SusMat,
Год журнала:
2023,
Номер
3(6), С. 730 - 748
Опубликована: Ноя. 15, 2023
Abstract
Two‐dimensional
(2D)
high‐entropy
alloys
(HEAs)
have
emerged
as
promising
electrocatalysts
due
to
the
benefits
of
polymetallic
coordination
and
robust
electrical
conductivity.
However,
multiple
elements
in
2D
HEAs
pose
challenges
achieving
a
uniform
composition
maintaining
limit
morphology,
complicating
their
structural
characterization.
Furthermore,
even
minor
adjustments
can
significantly
alter
properties
HEAs,
underscoring
need
for
deeper
understanding
structure–property
relationships
advance
synthesis
application.
Therefore,
this
review
critically
examines
intrinsic
factors
influencing
methods
practical
applications
electrocatalysis
sustainable
energy
conversion.
The
urgency
is
emphasized
developing
new
techniques,
enhancing
advanced
characterization
methods,
gaining
profound
insights
into
functional
mechanisms
HEAs.
Proceedings of the National Academy of Sciences,
Год журнала:
2024,
Номер
121(30)
Опубликована: Июль 16, 2024
High-entropy
compounds
have
been
emerging
as
promising
candidates
for
electrolysis,
yet
their
controllable
electrosynthesis
strategy
remains
a
formidable
challenge
because
of
the
ambiguous
ionic
interaction
and
codeposition
mechanism.
Herein,
we
report
oxygenates
directionally
induced
electrodeposition
to
construct
high-entropy
materials
with
amorphous
features,
on
which
structural
evolution
from
phosphide
oxide
is
confirmed
by
introducing
vanadate,
thus
realizing
simultaneous
optimization
composition
structure.
The
representative
P-CoNiMnWVO
x
shows
excellent
bifunctional
catalytic
performance
toward
alkaline
hydrogen
reaction
ethanol
oxidation
(EOR),
small
potentials
−168
mV
1.38
V
at
100
mA
cm
−2
,
respectively.
In
situ
spectroscopy
illustrates
that
electrochemical
reconstruction
induces
abundant
Co–O
species
main
active
EOR
follows
conversion
pathway
C
2
product.
Theoretical
calculations
reveal
optimized
electronic
structure
adsorption
free
energy
intermediates
thereby
resulting
in
facilitated
kinetic
process.
A
membrane-free
electrolyzer
delivers
both
high
Faradaic
efficiencies
acetate
H
over
95%
superior
stability
at100
during
120
h
electrolysis.
addition,
unique
advantages
endow
multifunctional
activity
realize
multipathway
formate-coupled
production.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(17)
Опубликована: Янв. 17, 2024
Abstract
Understanding
and
modulating
the
unique
electronic
interaction
between
single‐metal
atoms
high
entropy
compounds
are
of
great
significance
to
enable
their
high‐efficiency
oxygen
electrocatalysis
for
aprotic
lithium‐oxygen
(Li‐O
2
)
batteries.
Herein,
a
novel
bi‐functional
electrocatalyst
is
first
time
created
by
immobilizing
single‐atom
ruthenium
(Ru)
on
lanthanum‐based
perovskite
oxide
La(Mn
0.2
Co
Fe
Ni
Cr
)O
3
(Ru@HEPO),
which
demonstrates
activity
stability
in
Li‐O
The
heteronuclear
coordination
Ru
HEPO
facilitates
fast
electron
transfer
from
establishing
Ru‐O‐M
(M
stands
Mn,
Co,
Fe,
Ni)
bridges,
well
redistributes
electrons
within
Ru@HEPO
hence
significantly
improving
its
interfacial
charge
kinetics
electrocatalytic
activity.
Additionally,
strong
coupling
Mn
enhances
hybridization
3d
O
2p
orbitals,
promotes
inherent
affinity
toward
LiO
intermediate,
thereby
reducing
reaction
energy
barrier
electrode.
As
result,
Ru@HEPO‐based
batteries
deliver
remarkable
electrochemical
performances,
such
as
efficiency
(87.3%
at
100
mA
g
−1
),
excellent
rate
capability
(low
overpotential
0.52
V
durable
cyclability
(345
cycles
300
).
This
work
opens
up
promising
avenue
development
entropy‐based
electrocatalysts
precisely
tailoring
distributions
an
atomic
scale.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(17), С. 9933 - 9961
Опубликована: Янв. 1, 2024
Nano-sized
high
entropy
alloy
(HEA)
catalysts
have
attracted
much
attention
as
extraordinary
electrocatalysts
in
water-splitting
applications,
i.e.
,
the
hydrogen
evolution
reaction
(HER)
and
oxygen
(OER).
Materials Today Catalysis,
Год журнала:
2024,
Номер
4, С. 100039 - 100039
Опубликована: Янв. 17, 2024
Electrocatalysis
plays
a
crucial
role
in
the
conversion
and
storage
of
renewable
energy,
offering
significant
potential
for
addressing
energy
crisis
environmental
concerns.
High-entropy
oxides
(HEOs),
class
emerging
functional
materials,
have
gained
increasing
attention
electrocatalysis
due
to
their
stable
crystal
structure,
exceptional
geometric
compatibility,
unique
electronic
balance
factors,
abundant
active
sites.
In
this
comprehensive
review,
we
present
recent
advancements
utilizing
HEOs
as
catalysts
various
energy-based
electrocatalytic
reactions.
We
begin
with
an
overview
that
includes
definitions,
fundamental
properties,
theoretical
investigations.
Subsequently,
describe
different
synthetic
methods
while
highlighting
two
newly-developed
techniques.
Furthermore,
extensively
discuss
developments
HEO-based
electrocatalysts
diverse
structures
such
rock-salt-type,
rutile-type,
spinel-type,
perovskite-type,
other
specially-structured
HEOs.
Special
emphasis
is
placed
on
designed
strategies
aimed
at
enhancing
performance
exploring
correlations
between
structure/
composition
performance.
Finally,
provide
concluding
remarks
along
perspectives
future
opportunities
exciting
field.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(27), С. 16815 - 16830
Опубликована: Янв. 1, 2024
The
photocatalytic
application
of
magnetic
high
entropy
oxide
nanoparticles
in
water
and
wastewater
treatment
processes
is
exemplified
for
the
first
time,
purely
from
a
practical
perspective.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(22)
Опубликована: Апрель 20, 2023
Abstract
The
oxygen
evolution
reaction
(OER)
is
a
crucial
process
in
electrochemical
water
splitting,
promising
technology
to
renewably
yield
hydrogen
gas
from
water.
Designing
and
developing
earth‐abundant,
efficient,
stable
OER
electrocatalysts
replace
the
most
widely
used
but
scarce
RuO
2
IrO
are
thus
of
critical
interest.
Recently,
ABO
3
‐structured
perovskite
oxides,
especially
rare‐earth
nickelates,
extensively
studied
for
their
potential
use
as
electrocatalysts.
In
particular,
epitaxial
synthesis
complex
oxide
thin
films
allows
flexible
precise
control
over
materials
so
that
structure–stability–property
relationships
can
be
established.
Using
nickelate
model
systems,
this
review
illustrates
how
design
researchers
test
different
hypotheses
proposed
descriptors,
well
formulate
new
principles.
Following
brief
introduction
background
mechanisms,
activity
methods,
various
strategies
surveyed
including
strain
tuning,
composition
control,
surface
termination/orientation
selection,
defect
engineering,
interface
design.
These
have
led
atomic
structures
electronic
properties
nickelates
which
turn
determine
performance.
Finally,
remaining
challenges
perspectives
toward
deeper
understanding
oxides
catalysts
discussed.