Nature Communications,
Год журнала:
2025,
Номер
16(1)
Опубликована: Март 21, 2025
Electrosynthesis
of
acetate
from
carbon
monoxide
(CO)
powered
by
renewable
electricity
offers
one
promising
avenue
to
obtain
valuable
carbon-based
products
but
undergoes
unsatisfied
selectivity
because
the
competing
hydrogen
evolution
reaction.
We
report
here
a
cerium
single
atoms
(Ce-SAs)
modified
crystalline-amorphous
dual-phase
copper
(Cu)
catalyst,
in
which
Ce
SAs
reduce
electron
density
Cu,
lowering
proportion
interfacial
K+
ion
hydrated
water
(K·H2O)
and
thereby
decreasing
H*
coverage
on
catalyst
surface.
Meanwhile,
transfer
Cu
yields
Cu+
species,
boost
formation
active
atop-adsorbed
*CO
(COatop),
improving
COatop-COatop
coupling
kinetics.
These
together
lead
preferential
pathway
ketene
intermediate
(*CH2-C=O)
formation,
then
reacts
with
OH-
enriched
pulsed
electrolysis
generate
acetate.
Using
this
we
achieve
high
Faradaic
efficiency
71.3
±
2.1%
toward
time-averaged
current
110.6
2.0
mA
cm−2
under
mode.
Furthermore,
flow-cell
reactor
assembled
can
produce
steadily
for
at
least
138
hours
greater
than
60%.
CO
using
faces
low
selectivity.
Here,
authors
atom
modulated
where
tailor
structure,
enabling
highly
selective
CO-to-acetate
conversion
electrolysis.
Nano Letters,
Год журнала:
2024,
Номер
24(23), С. 6957 - 6964
Опубликована: Май 28, 2024
Highly
active
and
robust
Pt-based
electrocatalysts
for
an
oxygen
reduction
reaction
(ORR)
are
of
crucial
significance
the
development
proton
exchange
membrane
fuel
cells
(PEMFCs).
Herein,
high-loading
well-dispersive
Pt
clusters
on
graphitic
carbon-supported
CeO2
with
abundant
vacancies
(PtAC/CeO2-OV@GC)
were
successfully
fabricated
by
a
molten-salt
electrochemical-assisted
method.
The
bonding
highly
electronegative
O
induces
charge
redistribution
through
Pt–O–Ce
structure,
thus
reducing
adsorption
energies
oxygen-containing
species.
Such
PtAC/CeO2-OV@GC
electrocatalyst
exhibits
greatly
enhanced
ORR
performance
mass
activity
0.41
±
0.02
A·mg–1Pt
at
0.9
V
versus
reversible
hydrogen
electrode,
which
is
2.7
times
value
commercial
Pt/C
catalyst
shows
negligible
decay
after
20000
cycles
accelerated
degradation
tests.
It
anticipated
that
this
work
will
provide
enlightening
guidance
controllable
synthesis
rational
design
high-performance
PEMFCs.
Journal of Materials Chemistry A,
Год журнала:
2023,
Номер
11(45), С. 24823 - 24835
Опубликована: Янв. 1, 2023
Core–shell
structure
of
Cu
2
O
constructed
by
carbon
quantum
dots
exhibited
high
discharge
specific
capacity
and
excellent
rate
performance.
And
the
conversion-type
zinc
storage
mechanism
was
confirmed
in
situ
XRD
Raman
technology.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(37)
Опубликована: Июнь 24, 2024
Spin
state
is
often
regarded
as
the
crucial
valve
to
release
reactivity
of
energy-related
catalysts,
yet
it
also
challenging
precisely
manipulate,
especially
for
active
center
ions
occupied
at
specific
geometric
sites.
Herein,
a
π-π
type
orbital
coupling
3d
(Co)-2p
(O)-4f
(Ce)
was
employed
regulate
spin
octahedral
cobalt
sites
(Co
ACS Applied Materials & Interfaces,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 20, 2025
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
