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.
ACS Nano,
Journal Year:
2023,
Volume and Issue:
17(19), P. 18688 - 18705
Published: Sept. 19, 2023
Electrochemical
CO2
reduction
(ECO2R)
with
renewable
electricity
is
an
advanced
carbon
conversion
technology.
At
present,
copper
the
only
metal
to
selectively
convert
into
multicarbon
(C2+)
products.
Among
them,
atomically
dispersed
(AD)
Cu
catalysts
have
received
great
attention
due
relatively
single
chemical
environment,
which
are
able
minimize
negative
impact
of
morphology,
valence
state,
and
crystallographic
properties,
etc.
on
product
selectivity.
Furthermore,
completely
exposed
atomic
sites
not
provide
space
bonding
electrons
for
adsorption
reactants
in
favor
better
catalytic
activity
but
also
ideal
platform
studying
its
reaction
mechanism.
This
review
summarizes
recent
progress
AD
as
a
chemically
tunable
ECO2R,
including
dynamic
evolution,
performance,
prospects
challenges
ECO2R
carefully
discussed.
We
sincerely
hope
that
this
can
contribute
rational
design
enhanced
performance
ECO2R.
Small,
Journal Year:
2023,
Volume and Issue:
19(25)
Published: March 15, 2023
Electrochemical
CO2
reduction
reaction
(CO2
RR),
powered
by
renewable
electricity,
has
attracted
great
attention
for
producing
high
value-added
fuels
and
chemicals,
as
well
feasibly
mitigating
emission
problem.
Here,
this
work
reports
a
facile
hard
template
strategy
to
prepare
the
Ni@N-C
catalyst
with
core-shell
structure,
where
nickel
nanoparticles
(Ni
NPs)
are
encapsulated
thin
nitrogen-doped
carbon
shells
(N-C
shells).
The
demonstrated
promising
industrial
current
density
of
236.7
mA
cm-2
superb
FECO
97%
at
-1.1
V
versus
RHE.
Moreover,
can
drive
reversible
Zn-CO2
battery
largest
power
1.64
mW
,
endure
tough
cycling
durability.
These
excellent
performances
ascribed
synergistic
effect
that
Ni
NPs
regulate
electronic
microenvironment
N-doped
shells,
which
favor
enhance
adsorption
capacity
electron
transfer
capacity.
Density
functional
theory
calculations
prove
binding
configuration
N-C
located
on
top
slabs
(Top-Ni@N-C)
is
most
thermodynamically
stable
possess
lowest
thermodynamic
barrier
formation
COOH*
desorption
CO.
This
may
pioneer
new
method
seeking
high-efficiency
worthwhile
electrocatalysts
RR
battery.
Catalysis Today,
Journal Year:
2023,
Volume and Issue:
421, P. 114217 - 114217
Published: May 18, 2023
The
electrocatalytic
reduction
of
carbon
dioxide
(CO2RR)
is
a
crucial
technology
to
develop
the
decarbonisation
strategy
for
circularity
and
producing
solar
fuels
substituting
fossil
fuels.
This
viewpoint
discusses
role
electrode
reactor
design
as
main
factor
in
determining
performance
CO2RR,
at
least
under
reaction
conditions
relevant
industrial
scalability,
evidencing
need
overturn
current
strategic
vision
focused
more
on
improving
characteristics
materials.
Many
parameters
characterising
performances
(such
Faradaic
efficiency,
selectivity
potential
onset,
besides
density)
are
strongly
influenced
typically
dominated
(under
conditions)
by
effective
population
adspecies
surface,
which
is,
turn,
related
mass
control
transport
resistances,
local
pH
changes,
multiphase
boundaries,
wettability
other
aspects.
Even
preliminary
screening
catalysts
could
be
incorrect,
not
operating
representative
conditions,
thus
without
properly
choosing
reactor.
Advanced
electrode/reactor
designs,
e.g.,
based
gas-diffusion
electrodes
(GDEs)
that
avoid
having
liquid
electrolyte
(zero-gap
design),
necessary
improve
CO2RR
scalability
applications.
situ
catalyst
nanoparticle
reconstruction
may
depend
these
Electrochemical
characterization
methods
like
electrochemical
impedance
spectroscopy
(EIS)
right
approach
study
reactions,
providing
indications
controlling
elements
determine
electrocatalyst/electrode
performances.
Small,
Journal Year:
2024,
Volume and Issue:
20(27)
Published: Jan. 29, 2024
Abstract
Cu‐based
metal‐organic
frameworks
(MOFs)
have
attracted
much
attention
for
electrocatalytic
CO
2
reduction
to
high
value‐added
chemicals,
but
they
still
suffer
from
low
selectivity
and
instability.
Here,
an
associative
design
strategy
the
valence
coordination
environment
of
metal
node
in
MOFs
is
employed
regulate
CO2
electroreduction
ethylene.
A
novel
“reduction‐cleavage‐recrystallization”
method
developed
modulate
Cu(II)‐Trimesic
acid
(BTC)
framework
form
a
Cu(I)‐BTC
structure
enriched
with
free
carboxyl
groups
secondary
(SCE).
In
contrast
Cu(II)‐BTC,
shows
higher
catalytic
activity
better
ethylene
(≈2.2‐fold)
electroreduction,
which
further
enhanced
by
increasing
content
groups,
resulting
Faraday
efficiency
up
57%
durability
catalyst
could
last
38
h
without
performance
decline.
It
indicates
that
synergistic
effect
between
Cu(I)‐O
coordinated
considerably
enhances
dimerization
*CO
intermediates
hinders
hydrogenation
these
competitive
pathways.
This
work
unravels
strong
dependence
on
Cu
state
provides
platform
designing
highly
selective
catalysts.
