obstacles.
Abstract
Solar‐driven
carbon
dioxide
(CO
2
)
methanation
holds
significant
research
value
in
the
context
of
emission
reduction
and
energy
crisis.
However,
this
eight‐electron
catalytic
reaction
presents
substantial
challenges
activity
selectivity.
In
regard,
researchers
have
conducted
extensive
exploration
achieved
developments.
This
review
provides
an
overview
recent
advances
efficient
selective
photocatalytic
CO
methanation.
It
begins
by
discussing
fundamental
principles
detail,
analyzing
strategies
for
improving
efficiency
conversion
to
CH
4
comprehensively.
Subsequently,
it
outlines
applications
advanced
characterization
methods
Finally,
highlights
prospects
opportunities
area,
aiming
inspire
into
high‐value
shed
light
on
mechanisms.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(38)
Опубликована: Апрель 10, 2024
Abstract
Many
non‐precious
metal‐nitrogen
(M–N
x
)‐containing
catalysts
are
highly
efficient
for
electrochemical
reduction
of
CO
2
to
and
yet
encounter
challenges
in
further
converting
more
valuable
two‐carbon
products
(C2),
such
as
ethanol
acetic
acid.
The
ambiguous
structure‐activity
relationship
the
M–N
moieties
toward
reaction
(CO
RR)
results
difficulties
regulating
RR
product
selectivity
on
‐containing
catalysts.
Herein,
by
using
fluorinated
iron
phthalocyanines
with
axial‐coordinated
ligands
(L–FePc–F)
an
4
‐based
model
electrocatalyst
RR,
a
correlation
between
electronic
structure
C2
Fe–N
is
revealed
comprehensive
descriptor
based
Fe–CO
π‐backbonding
proposed
guiding
regulation
higher
selectivity.
Based
principle,
Br‐axial‐coordinated
FePc–F
(Br–FePc–F)
remarkably
increases
Faradic
efficiency
(FE)
from
0%
(i.e.,
FE
FePc–F)
34%
due
strengthened
stemming
elevated
3
d
xz
/
yz
orbital
energy
enhanced
electron‐donating
ability
Fe
centers
.
This
work
provides
strategy
mechanism
insights
moieties,
which
may
be
inspiring
precise
construction
specific
products.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 29, 2024
Abstract
Ethylene
(C
2
H
4
)
electrosynthesis
from
the
electrocatalytic
CO
reduction
process
holds
enormous
potential
applications
in
industrial
production.
However,
sluggish
kinetics
of
C─C
coupling
often
result
low
yield
and
poor
selectivity
for
C
Herein,
performance
Cu
catalysts
varying
sizes
is
investigated,
prepared
via
a
cryo‐mediated
liquid
phase
exfoliation
technique,
electrochemical
to
.
The
activity
gradually
increase
as
size
decreases
tens
nanometers
few
nanometers.
Impressively,
5
nm
quantum
dots
(Cu‐5)
achieve
maximum
Faradaic
efficiency
(FE)
81.5%
half‐cell
cathodic
energy
(CEE)
42.2%
with
large
partial
current
density
1.1
A
cm
−2
at
−0.93
V
versus
reversible
hydrogen
electrode.
Structural
characterization
situ
spectroscopic
analysis
reveal
that
Cu‐5
dots,
dominated
by
(100)
facet,
provide
an
abundance
active
sites
enhance
adsorption
activation,
promoting
formation
*CO
intermediates.
accumulation
intermediates
on
facilitates
CO‐CHO
reaction,
thus
enhancing
production
rate.