Journal of the American Chemical Society,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 4, 2024
The
pursuit
of
precision
in
the
engineering
metal
nanoparticle
assemblies
has
long
fascinated
scientists,
but
achieving
atomic-level
accuracy
continues
to
pose
a
significant
challenge.
This
research
sheds
light
on
hierarchical
assembly
processes
two
high-nuclearity
Cu(I)
nanoclusters
(NCs).
By
employing
multiligand
cooperative
stabilization
strategy,
we
have
isolated
series
thiacalix[4]arene
(TC4A)/alkynyl
coprotected
NCs
(
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 28, 2025
Abstract
Electrode‐electrolyte
interfacial
modification
by
hydrophobic
molecules
represents
a
promising
strategy
for
suppressing
competing
proton
reduction
in
acidic
electrocatalytic
carbon
dioxide
reactions
(CO
2
RR),
meanwhile
sacrificing
extra
overpotential
due
to
increased
ohmic
resistance.
Herein,
multifunctional
conductive
polymer,
polyaniline
modified
p‐aminobenzenesulfonic
acid
(ABSA‐polyaniline),
is
constructed
between
Cu
catalyst
layer
and
electrolyte
simultaneously
create
an
ideal
microenvironment
CO
RR
enhance
the
charge
transfer
ion
transport
processes
at
electrochemical
reaction
interface.
This
polymer
balances
local
hydrophobicity,
promotes
adsorption
activation,
regulates
mass
of
K
+
,
H
OH
−
ions,
thus
significantly
enhancing
kinetics
medium,
yielding
high
Faraday
efficiency
(FE
=
81%)
multicarbon
products
600
mA
cm
−2
.
More
importantly,
compared
with
commonly
used
molecules,
nature
ABSA‐PANI
helps
reduce
resistance
electrode,
leading
notably
lowered
cathode
industrial‐grade
current
density
improve
energy
over
wide
potential
window.
work
sheds
light
on
development
highly
efficient
systems,
especially
those
low
alkali
cation
concentrations
concentrations.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 4, 2025
Understanding
the
effect
of
internal
atoms
in
metal
nanoparticles
on
heterogeneous
catalytic
processes
is
crucial
for
achieving
high
activity
and
selectivity.
This
requires
meticulous
synthetic
control
over
size,
composition,
atomic
arrangement
nanoparticles.
Here,
we
report
design
ligand-exchange-induced
structure
transformation
nanomolecule-templated
atomic-level
galvanic
exchange
strategies
to
synthesize
PtAg24(IPBT)18
(denoted
as
PtAg24)
AuAg24(IPBT)18
AuAg24)
nanoclusters
(NCs).
Both
NCs
exhibit
identical
total
atom
ligand
(IPBT:
2-isopropylbenzenethiolate)
counts,
well
structure,
except
difference
core
(Pt
Au).
Using
these
model
NCs,
uncover
impact
heterocore
electrochemical
CO2
reduction
reaction
(eCO2RR)
The
central
Pt
PtAg24
less
favorable
eCO2RR
activity,
with
an
approximately
4
times
smaller
than
that
Au
AuAg24.
product
CO
selectivity
<30%
PtAg24,
while
it
exceeds
70%
AuAg24,
revealing
critical
role
surface
pathways.
Furthermore,
AuAg24
exhibits
a
partial
current
density
-202.2
mA
cm-2,
stability
24
h,
retaining
90%
membrane
electrode
assembly
configuration.
Operando
spectroscopy
functional
theory
calculations
suggest
weaker
adsorption
*CO
intermediates
energy
barrier
facilitate
production
compared
providing
valuable
atomistic
insights
into
mechanism.
findings
this
work
will
inspire
more
atomically
precise
nanocatalysts
explore
their
remarkable
features
renewable
conversion
storage.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 4, 2024
The
pursuit
of
precision
in
the
engineering
metal
nanoparticle
assemblies
has
long
fascinated
scientists,
but
achieving
atomic-level
accuracy
continues
to
pose
a
significant
challenge.
This
research
sheds
light
on
hierarchical
assembly
processes
two
high-nuclearity
Cu(I)
nanoclusters
(NCs).
By
employing
multiligand
cooperative
stabilization
strategy,
we
have
isolated
series
thiacalix[4]arene
(TC4A)/alkynyl
coprotected
NCs
(
