ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
15(2), P. 768 - 779
Published: Dec. 25, 2024
Effective
local
electron
regulation
in
ruthenium-based
catalysts
acidic
oxygen
evolution
reactions
(OER)
remains
a
key
challenge.
The
lack
of
unified
understanding
catalyst
activity
and
stability
based
on
limits
the
further
development
proton
exchange
membrane
water
electrolysis
(PEMWE).
In
this
study,
we
develop
concept
coordination
unsaturated
Ti
(TiOCU)
sites.
Based
constructed
dual-oxide
heterojunction
interface
Ru/TiOx
catalyst,
achieve
precise
modulation
d-electron
orbitals
Ru
charge
redistribution
between
Ru–Obridge–TiOCU
units
strengthened
Ru–O
bonds
suppresses
formation
high-valence
species
deactivation
catalyst.
Combined
with
density
functional
theory
(DFT)
calculations
situ
spectroscopic
experiments,
confirm
that
dz2
orbital
significantly
optimizes
deprotonation
process
interfacial
hydroxyl-rich
interface,
thereby
enhancing
OER
kinetics
dominance
adsorbed
mechanism
(AEM).
Consequently,
exhibits
superior
performance,
achieving
current
10
mA/cm2
at
an
overpotential
only
237
mV
0.5
M
H2SO4,
demonstrates
for
over
160
h.
This
work
reveals
application
TiOCU,
providing
perspective
transition
metal
defect
materials
electrolysis.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 30, 2024
Abstract
The
development
of
efficient
and
durable
electrocatalysts
for
the
acidic
oxygen
evolution
reaction
(OER)
is
essential
advancing
renewable
hydrogen
energy
technology.
However,
slow
deprotonation
kinetics
oxo‐intermediates,
involving
four
proton‐coupled
electron
steps,
hinder
OER
progress.
Herein,
a
RuTiO
x
solid
solution
electrocatalyst
investigated,
which
features
bridged
(O
bri
)
sites
that
act
as
proton
acceptors,
accelerating
oxo‐intermediates.
Electrochemical
tests,
infrared
spectroscopy,
density
functional
theory
results
reveal
moderate
adsorption
on
O
facilitates
fast
through
adsorbate
mechanism.
This
process
effectively
prevents
over‐oxidation
deactivation
Ru
caused
by
lattice
Consequently,
shows
low
overpotential
198
mV
at
10
mA
cm
−2
geo
performance
exceeding
1400
h
50
with
negligible
deactivation.
These
insights
into
mechanism
structure‐function
relationship
are
crucial
advancement
catalytic
systems.
Small,
Journal Year:
2024,
Volume and Issue:
20(46)
Published: Aug. 9, 2024
Abstract
The
seawater
electrolysis
to
produce
hydrogen
is
a
significant
topic
on
alleviating
the
energy
crisis.
Here,
Fe,
Nb‐Ni
3
S
2
catalyst
prepared
by
metal‐doping
strategy,
and
it
shows
high
oxygen
evolution
reaction
(OER)
activity
in
alkaline
medium,
only
needs
1.491
V
deliver
current
density
of
100
mA
cm
−2
simulated
seawater.
Using
as
bifunctional
catalyst,
two‐electrode
electrolyzer
requires
voltage
1.751
(without
impedance
compensation)
drive
50
,
can
run
over
150
h
stably
Importantly,
In
situ
Raman
test
demonstrates
that
outstanding
performance
ascribed
formed
sulfate
protective
layer
induced
Nb
doping,
which
effectively
inhibit
corrosion
chloride
ion,
while
absent
for
Fe‐Ni
.
stable
operation
under
industrial
further
confirms
stability
improvement
mechanism
forming
layer.
short,
this
study
provides
new
strategy
using
dopants
inducing
formation
enhance
electrolysis.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
15(2), P. 768 - 779
Published: Dec. 25, 2024
Effective
local
electron
regulation
in
ruthenium-based
catalysts
acidic
oxygen
evolution
reactions
(OER)
remains
a
key
challenge.
The
lack
of
unified
understanding
catalyst
activity
and
stability
based
on
limits
the
further
development
proton
exchange
membrane
water
electrolysis
(PEMWE).
In
this
study,
we
develop
concept
coordination
unsaturated
Ti
(TiOCU)
sites.
Based
constructed
dual-oxide
heterojunction
interface
Ru/TiOx
catalyst,
achieve
precise
modulation
d-electron
orbitals
Ru
charge
redistribution
between
Ru–Obridge–TiOCU
units
strengthened
Ru–O
bonds
suppresses
formation
high-valence
species
deactivation
catalyst.
Combined
with
density
functional
theory
(DFT)
calculations
situ
spectroscopic
experiments,
confirm
that
dz2
orbital
significantly
optimizes
deprotonation
process
interfacial
hydroxyl-rich
interface,
thereby
enhancing
OER
kinetics
dominance
adsorbed
mechanism
(AEM).
Consequently,
exhibits
superior
performance,
achieving
current
10
mA/cm2
at
an
overpotential
only
237
mV
0.5
M
H2SO4,
demonstrates
for
over
160
h.
This
work
reveals
application
TiOCU,
providing
perspective
transition
metal
defect
materials
electrolysis.