Chemistry of Materials,
Journal Year:
2024,
Volume and Issue:
36(22), P. 11296 - 11305
Published: Nov. 14, 2024
The
electrochemical
synthesis
of
nitrates
through
nitrogen
oxidation
reactions
(NOR)
faces
challenges
due
to
the
chemical
stability
N2
and
complexity
its
electron
transfer
mechanisms.
Here,
we
report
enhancement
NOR
via
Al
doping
into
Co3O4.
This
modifies
electronic
structure
Co3O4,
particularly
by
increasing
eg
orbital
occupation,
which
effectively
activates
N2.
Our
experimental
results,
corroborated
density
functional
theory
(DFT)
calculations,
reveal
that
shortens
Co–N
bond
lengths
elongates
N≡N
bond,
thereby
enhancing
polarization.
altered
material,
Al–Co3O4,
delivers
a
nitrate
yield
78.45
μg·h–1·mgcat–1
with
Faradaic
efficiency
11.91%.
These
improvements
are
attributed
an
optimized
configuration
enhanced
adsorption
characteristics
modified
occupancy.
study
highlights
crucial
role
engineering
in
electrocatalyst
for
activation,
offering
promising
route
advancement
technology.
Nano-Micro Letters,
Journal Year:
2024,
Volume and Issue:
17(1)
Published: Sept. 27, 2024
Abstract
High-entropy
materials
represent
a
new
category
of
high-performance
materials,
first
proposed
in
2004
and
extensively
investigated
by
researchers
over
the
past
two
decades.
The
definition
high-entropy
has
continuously
evolved.
In
last
ten
years,
discovery
an
increasing
number
led
to
significant
advancements
their
utilization
energy
storage,
electrocatalysis,
related
domains,
accompanied
rise
techniques
for
fabricating
electrode
materials.
Recently,
research
emphasis
shifted
from
solely
improving
performance
toward
exploring
reaction
mechanisms
adopting
cleaner
preparation
approaches.
However,
current
remains
relatively
vague,
method
is
based
on
single
metal/low-
or
medium-entropy
It
should
be
noted
that
not
all
methods
applicable
can
directly
applied
this
review,
development
are
briefly
reviewed.
Subsequently,
classification
presented,
followed
discussion
applications
storage
catalysis
perspective
synthesis
methods.
Finally,
evaluation
advantages
disadvantages
various
production
process
different
provided,
along
with
proposal
potential
future
directions
ACS Nano,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 14, 2025
Quadruple
perovskite
oxides
have
received
extensive
attention
in
electronics
and
catalysis,
owing
to
their
cation-ordering
structure
intriguing
physical
properties.
However,
repertoires
still
remain
limited.
In
particular,
piezoelectricity
from
quadruple
perovskites
has
been
rarely
reported
due
the
frustrated
symmetry-breaking
transition
A-site-ordered
structures,
disabling
piezoelectric
applications.
Herein,
we
report
a
feasible
strategy
achieve
CaCu3Ti4O12
(CCTO)
via
cation
defect
engineering,
specifically
through
thermal-driven
selective
exsolution
introduce
Cu
vacancies.
The
introduction
of
point
defects
CCTO
locally
destabilizes
constrained
tilted
TiO6
octahedra
framework,
relaxing
octahedral
tilting
inducing
structural
heterogeneity
which,
turn,
disrupts
high
symmetry
pristine
cubic
phase.
As
result,
defective
with
localized
asymmetry
exhibits
intense
polarization
robust
7
pC
N-1.
created
is
further
validated
by
its
application
as
piezo-photocatalyst,
enabling
efficient
charge
separation
transfer
2.5-times
increment
lifetime
photoexcitations.
This
enhancement
leads
3.86-
31-fold
increase
production
hydrogen
peroxide
reactive
oxygen
species
compared
individual
piezocatalysis
photocatalysis,
respectively.
study
establishes
pathway
engineer
perovskites,
potentially
unlocking
wide
range
applications
modern
microelectronics
beyond
demonstrated
piezo-photocatalysis.
Small,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 6, 2024
Abstract
High‐entropy
perovskite
oxides
exhibit
promising
application
prospects
in
the
field
of
electrocatalysis,
owing
to
their
flexible
elemental
composition,
plentiful
active
sites,
and
superior
structural
stability.
Herein,
high‐entropy
oxide
nanotubes
are
prepared
with
La,
Nd,
Pr,
Er,
Eu
at
A‐site
by
electrospinning
as
efficient
electrocatalysts
for
nitrate
reduction
reaction
(NO
3
RR).
Electrochemical
tests
demonstrate
that
LaNd
0.25
Pr
Er
CuO
4
(LNPEEC
NTs)
display
outstanding
NO
RR
performance,
achieving
a
NH
Faraday
efficiency
(FE
NH3
)
100%
−0.7
V
versus
reversible
hydrogen
electrode
(RHE)
yield
rate
1378
µg
h
−1
mg
cat.
−1.0
RHE
,
outperforming
Nd
2
(NC
NTs).
Furthermore,
LNPEEC
NTs
also
excellent
stability
even
after
10
cycles
.
X‐ray
absorption
spectroscopy
confirms
multi‐component
regulation
optimizes
coordination
environment
Cu
B‐site,
increasing
unsaturated
sites
thus
providing
more
sites.
Additionally,
density
functional
theory
calculations
reveal
doping
rare‐earth
elements
modulates
d‐band
center
B‐site
reduces
energy
barrier
rate‐determining
step,
enhancing
adsorption
−
promoting
performance.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 3, 2025
Abstract
Electrocatalytic
nitrate
reduction
to
ammonia
(NRA)
offers
an
arousing
route
for
converting
widespread
pollutant
under
mild
conditions.
Among
other
NRA
catalysts,
single‐atom
catalyst
(SAC)
has
emerged
as
a
promising
candidate
due
its
numerous
advantages
such
maximum
metal‐atom‐utilization
efficiency,
homogeneous
and
tailorable
active
sites,
which
still
encounters
formidable
challenge
accelerate
the
kinetics
simultaneously
suppress
competitive
hydrogen
evolution
reaction,
especially
when
operated
in
electrolytes
with
low
concentration
nitrate.
Herein,
general
strategy
is
reported
prepare
defect‐enriched
coordination
polymer
catalysts
featuring
well‐defined
unsaturated
metal
can
exhibit
exceptional
performance
even
at
surpass
SACs
toward
catalysis.
Taking
cobalt
(Co)
example,
Co‐based
polymers
(d‐CoCP)
counterpart
CoCP
without
defects
are
investigated
proof‐of‐concept
study.
Both
experimental
theoretical
results
elucidate
that
elaborately‐engineered
d‐CoCP
markedly
decrease
thermodynamic
barrier
reducing
*NO
*HNO
rate‐limiting
step
along
pathway,
thus
accelerating
adsorption
of
promoting
kinetics.
