Angewandte Chemie,
Год журнала:
2024,
Номер
136(39)
Опубликована: Июль 2, 2024
Abstract
Developing
non‐platinum
group
metal
catalysts
for
the
sluggish
hydrogen
oxidation
reaction
(HOR)
is
critical
alkaline
fuel
cells.
To
date,
Ni‐based
materials
are
most
promising
candidates
but
still
suffer
from
insufficient
performance.
Herein,
we
report
an
unconventional
hcp/fcc
Ni
(u‐
Ni)
heteronanocrystal
with
multiple
epitaxial
heterointerfaces
and
coherent
twin
boundaries,
generating
rugged
surfaces
plenty
of
asymmetric
convex
sites.
Systematic
analyses
discover
that
such
sites
enable
adsorption
*H
in
unusual
bridge
positions
weakened
binding
energy,
circumventing
over‐strong
on
traditional
hollow
positions,
simultaneously
stabilizing
interfacial
2
O.
It
thus
synergistically
optimizes
HOR
thermodynamic
process
as
well
reduces
kinetic
barrier
rate‐determining
Volmer
step.
Consequently,
developed
u‐
exhibits
top‐rank
activity
a
mass
40.6
mA
mg
−1
(6.3
times
higher
than
fcc
control)
together
superior
stability
high
CO‐tolerance.
These
results
provide
paradigm
designing
high‐performance
by
shifting
state
intermediates
through
configuring
surface
ACS Applied Nano Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 18, 2024
The
development
of
highly
effective
and
durable
catalysts
for
the
hydrogen
evolution
reaction
(HER)
using
abundant
earth
materials
is
crucial
advancing
economy.
In
this
work,
we
present
an
approach
synthesizing
two-dimensional
(2D)
combined
phase
with
tunable
catalytic
magnetic
properties.
We
successfully
synthesized
ferromagnetic
pristine
pyrite
(FeS2)
nanoparticles
(NPs)
hybrid
2D
troilite
(FeS)
nanosheets
utilizing
hot-filament
metal–chemical
vapor
deposition
(HFMCVD)
technique.
mixed
FeS/FeS2
exhibited
exceptional
HER
performance,
achieving
a
low
overpotential
40
mV
at
10
mA·cm–2
current
density.
Additionally,
saturation
moments
were
significantly
higher
compared
to
FeS2
NPs.
This
increase
attributed
density
unpaired
electrons
spins
in
materials.
These
enhanced
properties
facilitate
more
efficient
electron
transfer,
leading
superior
performance
overpotentials
during
HER.
material
holds
promise
as
electrocatalyst
next-generation
water
splitting
well
energy
conversion
applications.
Moreover,
our
computational
results
based
on
DFT
are
consistent
experimental
findings.
Angewandte Chemie,
Год журнала:
2024,
Номер
136(39)
Опубликована: Июль 2, 2024
Abstract
Developing
non‐platinum
group
metal
catalysts
for
the
sluggish
hydrogen
oxidation
reaction
(HOR)
is
critical
alkaline
fuel
cells.
To
date,
Ni‐based
materials
are
most
promising
candidates
but
still
suffer
from
insufficient
performance.
Herein,
we
report
an
unconventional
hcp/fcc
Ni
(u‐
Ni)
heteronanocrystal
with
multiple
epitaxial
heterointerfaces
and
coherent
twin
boundaries,
generating
rugged
surfaces
plenty
of
asymmetric
convex
sites.
Systematic
analyses
discover
that
such
sites
enable
adsorption
*H
in
unusual
bridge
positions
weakened
binding
energy,
circumventing
over‐strong
on
traditional
hollow
positions,
simultaneously
stabilizing
interfacial
2
O.
It
thus
synergistically
optimizes
HOR
thermodynamic
process
as
well
reduces
kinetic
barrier
rate‐determining
Volmer
step.
Consequently,
developed
u‐
exhibits
top‐rank
activity
a
mass
40.6
mA
mg
−1
(6.3
times
higher
than
fcc
control)
together
superior
stability
high
CO‐tolerance.
These
results
provide
paradigm
designing
high‐performance
by
shifting
state
intermediates
through
configuring
surface