ACS Catalysis,
Год журнала:
2023,
Номер
13(20), С. 13804 - 13815
Опубликована: Окт. 12, 2023
Rare
earth-based
alloy
nanostructures
show
great
potential
as
materials
in
the
hydrogen
evolution
reaction
(HER),
and
they
have
a
relatively
negative
enthalpy
of
formation
compared
to
traditional
transition
metal
alloys,
which
resist
dissolution
alloys
reaction.
In
addition,
liner
relationship
can
be
observed
d-band
filling
electrochemical
activity.
Therefore,
rare
nanostructure
contains
advantages
transmission
catalysts
performs
better
selectivity
stability.
However,
reduction
potentials
earth
(RE)
group
are
relevantly
low,
typically
less
than
−1.9
V,
synthesis
methods
RE
very
important.
this
Perspective,
we
generalize
preparation
method
their
applications
related
Through
recent
research
on
reaction,
future
development
direction
is
pointed
out.
Advanced Materials,
Год журнала:
2023,
Номер
35(41)
Опубликована: Июль 1, 2023
By
providing
dual
active
sites
to
synergistically
accelerate
H2
O
dissociation
and
H+
reduction,
ordered
intermetallic
alloys
usually
show
extraordinary
performance
for
pH-universal
hydrogen
evolution
reaction
(HER).
Herein,
activated
N-doped
mesoporous
carbon
spheres
supported
Pt3
Fe
(Pt3
Fe/NMCS-A),
as
a
highly-efficient
electrocatalyst
HER,
are
reported.
The
Fe/NMCS-A
exhibits
low
overpotentials
(η10
)
of
13,
29,
48
mV
deliver
10
mA
cm-2
in
0.5
m
SO4
,
1.0
KOH,
phosphate
buffered
solution
(PBS),
respectively,
well
robust
stability
maintain
the
overall
catalytic
performances.
Theoretical
studies
reveal
that
strong
Pt
5d-Fe
3d
orbital
electronic
interactions
negatively
shift
d-band
center
(εd
5d
orbital,
resulting
reduced
H*
adsorption
energy
enhanced
acidic
HER
activity.
With
acting
co-adsorption
*OH
intermediates,
barrier
is
required
dissociate
afford
which
greatly
promotes
formation
alkaline
neutral
conditions.
synthetic
strategy
further
extended
synthesis
Co
Ni
with
excellent
activity
electrolytes,
demonstrating
great
potential
these
Pt-based
practical
applications.
Advanced Materials,
Год журнала:
2021,
Номер
33(41)
Опубликована: Авг. 22, 2021
Abstract
A
crucial
issue
restricting
the
application
of
direct
alcohol
fuel
cells
(DAFCs)
is
low
activity
Pt‐based
electrocatalysts
for
oxidation
reaction
caused
by
intermediate
(CO*)
poisoning.
Herein,
a
new
strategy
demonstrated
making
class
sub‐monolayer
YO
x
/MoO
‐surface
co‐decorated
ultrathin
platinum
nanowires
(YO
–Pt
NWs)
to
effectively
eliminate
CO
poisoning
enhancing
methanol
electrocatalysis.
By
adjusting
amounts
and
MoO
decorated
on
surface
Pt
NWs,
optimized
22%
NWs
achieve
high
specific
3.35
mA
cm
−2
mass
2.10
mg
−1
,
as
well
enhanced
stability.
In
situ
Fourier
transform
infrared
(FTIR)
spectroscopy
stripping
studies
confirm
contribution
anti‐CO
ability
NWs.
Density
functional
theory
(DFT)
calculations
further
reveal
that
Y
Mo
atoms
with
states
allow
COOH*
bind
through
both
carbon
oxygen
atoms,
which
can
lower
free
energy
barriers
CO*
into
COOH*.
The
optimal
also
show
superior
activities
toward
electro‐oxidation
ethanol,
ethylene
glycol,
glycerol.
Layered
double-hydroxide
(LDH)
has
been
considered
an
important
class
of
electrocatalysts
for
the
oxygen
evolution
reaction
(OER),
but
adsorption-desorption
behaviors
intermediates
on
its
surface
still
remain
unsatisfactory.
Apart
from
transition-metal
doping
to
solve
this
electrocatalytic
problem
LDH,
rare-earth
(RE)
species
have
sprung
up
as
emerging
dopants
owing
their
unique
4f
valence-electronic
configurations.
Herein,
Er
is
chosen
a
RE
model
improve
OER
activity
LDH
via
constructing
nickel
foam
supported
Er-doped
NiFe-LDH
catalyst
(Er-NiFe-LDH@NF).
The
optimal
Er-NiFe-LDH@NF
exhibits
low
overpotential
(191
mV
at
10
mA
cm-2
),
high
turnover
frequency
(0.588
s-1
and
activation
energy
(36.03
kJ
mol-1
which
are
superior
Er-free
sample.
Electrochemical
in
situ
Raman
spectra
reveal
facilitated
transition
Ni-OH
into
Ni-OOH
promoted
kinetics
through
effect.
Theoretical
calculations
demonstrate
that
introduction
facilitates
spin
crossover
valence
electrons
by
optimizing
d
band
center
NiFe-LDH,
leads
GO
-GHO
closer
kinetic
volcano
balancing
bonding
strength
*O
*OH.
Moreover,
presents
practicability
electrochemical
water-splitting
devices
with
driving
potential
well-extended
period.
Energy & Environmental Science,
Год журнала:
2021,
Номер
14(11), С. 5911 - 5918
Опубликована: Янв. 1, 2021
A
series
of
PtLn
alloys
have
been
synthesized
to
act
as
efficient
electrocatalysts
for
methanol
oxidation
reactions,
where
the
electronic
perturbations
lanthanide
guarantee
high
electroactivity
and
long-term
durability.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(52)
Опубликована: Ноя. 9, 2023
The
active-site
density,
intrinsic
activity,
and
durability
of
Pd-based
materials
for
oxygen
reduction
reaction
(ORR)
are
critical
to
their
application
in
industrial
energy
devices.
This
work
constructs
a
series
carbon-based
rare-earth
(RE)
oxides
(Gd2
O3
,
Sm2
Eu2
CeO2
)
by
using
RE
metal-organic
frameworks
tune
the
ORR
performance
Pd
sites
through
Pd-REx
Oy
interface
interaction.
Taking
Pd-Gd2
/C
as
representative,
it
is
identified
that
strong
coupling
between
Gd2
induces
formation
Pd-O-Gd
bridge,
which
triggers
charge
redistribution
.
screened
exhibits
impressive
with
high
onset
potential
(0.986
VRHE
),
half-wave
(0.877
excellent
stability.
Similar
results
also
found
Pd-Sm2
/C,
Pd-Eu2
Pd-CeO2
catalysts.
Theoretical
analyses
reveal
promotes
electron
transfer
antibonding-orbital
occupancy
Pd-*OH
optimization
*OH
adsorption
rate-determining
step
ORR.
pH-dependent
microkinetic
modeling
shows
close
theoretical
optimal
activity
ORR,
outperforming
Pt
under
same
conditions.
By
its
ascendancy
superior
Zn-air
battery
an
air
cathode,
implying
practicability.