ChemSusChem,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 30, 2024
Abstract
As
the
global
energy
structure
evolves
and
clean
technologies
advance,
electrocatalysis
has
become
a
focal
point
as
critical
conversion
pathway
in
new
sector.
Transitional
metal
electrocatalysts
(TMEs)
with
their
distinctive
electronic
structures
redox
properties
show
great
potential
electrocatalytic
reactions.
However,
complex
reaction
mechanisms
kinetic
limitations
hinder
improvement
of
efficiency,
highlighting
necessity
for
comprehensive
studies
on
performance
electrocatalysts.
X‐ray
Absorption
Fine
Structure
(XAFS)
spectra
stand
out
robust
tool
examining
electrocatalyst′s
due
to
its
atomic
selectivity
sensitivity
local
environments.
This
review
delves
into
application
XAFS
technology
characterizing
TMEs,
providing
in‐depth
analyses
Near‐Edge
(XANES)
spectra,
Extended
(EXAFS)
both
R‐space
k
‐space.
These
reveal
intrinsic
structural
information,
interactions,
catalyst
stability,
aggregation
morphology.
Furthermore,
paper
examines
advancements
in‐situ
techniques
real‐time
monitoring
active
site
changes,
capturing
intermediate
transitional
states,
elucidating
evolution
species
during
insights
deepen
our
understanding
structure‐activity
relationship
offer
valuable
guidance
designing
developing
highly
stable
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Sept. 30, 2024
Abstract
Chemical
synthesis
of
unconventional
topologically
close‐packed
intermetallic
nanocrystals
(NCs)
remains
a
considerable
challenge
due
to
the
limitation
large
volume
asymmetry
between
components.
Here,
series
Frank‐Kasper
C15
phase
Ir
2
M
(M
=
rare
earth
metals
La,
Ce,
Gd,
Tb,
Tm)
NCs
is
successfully
prepared
via
molten‐salt
assisted
reduction
method
as
efficient
electrocatalysts
for
hydrogen
evolution
reaction
(HER).
Compared
disordered
counterpart
(A1‐Ir
Ce),
C15‐Ir
Ce
features
higher
Ir‐Ce
coordination
number
that
leads
an
electron‐rich
environment
sites.
The
catalyst
exhibits
excellent
and
pH‐universal
HER
activity
requires
only
9,
16,
27
mV
overpotentials
attain
10
mA
cm
−2
in
acidic,
alkaline,
neutral
electrolytes,
respectively,
representing
one
best
ever
reported.
In
proton
exchange
membrane
water
electrolyzer,
cathode
achieves
industrial‐scale
current
density
1
A
with
remarkably
low
cell
voltage
1.7
V
at
80
°C
can
operate
stably
1000
h
sluggish
decay
rate
50
µV
−1
.
Theoretical
investigations
reveal
sites
intensify
polarization
*H
O
intermediate
on
thus
lowering
energy
barrier
dissociation
facilitating
kinetics.
Small,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Oct. 26, 2024
Molecular
oxygen
redox
electrocatalysis
involves
reduction
and
evolution
as
core
reactions
in
various
energy
conversion
environmental
technology
fields.
Strong
metal-support
interactions
(SMSIs)
based
nanomaterials
are
regarded
desirable
state-of-the-art
heterogeneous
electrocatalysts
due
to
their
exceptional
physicochemical
properties.
Over
the
past
decades,
considerable
advancements
theory
experiment
have
been
achieved
related
studies,
especially
modulating
electronic
structure
geometrical
configuration
of
SMSIs
enable
activity,
selectivity,
stability.
In
this
focuses
on
concept
SMSI,
explore
manifestations
mechanisms
action,
summarizes
recent
advances
for
efficient
applications.
Additionally,
correlation
between
properties
different
metals
supports
is
systematically
elucidated,
potential
structure-activity
relationships
catalytic
performance
outlined
through
theoretical
models.
Finally,
obstacles
confronting
burgeoning
field
comprehensively
concluded,
targeted
recommendations
coping
strategies
proposed,
future
research
perspectives
outlined.
Metal–support
interactions
(MSI)
play
a
crucial
role
in
enhancing
the
catalytic
activity
and
stability
of
metal
catalysts
by
establishing
stable
metal-oxide
interface.
However,
precisely
controlling
MSI
at
atomic
scale
remains
significant
challenge,
as
how
to
construct
an
optimal
is
still
not
fully
understood:
Both
insufficient
excessive
showed
inferior
performance.
In
this
study,
we
propose
finely
tuning
using
temporal-precise
transient
high-temperature
pulse
heating.
Using
Pt/CeO2
model
system,
systematically
investigate
variations
duration
atmosphere
influence
reconstruction
metal–support
interface
MSIs.
This
leads
formation
two
distinct
types
MSI:
(1)
strong
(SMSI,
Pt@CeO2)
(2)
reactive
(RMSI,
Pt5Ce@CeO2),
each
with
unique
compositions,
structures,
electrochemical
behaviors.
Notably,
Pt5Ce@CeO2
RMSI
exhibits
remarkable
performance
alkaline
hydrogen
evolution,
showing
overpotential
−29
mV
operation
for
over
300
h
−10
mA·cm–2.
Theoretical
studies
reveal
that
alloying
Pt
Ce
form
Pt5Ce
modifies
electronic
structure
Pt,
shifting
d-band
center
optimize
adsorption
dissociation
intermediates,
thereby
reducing
reaction
energy
barrier.
Moreover,
intimate
interaction
CeO2
further
improves
stability.
Our
strategy
enables
precise,
stepwise,
controllable
regulation
MSIs,
providing
insights
development
highly
efficient
durable
heterostructured
wide
range
applications.
