Advanced Materials,
Год журнала:
2023,
Номер
35(52)
Опубликована: Авг. 20, 2023
Abstract
Electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
driven
by
renewable
energy
shows
great
promise
in
mitigating
and
potentially
reversing
the
devastating
effects
of
anthropogenic
climate
change
environmental
degradation.
The
simultaneous
synthesis
energy‐dense
chemicals
can
meet
global
demand
while
decoupling
emissions
from
economic
growth.
However,
development
CO
RR
technology
faces
challenges
catalyst
discovery
device
optimization
that
hinder
their
industrial
implementation.
In
this
contribution,
a
comprehensive
overview
current
state
research
is
provided,
starting
with
background
motivation
for
technology,
followed
fundamentals
evaluated
metrics.
Then
underlying
design
principles
electrocatalysts
are
discussed,
emphasizing
structure–performance
correlations
advanced
electrochemical
assembly
cells
increase
selectivity
throughput.
Finally,
review
looks
to
future
identifies
opportunities
innovation
mechanism
discovery,
material
screening
strategies,
assemblies
move
toward
carbon‐neutral
society.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(15), С. 10599 - 10607
Опубликована: Апрель 3, 2024
The
success
of
electrochemical
CO2
reduction
at
high
current
densities
hinges
on
precise
interfacial
transportation
and
the
local
concentration
gaseous
CO2.
However,
creation
efficient
channels
remains
an
unexplored
frontier.
In
this
study,
we
design
synthesize
hydrophobic
porous
Cu2O
spheres
with
varying
pore
sizes
to
unveil
nanoporous
channel's
impact
gas
transfer
triple-phase
interfaces.
not
only
facilitate
rapid
but
also
trap
compressed
bubbles
form
abundant
stable
interfaces,
which
are
crucial
for
high-current-density
electrocatalysis.
electrolysis,
in
situ
spectroscopy
density
functional
theory
results
reveal
that
atomic
edges
concave
surfaces
promote
C–C
coupling
via
energetically
favorable
OC-COH
pathway,
leading
overwhelming
CO2-to-C2+
conversion.
Leveraging
optimal
active
site
exposure,
a
240
nm
size
(P-Cu2O-240)
stands
out
among
all
samples
exhibits
best
productivity
remarkable
Faradaic
efficiency
formation
rate
up
75.3
±
3.1%
2518.2
8.1
μmol
h–1
cm–2,
respectively.
This
study
introduces
novel
paradigm
electrocatalysts
concurrently
addresses
gas-transfer
challenges.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(33)
Опубликована: Май 27, 2024
Triggering
the
lattice
oxygen
oxidation
mechanism
is
crucial
for
improving
evolution
reaction
(OER)
performance,
because
it
could
bypass
scaling
relation
limitation
associated
with
conventional
adsorbate
through
direct
formation
of
oxygen-oxygen
bond.
High-valence
transition
metal
sites
are
favorable
activating
oxygen,
but
deep
pre-catalysts
suffers
from
a
high
thermodynamic
barrier.
Here,
taking
advantage
Jahn-Teller
(J-T)
distortion
induced
structural
instability,
we
incorporate
high-spin
Mn
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Март 18, 2024
Abstract
Owing
to
the
specific
electronic-redistribution
and
spatial
proximity,
diatomic
catalysts
(DACs)
have
been
identified
as
principal
interest
for
efficient
photoconversion
of
CO
2
into
C
H
4
.
However,
predominant
bottom-up
strategy
DACs
synthesis
has
critically
constrained
development
highly
ordered
due
random
distribution
heteronuclear
atoms,
which
hinders
optimization
catalytic
performance
exploration
actual
reaction
mechanism.
Here,
an
up-bottom
ion-cutting
architecture
is
proposed
fabricate
well-defined
DACs,
superior
proximity
CuAu
diatomics
(DAs)
decorated
TiO
(CuAu-DAs-TiO
)
successfully
constructed
compact
heteroatomic
spacing
(2-3
Å).
profoundly
low
C-C
coupling
energy
barrier
CuAu-DAs-TiO
,
a
considerable
production
with
sustainability
achieved.
Our
discovery
inspires
novel
fabrication
motivate
distinct
deduction
heteroatom
synergistically
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Фев. 26, 2024
Abstract
The
copper
(Cu)-catalyzed
electrochemical
CO
2
reduction
provides
a
route
for
the
synthesis
of
multicarbon
(C
2+
)
products.
However,
thermodynamically
favorable
Cu
surface
(i.e.
Cu(111))
energetically
favors
single-carbon
production,
leading
to
low
energy
efficiency
and
production
rates
C
Here
we
introduce
in
situ
faceting
from
enable
preferential
exposure
Cu(100)
facets.
During
precatalyst
evolution,
phosphate
ligand
slows
assists
generation
co-adsorption
hydroxide
ions,
steering
reconstruction
(100).
resulting
catalyst
enables
current
densities
>
500
mA
cm
−2
Faradaic
efficiencies
>83%
towards
products
both
reduction.
When
run
at
150
hours,
maintains
37%
full-cell
95%
single-pass
carbon
throughout.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июнь 18, 2024
Abstract
The
carbon−carbon
coupling
at
the
Cu/Cu
2
O
Schottky
interface
has
been
widely
recognized
as
a
promising
approach
for
electrocatalytic
CO
conversion
into
value-added
alcohols.
However,
limited
selectivity
of
C
2+
alcohols
persists
due
to
insufficient
control
over
rectifying
characteristics
required
precise
bonding
oxyhydrocarbons.
Herein,
we
present
an
investigation
manipulation
coordination
environment
Cu
sites
through
in-situ
electrochemical
reconstruction
strategy,
which
indicates
that
construction
low-coordinated
facilitates
enhanced
interfaces,
and
induces
asymmetric
electronic
perturbation
faster
electron
exchange,
thereby
boosting
C-C
oxyhydrocarbons
towards
nucleophilic
reaction
process
*H
CCO-CO.
Impressively,
exhibit
superior
faradic
efficiency
64.15
±
1.92%
energy
~39.32%
production,
while
maintaining
stability
50
h
(faradic
>50%,
total
current
density
=
200
mA
cm
−2
)
in
flow-cell
electrolyzer.
Theoretical
calculations,
operando
synchrotron
radiation
Fourier
transform
infrared
spectroscopy,
Raman
experiments
decipher
can
enhance
coverage
*CO
adsorption
*CH
CH
CHO,
facilitating
formation
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(15)
Опубликована: Фев. 12, 2024
Abstract
Electroreduction
of
CO
2
to
C
2+
products
provides
a
promising
strategy
for
reaching
the
goal
carbon
neutrality.
However,
achieving
high
selectivity
at
current
density
remains
challenge.
In
this
work,
we
designed
and
prepared
multi‐sites
catalyst,
in
which
Pd
was
atomically
dispersed
Cu
(Pd−Cu).
It
found
that
Pd−Cu
catalyst
had
excellent
performance
producing
from
electroreduction.
The
Faradaic
efficiency
(FE)
could
be
maintained
approximately
80.8
%,
even
0.8
A
cm
−2
least
20
hours.
addition,
FE
above
70
%
1.4
.
Experiments
functional
theory
(DFT)
calculations
revealed
three
distinct
catalytic
sites.
These
active
sites
allowed
efficient
conversion
,
water
dissociation,
conversion,
ultimately
leading
yields
products.
Energy & Environmental Science,
Год журнала:
2024,
Номер
17(16), С. 5795 - 5818
Опубликована: Янв. 1, 2024
Recent
developments
in
heteroatom-doped
Cu-based
catalysts
for
CO
2
electroreduction
into
C
2+
products
are
highlighted.
The
design
strategies
doped
and
situ
technologies
discussed.
ACS Catalysis,
Год журнала:
2024,
Номер
14(11), С. 8776 - 8785
Опубликована: Май 21, 2024
Selective
electroreduction
of
CO2
to
ethanol
has
economic
value
and
environmental
significance.
However,
the
activity
selectivity
reduction
toward
are
still
low
due
sluggish
kinetics
C–C
coupling
intense
competition
hydrocarbon
production.
Herein,
we
report
a
layered
tandem
catalyst
consisting
Cu
nanosheets
with
Cu(111)-oriented
surface
Ag
nanoparticles,
which
can
effectively
shift
from
hydrocarbons
ethanol.
The
Faradaic
efficiency
was
improved
less
than
30%
on
bare
Cu(111)
56.5
±
2.6%
Cu/Ag
catalysts,
partial
current
density
356.7
9.5
mA
cm–2.
In
situ
Raman
spectroscopy
results
functional
theory
calculations
suggest
that
high
be
attributed
asymmetric
*CH2–CO
mechanism,
is
facilitated
by
selective
generation
*CH2
species
(111)-facet-exposed
local
CO
concentration
supplied
catalyst.
