Orbital
structures
are
strongly
correlated
with
catalytic
performance,
whereas
their
regulation
strategy
is
still
in
pursuit.
Herein,
the
Fe
3d
and
O
2p
orbital
hybridization
was
optimized
by
controlling
content
of
amorphous
NiFe(OH)x
(a-NiFe(OH)x),
which
grown
situ
on
crystalline
NiFe2O4
(c-NiFe2O4)
using
an
ultrasonic
reduction
method.
The
results
electron
energy
loss
spectroscopy
(EELS)
X-ray
absorption
spectra
(XAS)
revealed
that
Fe-Oa
a-NiFe(OH)x
effectively
strengthened
jointing
adjacent
oxygen
(Oc)
c-NiFe2O4,
further
confirmed
higher
antibonding
energies
based
density
functional
theory
(DFT)
calculations.
resultant
Oa-Fe-Oc
at
composite
interface
leads
to
balanced
adsorption
desorption
energies.
Accordingly,
optimal
strong
3d-O
enhanced
OER
overpotential
150
mV,
lower
than
pristine
sample.
This
work
represents
a
promising
approach
via
introduction
phase
construct
highly
efficient
catalysts.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(11)
Опубликована: Янв. 24, 2024
Abstract
Alloying‐type
antimony
(Sb)
with
high
theoretical
capacity
is
a
promising
anode
candidate
for
both
lithium‐ion
batteries
(LIBs)
and
sodium‐ion
(SIBs).
Given
the
larger
radius
of
Na
+
(1.02
Å)
than
Li
(0.76
Å),
it
was
generally
believed
that
Sb
would
experience
even
worse
degradation
in
SIBs
due
to
more
substantial
volumetric
variations
during
cycling
when
compared
LIBs.
However,
unexpectedly
exhibited
better
electrochemical
structural
stability
LIBs,
mechanistic
reasons
underlie
this
performance
discrepancy
remain
undiscovered.
Here,
using
situ
transmission
electron
microscopy,
X‐ray
diffraction,
Raman
techniques
complemented
by
simulations,
we
explicitly
reveal
lithiation/delithiation
process,
sodiation/desodiation
process
displays
previously
unexplored
two‐stage
alloying/dealloying
mechanism
polycrystalline
amorphous
phases
as
intermediates
featuring
improved
resilience
mechanical
damage,
contributing
superior
SIBs.
Additionally,
properties
weaker
atomic
interaction
Na−Sb
alloys
Li−Sb
favor
enabling
mitigated
stress,
accounting
enhanced
unveiled
simulations.
Our
finding
delineates
origins
potential
implications
other
large‐volume‐change
electrode
materials.
Chemical Society Reviews,
Год журнала:
2023,
Номер
53(2), С. 684 - 713
Опубликована: Дек. 20, 2023
Crystalline-amorphous
hybrid
materials
(CA-HMs)
possess
the
merits
of
both
pure
crystalline
and
amorphous
phases.
Abundant
dangling
bonds,
unsaturated
coordination
atoms,
isotropic
structural
features
in
phase,
as
well
relatively
high
electronic
conductivity
thermodynamic
stability
phase
simultaneously
take
effect
CA-HMs.
Furthermore,
atomic
bandgap
mismatch
at
CA-HM
interface
can
introduce
more
defects
extra
active
sites,
reservoirs
for
promoted
catalytic
electrochemical
performance,
induce
built-in
electric
field
facile
charge
carrier
transport.
Motivated
by
these
intriguing
features,
herein,
we
provide
a
comprehensive
overview
CA-HMs
on
various
aspects-from
synthetic
methods
to
multiple
applications.
Typical
characteristics
are
discussed
beginning,
followed
representative
strategies
CA-HMs,
including
hydrothermal/solvothermal
methods,
deposition
techniques,
thermal
adjustment,
templating
methods.
Diverse
applications
such
electrocatalysis,
batteries,
supercapacitors,
mechanics,
optoelectronics,
thermoelectrics
along
with
underlying
structure-property
mechanisms
carefully
elucidated.
Finally,
challenges
perspectives
proposed
an
aim
insights
into
future
development
Advanced Materials,
Год журнала:
2024,
Номер
36(25)
Опубликована: Март 8, 2024
Abstract
Non‐noble
transition
metal
(TM)‐based
compounds
have
recently
become
a
focal
point
of
extensive
research
interest
as
electrocatalysts
for
the
two
electron
oxygen
reduction
(2e
−
ORR)
process.
To
efficiently
drive
this
reaction,
these
TM‐based
must
bear
unique
physiochemical
properties,
which
are
strongly
dependent
on
their
phase
structures.
Consequently,
adopting
engineering
strategies
toward
structure
has
emerged
cutting‐edge
scientific
pursuit,
crucial
achieving
high
activity,
selectivity,
and
stability
in
electrocatalytic
This
comprehensive
review
addresses
intricate
field
applied
to
non‐noble
2e
ORR.
First,
connotation
fundamental
concepts
related
kinetics
thermodynamics
succinctly
elucidated.
Subsequently,
focus
shifts
detailed
discussion
various
approaches,
including
elemental
doping,
defect
creation,
heterostructure
construction,
coordination
tuning,
crystalline
design,
polymorphic
transformation
boost
or
revive
ORR
performance
(selectivity,
stability)
catalysts,
accompanied
by
an
insightful
exploration
phase‐performance
correlation.
Finally,
proposes
fresh
perspectives
current
challenges
opportunities
burgeoning
field,
together
with
several
critical
directions
future
development
electrocatalysts.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(44)
Опубликована: Май 21, 2024
Abstract
Amorphous
materials
with
a
high
number
of
unsaturated
coordinated
dangling
bonds
exhibits
macroscopic
homogeneity
and
isotropy,
making
it
easily
modifiable
to
improve
the
catalytic
properties.
At
present,
several
feasible
modification
strategies
for
amorphous
have
been
proposed
applied
multiple
fields.
This
review
aims
provide
comprehensive
overview
recent
research
advancements
in
catalysis.
First,
general
modifying
are
summarized.
Subsequently,
potential
applications
modified
electrocatalysis
photocatalysis
highlighted.
Additionally,
positive
effects
various
tools
on
properties
elucidated.
Finally,
summary
challenges
offer
critical
perspective
further
development
presented.
The
primary
goal
this
is
systematic
understanding
how
enhance
performance
stimulate
catalysts
future.
Abstract
Lithium‐ion
and
post‐lithium‐ion
batteries
are
important
components
for
building
sustainable
energy
systems.
They
usually
consist
of
a
cathode,
an
anode,
electrolyte,
separator.
Recently,
the
use
solid‐state
materials
as
electrolytes
has
received
extensive
attention.
The
electrolyte
(as
well
electrode
materials)
have
traditionally
been
overwhelmingly
crystalline
materials,
but
amorphous
(disordered)
gradually
emerging
alternatives
because
they
can
increase
number
ion
storage
sites
diffusion
channels,
enhance
diffusion,
tolerate
more
severe
volume
changes,
improve
reaction
activity.
To
develop
superior
battery
researchers
conducted
variety
experiments
theoretical
simulations.
This
review
highlights
recent
advances
in
using
(AMs)
fabricating
lithium‐ion
batteries,
focusing
on
correlation
between
material
structure
properties
(e.g.,
electrochemical,
mechanical,
chemical,
thermal
ones).
We
both
conventional
characterization
methods
analyzing
AMs
present
roles
disorder
influencing
performances
various
such
those
based
lithium,
sodium,
potassium,
zinc.
Finally,
we
describe
challenges
perspectives
commercializing
rechargeable
AMs‐based
batteries.
