Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(26)
Published: April 28, 2023
Electrochemical
conversion
of
CO2
to
highly
valuable
ethanol
has
been
considered
a
intriguring
strategy
for
carbon
neutruality.
However,
the
slow
kinetics
coupling
carbon-carbon
(C-C)
bonds,
especially
low
selectivity
than
ethylene
in
neutral
conditions,
is
significant
challenge.
Herein,
asymmetrical
refinement
structure
with
enhanced
charge
polarization
built
vertically
oriented
bimetallic
organic
frameworks
(NiCu-MOF)
nanorod
array
encapsulated
Cu2
O
(Cu2
O@MOF/CF),
which
can
induce
an
intensive
internal
electric
field
increase
C-C
producing
electrolyte.
Particularly,
when
directly
employed
O@MOF/CF
as
self-supporting
electrode,
faradaic
efficiency
(FEethanol
)
could
reach
maximum
44.3
%
energy
27
at
working-potential
-0.615
V
versus
reversible
hydrogen
electrode
(vs.
RHE)
using
-saturated
0.5
M
KHCO3
Experimental
and
theoretical
studies
suggest
that
atomically
localized
fields
derived
from
asymmetric
electron
distribution
tune
moderate
adsorption
*CO
assist
reduce
formation
H2
CCHO*-to-*OCHCH3
generation
ethanol.
Our
research
offers
reference
design
active
selective
electrocatalysts
reducing
multicarbon
chemicals.
Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(17), P. 10530 - 10583
Published: Aug. 17, 2023
Electrosynthesis
of
value-added
chemicals,
directly
from
CO2,
could
foster
achievement
carbon
neutral
through
an
alternative
electrical
approach
to
the
energy-intensive
thermochemical
industry
for
utilization.
Progress
in
this
area,
based
on
electrogeneration
multicarbon
products
CO2
electroreduction,
however,
lags
far
behind
that
C1
products.
Reaction
routes
are
complicated
and
kinetics
slow
with
scale
up
high
levels
required
commercialization,
posing
significant
problems.
In
review,
we
identify
summarize
state-of-art
progress
synthesis
a
multiscale
perspective
discuss
current
hurdles
be
resolved
generation
reduction
including
atomistic
mechanisms,
nanoscale
electrocatalysts,
microscale
electrodes,
macroscale
electrolyzers
guidelines
future
research.
The
review
ends
cross-scale
links
discrepancies
between
different
approaches
extensions
performance
stability
issues
arise
industrial
environment.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(11), P. 3627 - 3662
Published: Jan. 1, 2023
The
selective
methanation
of
CO2
is
an
important
research
area
to
meet
the
net-zero
emission
targets.
Furthermore,
it
crucial
develop
solutions
achieve
carbon
neutrality,
hydrogen
utilization,
circularity,
and
chemical-energy
storage.
This
conversion
can
be
realized
via
thermocatalytic
multistep
power-to-X
route
or
by
direct
electro-
(or
photoelectro)-catalytic
technologies.
Herein,
we
discuss
need
accelerate
Improving
these
technologies
requires
a
better
understanding
catalytic
chemistry
complexity
aspects
consider
in
bridging
electrocatalytic
methanation.
In
this
tutorial
review,
initially
analyze
fundamental
question
competitive
adsorption
key
reactants
regulation
strategies
promote
overall
reaction.
Then,
approach
used
guide
reader
differences
between
thermocatalysis
electrocatalysis.
Finally,
necessary
include
modelling
designing
next-generation
electrocatalysts
for
analyzed.
Energy & Environmental Science,
Journal Year:
2024,
Volume and Issue:
17(16), P. 5795 - 5818
Published: Jan. 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,
Journal Year:
2024,
Volume and Issue:
14(2), P. 741 - 750
Published: Jan. 2, 2024
Achieving
CO2
electroreduction
in
an
acidic
electrolyte
to
obtain
high-value
products
is
a
great
challenge,
but
it
has
remained
elusive
so
far
due
the
high
requirements
for
catalyst
stability.
Herein,
we
designed
and
constructed
highly
stable
(acid-
alkali-resistant)
well-defined
crystalline
coordination
compound
catalyst,
Inz-Cu3,
which
can
switch
structural
symmetry
by
varying
distance
angle
between
adjacent
synergistic
Cu
active
sites,
thus
achieving
selective
conversion
of
C2
product
electrolyte.
At
current
density
−320
mA·cm–2,
achieved
up
42.20%
selectivity
electrocatalytic
reduction
electrolyte,
catalytic
(66.79%,
containing
35.27%
FEC2H4
31.52%
FEC2H5OH)
also
be
conventional
alkaline
Moreover,
functional
theory
(DFT)
calculation
control
experiments
revealed
that
asymmetric
sites
with
close
stabilize
*CHOHCH3
intermediates,
improving
product.
This
work
demonstrates
strategy
design
catalysts
enables
achievement
high-value-added
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(5), P. 3266 - 3277
Published: Feb. 15, 2024
Copper
oxide
(Cu2O)
is
considered
a
promising
catalyst
that
can
effectively
reduce
the
overpotential
of
CO2
reduction
reaction
(CO2
RR)
and
increase
selectivity
for
C2+
products.
However,
developing
high-performance
stable
CO2-to-ethanol
(C2H5OH)
based-Cu2O
electrocatalysts
remains
challenging.
In
this
work,
Cu2O@Cu2S
twin
heterojunction
catalysts
with
multitwin
boundaries
are
designed
to
afford
C2H5OH
productivity
at
low
potential
through
electrocatalytic
RR,
highly
dependent
on
facet
nanocubes
outperforming
octahedra.
Detailed
electrochemical
experiments,
density
functional
theory
(DFT)
calculations
in
situ
infrared
spectroscopy
reveals
introduction
Cu2S
boosts
high
coverage
*CO,
which
easily
spillover
generate
*CHOH_*CO
coupling
pathway.
A
production
begins
an
ultralow
−0.45
V
vs
RHE
reaches
34
43.9%
Faradaic
efficiencies
(FE)
−0.65
H-cell
flow
cell,
respectively.
Meanwhile,
constructed
interface
coherent
structure
suitable
band
facilitate
electron
transfer
from
Cu2O
Cu2S,
leading
stability
Cu+
valence
states.
This
work
provides
avenue
precisely
design
by
regulating
configuration.
ACS Applied Materials & Interfaces,
Journal Year:
2024,
Volume and Issue:
16(3), P. 3368 - 3387
Published: Jan. 12, 2024
The
electrochemical
synthesis
of
syngas
(CO
and
H2)
has
garnered
considerable
attention
in
the
context
Fischer–Tropsch
(FT)
employing
thermal
catalysts.
Nonetheless,
need
for
a
novel,
cost-effective
technique
persists.
In
this
investigation,
we
introduce
direct
(dEC)
approach
FT
that
functions
under
ambient
conditions
by
utilizing
p-block
element
(Sn
In)
overlaid
Cu
electrode.
Surface
*CO
H*
species
were
obtained
an
electrolytic
medium
through
CO2
+
H+
e–
→
HOOCad
(or
CO
adsorption)
reactions,
respectively.
We
have
observed
C2–7
long-chain
hydrocarbons
with
CnH2n+2/CnH2n
ratio
1–3,
observation
can
be
explained
process
C–C
coupling
chain
growth
conventional
synthesis,
based
on
linearity
Anderson-Schulz–Flory
equation
plots.
Thick
Sn
overlayers
resulted
dominant
production
formate,
while
C2H4
found
to
proportional
inversely
correlated
H2,
C2H6,
C3–7
hydrocarbon
production.
EC
CO2/CO
reduction
used
dEC
offers
valuable
insights
into
mechanism
C2+
holds
promise
as
eco-friendly
producing
energy
environmental
purposes.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(52)
Published: Aug. 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.