Scientific Reports,
Journal Year:
2025,
Volume and Issue:
15(1)
Published: Jan. 14, 2025
Abstract
Gold-based
(Au)
nanostructures
are
efficient
catalysts
for
CO
oxidation,
hydrogen
evolution
(HER),
and
oxygen
(OER)
reactions,
but
stabilizing
them
on
graphene
(Gr)
is
challenging
due
to
weak
affinity
from
delocalized
$$p_{z}$$
carbon
orbitals.
This
study
investigates
forming
metal
alloys
enhance
stability
catalytic
performance
of
Au-based
nanocatalysts.
Using
ab
initio
density
functional
theory,
we
characterize
$${\text
{M}_{(n-x)}\text
{Au}_{x}}$$
sub-nanoclusters
(M
=
Ni,
Pd,
Pt,
Cu,
Ag)
with
atomicities
$$n=1-4$$
,
both
in
gas-phase
supported
Gr.
We
find
that
M
atoms
act
as
“anchors,”
enhancing
binding
Gr
modulating
efficiency.
Notably,
{Pt}_{(n-x)}\text
/Gr
shows
improved
stability,
segregation
tendencies
mitigated
upon
adsorption
The
d
-band
center
(
$$\varepsilon
_{\text
{d}}$$
)
model
indicates
potential,
correlating
an
optimal
range
$$-1
\text
{
}-2$$
eV
HER
OER
catalysts.
Incorporating
Au
into
$${\text{M}_n}$$
adjusts
closer
the
Fermi
level,
especially
Group-10
alloys,
offering
designs
efficiency
comparable
pure
Our
methodology
leveraged
SimStack,
a
workflow
framework
enabling
modeling
analysis,
reproducibility,
accelerating
discovery.
work
demonstrates
SimStack’s
pivotal
role
advancing
understanding
composition-dependent
properties
Au-alloy
clusters,
providing
systematic
approach
optimize
metal-support
interactions
applications.
Energy & Fuels,
Journal Year:
2024,
Volume and Issue:
38(21), P. 20791 - 20806
Published: Oct. 18, 2024
Creating
cost-effective,
chemically
stable
electrocatalysts
to
improve
the
hydrogen
evolution
reaction
(HER)
and
oxygen
(OER)
remains
a
major
challenge
in
electrocatalytic
water
splitting.
We
synthesized
highly
efficient
NiFe-layered
double
hydroxide
(LDH)
electrocatalyst
using
solvent-free
method.
The
formation
of
well-interconnected
metal
ions
with
nanospherical
architectures
created
an
extensive
electrochemically
active
surface
area
enriched
catalytically
sites,
demonstrating
synergistic
effects.
Preserving
suitable
stoichiometric
ratio,
such
as
Ni6Fe4LDH,
was
crucial
enhancing
catalytic
performance
for
both
HER
OER.
optimal
Ni6Fe4LDH
ratio
established
overpotentials
167
mV
(112
dec–1)
280
(116
OER,
attaining
10
mA
cm–2
current
density
1
M
KOH.
Moreover,
demonstrated
impressive
robustness,
up
90
h
minor
decrease
4.1
4.6%
Notably,
bifunctional
two-electrode
arrangement
Ni6Fe4LDH/NF||Ni6Fe4LDH/NF,
effective
electrolysis
accomplished,
preserving
at
bias
1.64
V
over
140
h,
slight
loss
3.9%
density.