Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Авг. 2, 2024
The
sluggish
kinetics
of
Volmer
step
in
the
alkaline
hydrogen
evolution
results
large
energy
consumption.
challenge
that
has
yet
well
resolved
is
to
control
water
adsorption
and
dissociation.
Here,
we
develop
biaxially
strained
MoSe2
three
dimensional
nanoshells
exhibit
enhanced
catalytic
performance
with
a
low
overpotential
58.2
mV
at
10
mA
cm−2
base,
long-term
stable
activity
membrane-electrode-assembly
based
electrolyser
1
A
cm−2.
Compared
flat
uniaxial-strained
MoSe2,
establish
stably
adsorbed
OH
engineer
on
changes
configuration
from
O-down
Mo
O-horizontal
OH*
via
stronger
bonds.
favorable
dissociation
3-coordinated
sites
4-coordinated
constitute
tandem
electrolysis,
resulting
thermodynamically
evolution.
This
work
deepens
our
understanding
impact
strain
dimensions
inspires
design
nanostructured
catalysts
for
accelerating
rate-determining
multi-electron
reactions.
Hydroxide
most
abundant
anion
solutions,
but
its
electrolysis
remains
unclear.
Herein,
authors
report
biaxial
induced
accelerate
by
modifying
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 6257 - 6358
Опубликована: Март 21, 2023
The
oxygen
evolution
reaction
(OER)
and
reduction
(ORR)
are
core
steps
of
various
energy
conversion
storage
systems.
However,
their
sluggish
kinetics,
i.e.,
the
demanding
multielectron
transfer
processes,
still
render
OER/ORR
catalysts
less
efficient
for
practical
applications.
Moreover,
complexity
catalyst–electrolyte
interface
makes
a
comprehensive
understanding
intrinsic
mechanisms
challenging.
Fortunately,
recent
advances
in
situ/operando
characterization
techniques
have
facilitated
kinetic
monitoring
under
conditions.
Here
we
provide
selected
highlights
mechanistic
studies
with
main
emphasis
placed
on
heterogeneous
systems
(primarily
discussing
first-row
transition
metals
which
operate
basic
conditions),
followed
by
brief
outlook
molecular
catalysts.
Key
sections
this
review
focused
determination
true
active
species,
identification
sites,
reactive
intermediates.
For
in-depth
insights
into
above
factors,
short
overview
metrics
accurate
characterizations
is
provided.
A
combination
obtained
time-resolved
information
reliable
activity
data
will
then
guide
rational
design
new
Strategies
such
as
optimizing
restructuring
process
well
overcoming
adsorption-energy
scaling
relations
be
discussed.
Finally,
pending
current
challenges
prospects
toward
development
homogeneous
presented.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Июнь 17, 2023
Direct
seawater
electrolysis
is
promising
for
sustainable
hydrogen
gas
(H2)
production.
However,
the
chloride
ions
in
lead
to
side
reactions
and
corrosion,
which
result
a
low
efficiency
poor
stability
of
electrocatalyst
hinder
use
technology.
Here
we
report
corrosion-resistant
RuMoNi
electrocatalyst,
situ-formed
molybdate
on
its
surface
repel
ions.
The
works
stably
over
3000
h
at
high
current
density
500
mA
cm-2
alkaline
electrolytes.
Using
catalyst
an
anion
exchange
membrane
electrolyzer,
energy
conversion
77.9%
1000
1.72
V.
calculated
price
per
gallon
gasoline
equivalent
(GGE)
H2
produced
$
0.85,
lower
than
2026
technical
target
2.0/GGE
set
by
United
Stated
Department
Energy,
thus,
suggesting
practicability
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(38)
Опубликована: Июнь 28, 2022
Abstract
As
the
kinetically
demanding
oxygen
evolution
reaction
(OER)
is
crucial
for
decarbonization
of
our
society,
a
wide
range
(pre)catalysts
with
various
non‐active‐site
elements
(e.g.,
Mo,
S,
Se,
N,
P,
C,
Si…)
have
been
investigated.
Thermodynamics
dictate
that
these
oxidize
during
industrial
operation.
The
formed
oxyanions
are
water
soluble
and
thus
predominantly
leach
in
reconstruction
process.
Nevertheless,
recently,
it
was
unveiled
thermodynamically
stable
(oxy)anions
can
adsorb
on
surface
or
intercalate
interlayer
space
active
catalyst.
There,
they
tune
electronic
properties
sites
interact
intermediates,
changing
OER
kinetics
potentially
breaking
persisting
*OH/*OOH
scaling
relations.
Thus,
addition
to
electrolyte
opens
new
design
dimension
catalysis
herein
discussed
observations
deepen
understanding
role
anions
OER.
Advanced Materials,
Год журнала:
2023,
Номер
35(21)
Опубликована: Март 7, 2023
Nickel-iron
catalysts
represent
an
appealing
platform
for
electrocatalytic
oxygen
evolution
reaction
(OER)
in
alkaline
media
because
of
their
high
adjustability
components
and
activity.
However,
long-term
stabilities
under
current
density
still
remain
unsatisfactory
due
to
undesirable
Fe
segregation.
Herein,
a
nitrate
ion
(NO3-
)
tailored
strategy
is
developed
mitigate
segregation,
thereby
improve
the
OER
stability
nickel-iron
catalyst.
X-ray
absorption
spectroscopy
combined
with
theoretical
calculations
indicate
that
introducing
Ni3
(NO3
)2
(OH)4
stable
NO3-
lattice
conducive
constructing
interface
FeOOH/Ni3
via
strong
interaction
between
incorporated
.
Time
flight
secondary
mass
spectrometry
wavelet
transformation
analysis
demonstrate
catalyst
greatly
alleviates
exhibiting
considerably
enhanced
six-fold
improvement
over
FeOOH/Ni(OH)2
without
modification.
This
work
represents
momentous
step
toward
regulating
segregation
stabilizing
catalytic
performances
catalysts.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(24)
Опубликована: Май 4, 2023
Abstract
Compared
to
traditional
modulation
by
metal
cations
doping,
oxyanions
offer
a
higher
possibility
of
mediating
the
performance
electrocatalysts
toward
oxygen
evolution
reaction
(OER)
due
their
special
polyanion
configurations
and
large
electronegativity.
However,
mechanism
rules
mediation
remain
poorly
understood.
Herein,
an
in
situ
electrochemical
oxyanion
(NO
3
−
,
PO
4
3−
SO
2−
or
SeO
)
steering
strategy
study
variation
OER
for
transition‐metal
(TM
=
Ni,
Fe,
Co)
hydroxide
is
reported.
Electrocatalytic
experiments
indicate
both
activity
stability
oxyanion‐modified
TM
hydroxides
follow
order
>
NO
.
Electrochemical
incorporation
improves
hydroxides.
Conversely,
doping
significantly
accelerates
leaching
thus
impairs
performance.
Theoretical
calculations
reveal
that
simultaneously
modulates
TM‐O
covalency
TM‐3
d
band
centers,
correlating
with
This
research
constructs
oxyanion‐mediated
rule
designing
high‐performance
energy
transformation.
