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.
Chemical Society Reviews,
Journal Year:
2022,
Volume and Issue:
51(20), P. 8676 - 8695
Published: Jan. 1, 2022
This
review
discusses
the
emerging
science
and
research
progress
underlying
electrochemical
processes
for
carbon
capture
mitigation
of
CO
2
emissions,
assesses
their
current
maturity
trajectory.
ACS Nano,
Journal Year:
2022,
Volume and Issue:
16(11), P. 19210 - 19219
Published: Oct. 18, 2022
Using
the
electrochemical
CO2
reduction
reaction
(CO2RR)
with
Cu-based
electrocatalysts
to
achieve
carbon-neutral
cycles
remains
a
significant
challenge
because
of
its
low
selectivity
and
poor
stability.
Modulating
surface
electron
distribution
by
defects
engineering
or
doping
can
effectively
improve
CO2RR
performance.
Herein,
we
synthesize
electrocatalyst
Vo-CuO(Sn)
nanosheets
containing
oxygen
vacancies
Sn
dopants
for
application
in
CO2RR-to-CO.
Density
functional
theory
calculations
confirm
that
incorporation
atoms
substantially
reduces
energy
barrier
*COOH
*CO
intermediate
formation,
which
results
high
efficiency,
overpotential,
superior
stability
CO
conversion.
This
possesses
Faraday
efficiency
(FE)
99.9%
at
overpotential
420
mV
partial
current
density
up
35.22
mA
cm-2
-1.03
V
versus
reversible
hydrogen
electrode
(RHE).
The
FECO
could
retain
over
95%
within
wide
potential
area
from
-0.48
-0.93
RHE.
Moreover,
obtain
long-term
more
than
180
h
only
slight
decay
activity.
Therefore,
this
work
provides
an
effective
route
designing
environmentally
friendly
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: April 12, 2023
Membrane
electrode
assemblies
enable
CO2
electrolysis
at
industrially
relevant
rates,
yet
their
operational
stability
is
often
limited
by
formation
of
solid
precipitates
in
the
cathode
pores,
triggered
cation
crossover
from
anolyte
due
to
imperfect
ion
exclusion
anion
exchange
membranes.
Here
we
show
that
concentration
affects
degree
movement
through
membranes,
and
this
substantially
influences
behaviors
copper
catalysts
catholyte-free
electrolysers.
Systematic
variation
(KOH
or
KHCO3)
ionic
strength
produced
a
distinct
switch
selectivity
between
either
predominantly
CO
C2+
products
(mainly
C2H4)
which
closely
correlated
with
quantity
alkali
metal
(K+)
crossover,
suggesting
cations
play
key
role
C-C
coupling
reaction
pathways
even
cells
without
discrete
liquid
catholytes.
Operando
X-ray
absorption
quasi
situ
photoelectron
spectroscopy
revealed
Cu
surface
speciation
showed
strong
dependence
on
concentration,
wherein
dilute
anolytes
resulted
mixture
Cu+
Cu0
species,
while
concentrated
led
exclusively
under
similar
testing
conditions.
These
results
cells,
effects
(including
unintentional
ones)
significantly
influence
pathways,
important
consider
future
development
devices.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(36)
Published: July 20, 2023
Abstract
We
propose
an
effective
highest
occupied
d‐orbital
modulation
strategy
engendered
by
breaking
the
coordination
symmetry
of
sites
in
atomically
precise
Cu
nanocluster
(NC)
to
switch
product
CO
2
electroreduction
from
HCOOH/CO
higher‐valued
hydrocarbons.
An
well‐defined
6
NC
with
symmetry‐broken
Cu−S
N
1
active
(named
(MBD)
,
MBD=2‐mercaptobenzimidazole)
was
designed
and
synthesized
a
judicious
choice
ligand
containing
both
S
atoms.
Different
previously
reported
high
HCOOH
selectivity
NCs
3
sites,
structure
shows
Faradaic
efficiency
toward
hydrocarbons
65.5
%
at
−1.4
V
versus
reversible
hydrogen
electrode
(including
42.5
CH
4
23
C
H
),
partial
current
density
−183.4
mA
cm
−2
.
Theoretical
calculations
reveal
that
can
rearrange
3d
orbitals
as
d‐orbital,
thus
favoring
generation
key
intermediate
*COOH
instead
*OCHO
favor
*CO
formation,
followed
hydrogenation
and/or
C−C
coupling
produce
This
is
first
attempt
regulate
mode
atom
for
generation,
provides
new
inspiration
designing
efficient
RR
towards
highly‐valued
products.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(27)
Published: April 27, 2023
Abstract
Electrolytes
have
a
profound
impact
on
the
chemical
environment
of
electrocatalysis,
influencing
reaction
rate
and
selectivity
products.
Experimental
theoretical
studies
extensively
investigated
interaction
mechanisms
between
electrolyte
ions
(i.e.,
alkali
metal
cations,
carbonate
anions)
reactants
or
catalyst
surface
in
electrocatalytic
reactions
such
as
hydrogen
evolution
reaction,
oxygen
reduction
water
oxidation
CO
2
reaction.
Past
demonstrated
noticeable
dependence
electrochemical
activity
identity
ions.
However,
few
overviews
comprehensively
specifically
discussed
effects
cations
anions
common
reactions.
In
order
to
clarify
give
more
insights
this
research
area,
review
aims
summarize
highlight
recent
progress
understanding
various
ionic
species
their
influence
diverse
for
splitting,
H
O
production,
reduction.
The
challenges
perspectives
effect
electrocatalysis
are
also
presented.
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.