Industrial & Engineering Chemistry Research,
Journal Year:
2024,
Volume and Issue:
63(43), P. 18371 - 18379
Published: Oct. 16, 2024
The
preparation
of
multicarbon
products,
such
as
ethylene
(C2H4),
is
primarily
achieved
through
gas-phase
CO2
electrolysis.
However,
this
method
faces
challenges,
including
low
utilization
and
inefficient
catalysts.
To
address
these
issues,
direct
carbonate
electrolysis
can
be
employed
effectively.
In
study,
we
propose
a
microenvironment-modulated
strategy
to
enhance
the
efficiency
C2H4
using
Cu
catalyst.
By
incorporating
hydrophobic
component,
polytetrafluoroethylene
(PTFE),
on
surface
catalyst,
significant
improvement
in
selectivity,
from
1.07%
for
catalyst
13.48%
Cu/50%
PTFE
at
100
mA
cm–2.
Furthermore,
by
optimizing
CO
coverage
catalytic
interface
with
tandem
components,
notably
Ni–N–C,
Faradaic
was
boosted
21.72%
same
current
density.
Notably,
gas
almost
undetectable
outlet
during
long-term
stability
test,
indicating
nearly
100%
utilization.
This
research
underscores
significance
adjusting
microenvironment
electrode–electrolyte
(bi)carbonate
ACS Energy Letters,
Journal Year:
2025,
Volume and Issue:
10(1), P. 600 - 619
Published: Jan. 2, 2025
The
electrochemical
reduction
reaction
of
CO2
(eCO2RR)
to
chemicals
presents
a
viable
solution
for
addressing
climate
change
and
sustainable
manufacturing.
In
this
Review,
we
describe
the
recent
advancements
in
eCO2RR
multicarbon
(C2+)
production
from
aspects
catalyst
structure,
microenvironments,
mechanistic
understanding.
We
draw
experimental
theoretical
comparisons
between
systems
containing
bulk
highly
dispersed
metals,
alloys,
metal
compounds
recount
new
results
microenvironmental
impacts
as
well
catalytic
mechanism.
From
our
own
studies,
offer
some
viewpoints
on
electrocatalytic
mechanism
during
complex
multistep
proton-coupled
electron
transfers
propose
several
research
directions
unlocking
full
potential
scalable
industrial
CO2-to-C2+
conversion.
Copper-based
catalysts
demonstrate
distinctive
multicarbon
product
activity
in
the
CO2
electroreduction
reaction
(CO2RR);
however,
their
low
selectivity
presents
significant
challenges
for
practical
applications.
Herein,
we
have
developed
a
multilevel
porous
spherical
Cu2O
structure,
wherein
mesopores
are
enriched
with
catalytic
active
sites
and
effectively
stabilize
Cu+,
while
macropores
facilitate
formation
of
"gas–liquid–solid"
three-phase
interface,
thereby
creating
microenvironment
an
increasing
water
concentration
gradient
from
interior
to
exterior.
Potential-driven
phase
engineering
protonation
synergistically
optimize
pathway,
facilitating
switch
between
CO
C2H4.
At
current
density
100
mA
cm–2,
faradaic
efficiency
(FE)
reaches
impressive
96.97%.
When
increases
1000
FEC2H4
attains
53.05%.
Experiments
theoretical
calculations
indicate
that
at
lower
potentials,
pure
diminishes
adsorption
*CO
intermediates,
weak
inhibits
hydrogen
evolution
reactions,
promoting
production.
Conversely,
more
negative
Cu0/Cu+
interface
strong
generate
locally
elevated
concentrations
*COOH
which
enhance
C–C
coupling
deep
hydrogenation,
ultimately
improving
toward
C2+
products.
This
study
provides
novel
insights
into
rational
design
copper-based
customizable
Small,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 21, 2025
Abstract
Achieving
fast
conversion
and
precise
regulation
of
product
selectivity
in
electrochemical
CO
2
reduction
reaction
(CO
RR)
remains
a
challenge.
The
space
confinement
effect
provides
theoretical
basis
for
the
design
catalysts
different
morphology
sizes
reveals
physical
phenomena
caused
by
electrons
other
particles
at
nanoscale.
In
this
work,
semi‐confinement
concept
is
introduced
mesoporous
silica
nanosphere
supported
Cu
catalyst
(Cu‐MSN)
prepared
as
typical
example
to
realize
RR
enhancement
(methane
vs
ethylene).
semi‐confined
structure
partially
solves
mass
transfer
problem
classical
confined
catalysis.
Cu‐MSN
allows
flexible
controls
aggregation
form
species
loading
amount,
which
achieves
free
switch
from
methane
Faraday
efficiency
71.1%
ethylene
66.4%.
Various
characterizations
confirm
that
adsorption
behavior
local
coordination
transformation
(from
Cu─O─Si
Cu─O─Cu),
can
stabilize
key
intermediates
*
CHO
COH
generating
respective
ethylene.
Advanced Science,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 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.
