Exploration,
Journal Year:
2024,
Volume and Issue:
unknown
Published: July 2, 2024
High-entropy
alloys
(HEAs)
have
attracted
significant
attention
for
electrocatalytic
energy
conversion
by
virtue
of
their
promisingly
high
efficiency,
stability,
and
low
cost.
Recently,
encouraging
progress
has
been
made
in
tuning
the
structure
composition
HEAs
used
electrolyzers
fuel
cells.
However,
understanding
on
synthetic
methods
structure-property-performance
relationship
well-defined
nanostructures
is
still
inadequate.
To
gain
insight
into
future
research
directions
electrocatalysis,
this
paper,
commonly
to
obtain
(0D
nanoparticles,
1D
nanowires,
2D
nanosheets/nanoplates,
3D
nanoporous
structures,
other
three-dimensional
morphologies)
are
first
summarized.
Then,
authors
discuss
application
several
typical
reactions,
including
hydrogen
evolution
reaction,
oxygen
reduction
alcohol
oxidation
carbon
dioxide
nitrogen
formic
acid
reaction.
Finally,
a
practical
perspective
nanostructured
electrocatalysts
provided.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(25), P. 13957 - 13967
Published: June 19, 2023
Harvesting
recyclable
ammonia
(NH3)
from
the
electrocatalytic
reduction
of
nitrate
(NO3RR)
offers
a
sustainable
strategy
to
close
ecological
nitrogen
cycle
nitration
contamination
in
an
energy-efficient
and
environmentally
friendly
manner.
The
emerging
intermetallic
single-atom
alloys
(ISAAs)
are
recognized
achieve
highest
site
density
single
atoms
by
isolating
contiguous
metal
into
sites
stabilized
another
within
structure,
which
holds
promise
couple
catalytic
benefits
nanocrystals
catalysts
for
promoting
NO3RR.
Herein,
ISAA
In-Pd
bimetallene,
Pd
isolated
surrounding
In
atoms,
is
reported
boost
neutral
NO3RR
with
NH3
Faradaic
efficiency
(FE)
87.2%,
yield
rate
28.06
mg
h-1
mgPd-1,
exceptional
stability
increased
activity/selectivity
over
100
h
20
cycles.
structure
induces
substantially
diminished
overlap
d-orbitals
narrowed
p-d
hybridization
In-p
Pd-d
states
around
Fermi
level,
resulting
stronger
NO3-
adsorption
depressed
energy
barrier
potential-determining
step
Further
integrating
catalyst
Zn-NO3-
flow
battery
as
cathode
delivers
power
12.64
mW
cm-2
FE
93.4%
production.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(10), P. 5710 - 5717
Published: March 6, 2023
Hydride
metallenes
show
great
potential
for
hydrogen-related
catalytic
applications
due
to
favorable
electronic
structures
modulated
by
interstitial
hydrogen
atoms
and
large
active
surface
areas
of
metallenes.
Metallene
nanostructures
generally
have
compressive
strain
relative
bulk,
which
can
affect
both
the
stability
behavior
hydride
but
in
general
cannot
be
controlled.
Here,
we
demonstrate
highly
stable
PdHx
with
a
tensile
strained
Ru
layer
reveal
spatial
confinement
effect
skin
multiple
spectroscopic
characterizations
molecular
dynamics
simulations.
These
PdHx@Ru
4.5%
expanded
outer
exhibit
outstanding
alkaline
evolution
reaction
activity
low
overpotential
30
mV
at
10
mA
cm-2
robust
negligible
decay
after
10,000
cycles,
are
superior
commercial
Pt/C
most
reported
Ru-based
electrocatalysts.
Control
experiments
first-principles
calculations
that
lowers
energy
barrier
H2O
dissociation
provides
moderate
adsorption
energy.
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
33(42)
Published: June 14, 2023
Abstract
Designing
the
high‐entropy
alloys
(HEAs)
electrocatalysts
with
controllable
nanostructures
is
of
great
significance
for
development
efficient
alkaline
hydrogen
evolution
reaction
(HER)
electrocatalysts.
In
this
study,
an
ultrathin
HEA‐PdPtRhIrCu
metallene
abundant
lattice
distortions
and
defects
prepared
via
a
facile
one‐step
hydrothermal
method.
The
synthesized
exhibits
superior
HER
performance
in
1
m
KOH
solution,
where
required
overpotential
only
15
mV
to
reach
current
density
−10
mA
cm
−2
while
possessing
low
Tafel
slope
37
dec
−1
.
Density
functional
theory
calculations
further
prove
that
synergistic
effect
five
elements
can
optimize
electronic
structure
enhance
activity
catalysts.
particular,
strong
coupling
bonding
arising
from
interaction
between
multi‐metal
components
facilitate
electron
transfer
surface
high
electroactivity.
Moreover,
optimized
Pt
promotes
optimal
PtH
binding
at
site,
thus
promoting
performance.
ACS Catalysis,
Journal Year:
2023,
Volume and Issue:
13(15), P. 10394 - 10404
Published: July 25, 2023
Electrochemical
reformation
of
nitrate
wastewater
and
poly(ethylene
terephthalate)
(PET)
plastic
waste
into
ammonia
(NH3)
fine
chemicals
is
a
sustainable
strategy
for
resource
utilization.
Herein,
co-production
system
glycolic
acid
(GA,
degradable
polymer
monomer)
constructed
by
coupling
reduction
ethylene
glycol
(EG,
in
PET
hydrolysate)
oxidation.
Low-crystalline
CoOOH
(LC-CoOOH/CF)
Pd
nanothorns
(Pd
NTs/NF)
grown
situ
on
the
metal
foam
substrates
are
employed
as
cathode
anode,
respectively.
The
high
density
amorphous
regions
LC-CoOOH/CF
enables
enhanced
adsorption
provides
abundant
active
sites,
ultimately
leading
to
an
Faradic
efficiency
(FE)
97.38
±
1.0%
at
−0.25
V
vs
reversible
hydrogen
electrode
(RHE).
Meanwhile,
unique
nanothorn
morphology
endows
NTs/NF
with
high-curvature
tip,
triggering
tip
effect
(TE)
promote
highly
selective
oxidation
EG
GA.
Furthermore,
two-electrode
system,
NH3
GA
operated
low
energy
consumption
(onset
voltage:
0.5
V),
much
lower
than
traditional
electrolysis
process
(1.4
V).
This
study
method
utilization
co-produce
value-added
chemicals.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(25)
Published: Jan. 30, 2024
Abstract
Oxygen
vacancy
engineering
is
a
promising
strategy
to
enhance
the
electrocatalytic
activities
in
conventional
metal
oxide
electrocatalysts.
However,
utilization
of
oxygen
vacancies
high‐entropy
oxides
remains
unknown,
primarily
due
challenges
associated
with
facile
introduction
and
explanation
their
roles
complex
systems.
Herein,
into
realized
unique
high
entropy‐driven
role
for
evolution
reaction
(OER)
process
revealed.
A
low‐temperature
surface
carbonization–decarbonization
approach
developed
introduce
regulate
spinel
(HEOs).
The
HEOs
can
both
facilitate
pre‐oxidation
faster
OH
−
adsorption
induce
bridge
site
pathway
easier
deprotonation,
distinctive
where
favor
*
yet
hinder
deprotonation.
Consequently,
as‐prepared
(HEOs‐Ov)
exhibit
superior
OER
activities,
outperforming
most
reported
oxide‐based
Besides,
this
universal
method
be
extended
other
different
configuration
entropies
scaled
up.
work
paves
way
exploration
toward
electrocatalysis
fields.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: July 28, 2024
Abstract
Electro‐reforming
of
poly(ethylene
terephthalate)
(PET)
into
valuable
chemicals
is
garnering
significant
attention
as
it
opens
a
mild
avenue
for
waste
resource
utilization.
However,
achieving
high
activity
and
selectivity
C2
products
during
ethylene
glycol
(EG)
oxidation
in
PET
hydrolysate
on
Pd
electrocatalysts
remains
challenging.
The
strong
interaction
between
carbonyl
(*CO)
intermediates
leads
to
undesirable
over‐oxidation
poisoning
sites,
which
hinders
the
highly
efficient
production.
Herein,
nonmetallic
alloying
strategy
employed
fabricate
Pd‐boron
alloy
aerogel
(PdB),
wherein
B
atoms
are
induced
regulate
electron
structure
surface
oxophilicity.
This
approach
allows
remarkable
mass
6.71
A
mg
−1
,
glycolic
acid
(GA)
Faradaic
efficiency
(FE)
93.8%,
stable
100
h
cyclic
electrolysis.
In
situ
experiments
density
functional
theory
calculations
reveal
contributions
inserted
lattice
effective
EG‐to‐GA
conversion.
Interestingly,
heightened
oxophilicity
regulated
electronic
by
incorporation
weakened
*CO
adsorption
enhanced
hydroxyl
species
affinity
accelerate
oxidative
*OH
adspecies
formation,
thereby
synergistically
avoiding
boosting
GA
synthesis.
work
provides
insights
rational
design
high‐performance
synthesis
via
an
oxophilic
motifs
strategy.