ACS Materials Letters,
Journal Year:
2024,
Volume and Issue:
6(7), P. 2642 - 2659
Published: May 30, 2024
High-entropy
alloys
(HEAs)
contain
five
or
more
main
elements,
and
each
element
ranges
in
content
from
5%
to
35%.
Due
the
abundant
selectivity
of
excellent
structural
stability,
adjustable
active
centers,
HEAs
have
been
widely
used
electrocatalysis.
Designing
HEA
catalysts
at
atomic
scale
can
deeply
describe
their
complexity
accurately
reflect
relationship
between
structure
catalytic
performance.
In
this
Review,
design
HEA-based
electrocatalysts
is
introduced
it
evaluated
terms
activity,
selectivity,
efficiency.
Ingenuity
level
customize
composition
geometric
HEAs,
thereby
enhancing
intrinsic
activity
site,
creating
new
sites,
improving
operational
stability.
The
Review
provides
insights
into
electrocatalytic
properties
guidance
for
synthesis
advanced
viewpoint
fabrication.
Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(22), P. 12507 - 12593
Published: Nov. 1, 2023
Electrocatalysis
underpins
the
renewable
electrochemical
conversions
for
sustainability,
which
further
replies
on
metallic
nanocrystals
as
vital
electrocatalysts.
Intermetallic
have
been
known
to
show
distinct
properties
compared
their
disordered
counterparts,
and
long
explored
functional
improvements.
Tremendous
progresses
made
in
past
few
years,
with
notable
trend
of
more
precise
engineering
down
an
atomic
level
investigation
transferring
into
practical
membrane
electrode
assembly
(MEA),
motivates
this
timely
review.
After
addressing
basic
thermodynamic
kinetic
fundamentals,
we
discuss
classic
latest
synthetic
strategies
that
enable
not
only
formation
intermetallic
phase
but
also
rational
control
other
catalysis-determinant
structural
parameters,
such
size
morphology.
We
demonstrate
emerging
nanomaterials
potentially
advancement
energy
electrocatalysis.
Then,
state-of-the-art
characterizations
representative
electrocatalysts
emphasis
oxygen
reduction
reaction
evaluated
a
MEA
setup.
summarize
review
by
laying
out
existing
challenges
offering
perspective
future
research
directions
toward
practicing
conversions.
Chemical Science,
Journal Year:
2023,
Volume and Issue:
14(45), P. 12850 - 12868
Published: Jan. 1, 2023
This
review
summarizes
the
synthesis
methods,
characterization
research
progress
and
regulation
strategies
of
HAEs
in
field
electrocatalytic
HER,
HOR,
OER,
ORR,
CO
2
RR,
NRR
AOR,
providing
deep
understanding
for
future
applications.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(35)
Published: May 4, 2024
Abstract
Directly
electrochemical
conversion
of
nitrate
(NO
3
−
)
is
an
efficient
and
environmentally
friendly
technology
for
ammonia
(NH
production
but
challenged
by
highly
selective
electrocatalysts.
High‐entropy
alloys
(HEAs)
with
unique
properties
are
attractive
materials
in
catalysis,
particularly
multi‐step
reactions.
Herein,
we
first
reported
the
application
HEA
(FeCoNiAlTi)
electrocatalytic
NO
reduction
to
NH
(NRA).
The
bulk
active
NRA
limited
unsatisfied
yield
0.36
mg
h
−1
cm
−2
Faradaic
efficiency
(FE)
82.66
%.
Through
effective
phase
engineering
strategy,
uniform
intermetallic
nanoparticles
introduced
on
increase
surface
area
charge
transfer
efficiency.
resulting
nanostructured
(n‐HEA)
delivers
enhanced
performance
terms
(0.52
FE
(95.23
%).
Further
experimental
theoretical
investigations
reveal
that
multi‐active
sites
(Fe,
Co,
Ni)
dominated
electrocatalysis
over
n‐HEA.
Notably,
typical
Co
exhibit
lowest
energy
barrier
*NH
2
as
rate‐determining
step.
Advanced Science,
Journal Year:
2024,
Volume and Issue:
11(33)
Published: July 1, 2024
Abstract
Modifying
the
coordination
or
local
environments
of
single‐,
di‐,
tri‐,
and
multi‐metal
atom
(SMA/DMA/TMA/MMA)‐based
materials
is
one
best
strategies
for
increasing
catalytic
activities,
selectivity,
long‐term
durability
these
materials.
Advanced
sheet
supported
by
metal
atom‐based
have
become
a
critical
topic
in
fields
renewable
energy
conversion
systems,
storage
devices,
sensors,
biomedicine
owing
to
maximum
utilization
efficiency,
precisely
located
centers,
specific
electron
configurations,
unique
reactivity,
precise
chemical
tunability.
Several
offer
excellent
support
are
attractive
applications
energy,
medical
research,
such
as
oxygen
reduction,
production,
hydrogen
generation,
fuel
selective
detection,
enzymatic
reactions.
The
strong
metal–metal
metal–carbon
with
metal–heteroatom
(i.e.,
N,
S,
P,
B,
O)
bonds
stabilize
optimize
electronic
structures
atoms
due
interfacial
interactions,
yielding
activities.
These
provide
models
understanding
fundamental
problems
multistep
This
review
summarizes
substrate
structure‐activity
relationship
different
active
sites
based
on
experimental
theoretical
data.
Additionally,
new
synthesis
procedures,
physicochemical
characterizations,
biomedical
discussed.
Finally,
remaining
challenges
developing
efficient
SMA/DMA/TMA/MMA‐based
presented.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(20)
Published: March 20, 2024
Abstract
The
poisoning
of
undesired
intermediates
or
impurities
greatly
hinders
the
catalytic
performances
noble
metal‐based
catalysts.
Herein,
high‐entropy
intermetallics
i
‐(PtPdIrRu)
2
FeCu
(HEI)
are
constructed
to
inhibit
strongly
adsorbed
carbon
monoxide
(CO*)
during
formic
acid
oxidation
reaction.
As
probed
by
multiple‐scaled
structural
characterizations,
HEI
nanoparticles
featured
with
partially
negative
Pt
states,
diluted
Pt/Pd/Ir/Ru
atomic
sites
and
ultrasmall
average
size
less
than
nm.
Benefiting
from
optimized
structures,
deliver
more
10
times
promotion
in
intrinsic
activity
that
pure
Pt,
well‐enhanced
mass
activity/durability
ternary
‐Pt
counterpart.
In
situ
infrared
spectroscopy
manifests
both
bridge
top
CO*
favored
on
but
limited
HEI.
Further
theoretical
elaboration
indicates
displayed
a
much
weaker
binding
sluggish
diffusion
among
different
sites,
contrast
bound
was
easy
diffuse
larger
ensembles.
This
work
verifies
HEIs
promising
catalysts
via
integrating
merits
alloys.
Nano Letters,
Journal Year:
2024,
Volume and Issue:
24(9), P. 2831 - 2838
Published: Feb. 22, 2024
High-entropy
borides
hold
potential
as
electrocatalysts
for
water
oxidation.
However,
the
synthesis
of
tailored
nanostructures
remains
a
challenge
due
to
thermodynamic
immiscibility
polymetallic
components.
Herein,
FeCoCuMnRuB
nanobox
decorated
with
nanosheet
array
was
synthesized
first
time
by
"coordination-etch-reduction"
method.
The
has
various
structural
characteristics
express
catalytic
performance;
meanwhile,
it
combines
high-entropy
effect
multiple
components
electron
trap
induced
electron-deficient
B,
synergistically
regulating
its
electronic
structure.
As
result,
exhibits
enhanced
OER
activity
low
overpotential
(η10
=
233
mV),
high
TOF
value
(0.0539
s–1),
small
Tafel
slope
(61
mV/dec),
and
satisfactory
stability
200
h,
outperforming
alloy
low-entropy
borides.
This
work
develops
entropy
B-driven
strategy
motivating
performance
oxidation,
which
broadens
diversity
category
materials.
Science Advances,
Journal Year:
2024,
Volume and Issue:
10(23)
Published: June 5, 2024
Alloying
has
proven
power
to
upgrade
metallic
electrocatalysts,
while
the
traditional
alloys
encounter
limitation
for
optimizing
electronic
structures
of
surface
sites
in
a
continuous
manner.
High-entropy
(HEAs)
overcome
this
by
manageably
tuning
adsorption/desorption
energies
reaction
intermediates.
Recently,
marriage
nanotechnology
and
HEAs
made
considerable
progresses
renewable
energy
technologies,
showing
two
important
trends
size
diminishment
multidimensionality.
This
review
is
dedicated
summarizing
recent
advances
that
are
rationally
designed
electrocatalysis.
We
first
explain
advantages
as
electrocatalysts
from
three
aspects:
high
entropy,
nanometer,
multidimension.
Then,
several
structural
regulation
methods
proposed
promote
electrocatalysis
HEAs,
involving
thermodynamically
nonequilibrium
synthesis,
regulating
(sub-)nanosize
anisotropic
morphologies,
well
engineering
atomic
ordering.
The
general
relationship
between
electrocatalytic
properties
further
discussed.
Finally,
we
outline
remaining
challenges
field,
aiming
inspire
more
sophisticated
HEA-based
nanocatalysts.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(5), P. 2917 - 2923
Published: Feb. 12, 2024
Elucidating
the
relationship
between
electrocatalytic
activity
and
surface
strain
is
pivotal
for
designing
highly
efficient
electrocatalysts
acidic
hydrogen
evolution
reaction
(HER).
However,
a
general
correlation
currently
absent
due
to
lack
of
ideal
catalytic
materials
platforms
with
well-defined
structures
components.
Herein,
we
select
L10
L12
Pt-based
intermetallic
compounds
as
model
construct
series
core–shell
catalysts
strained
Pt
skins
(IMC@Pt)
establish
HER
performance.
Density
functional
theory
calculations
were
performed
determine
degree,
d-band
center,
key
descriptor
ΔGH*
HER.
By
combining
theoretical
experimental
data,
propose
volcano-type
trend
IMC@Pt
an
apex
at
4%
compressive
strain.
In
addition,
demonstrate
class
active
durable
Among
them,
Pt3V@Pt
catalyst
exhibits
highest
intrinsic
specific
4.24
mA
cmPt–2
overpotential
20
mV,
which
4
times
higher
than
that
Pt.
This
work
provides
solid
understanding
essential
nature
PtM
alloy
can
guide
design
high-performance
water
electrolyzers.