ACS Applied Materials & Interfaces,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 24, 2025
Seawater
electrocatalysis
is
highly
desired
for
various
energy
storage
and
conversion
systems,
such
as
water
splitting
using
seawater
an
electrolyte
metal
fuel
cells.
However,
the
adsorption
of
chloride
ions
(Cl-)
on
active
sites
cathodes
would
worsen
oxygen
reduction
reaction
(ORR)
activity
stability,
thus
lowering
battery
performance.
Herein,
coupling
graphitic
N-regulated
adjacent
pentagon
defects
in
carbon
nanosheets
(GAP/CN)
were
first
synthesized
by
a
low-boiling-point
metal-mediated
partial
N-removal
strategy.
Experimental
theoretical
results
affirm
advantageous
cooperative
effect
between
pentagons
N
toward
ORR
harsh
environment,
where
act
authentic
effective
surrounding
site
serves
structural
regulator
to
weaken
binding
strength
harmful
Cl-
prevent
catalyst
poisoning.
As
result,
GAP/CN
delivers
excellent
activities
diverse
electrolytes,
including
0.1
M
KOH
(half-wave
potential
0.87
V),
alkaline
artificial
natural
0.71
also
good
long-term
which
can
be
comparable
commercial
Pt/C.
This
study
provides
valuable
guidance
rational
design
electrocatalysts
seawater-related
energy-conversion
devices.
Advanced Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 12, 2025
Abstract
Electrocatalytic
conversion
of
carbon
dioxide
(CO
2
)
into
valuable
carbon‐based
fuels
and
chemicals
represents
a
promising
approach
to
closing
the
cycle
setting
circular
economy.
Nevertheless,
for
current
electrocatalytic
CO
reduction
reaction
(ECO
RR)
systems,
realizing
100%
with
simultaneously
high
overall
rate
(i.e.,
single‐pass
conversion)
Faradaic
efficiency
(FE)
remains
significant
challenge.
Enhancing
often
results
in
decrease
FE,
conversely,
improving
FE
may
limit
rate.
Metal–CO
(M–CO
batteries
functions
face
similar
challenges,
particularly
reversible
M–CO
batteries,
which
do
not
accomplish
net
because
nearly
all
RR
products
are
reoxidized
during
subsequent
charging
process.
Such
system
neutrality
poses
substantial
challenges.
This
perspective
provides
an
in‐depth
analysis
state‐of‐the‐art
ECO
systems
alongside
main
strategies
employed
address
their
respective
The
critical
importance
achieving
both
is
underscored
practical
applications
effectively
close
cycle.
Furthermore,
strategic
roadmap
that
outlines
future
research
directions
presented,
thereby
facilitating
advancement
comprehensive
electroconversion
technologies.
Abstract
In
the
context
of
energy
conversion,
design
and
synthesis
high‐performance
metal‐free
carbon
electrocatalysts
for
oxygen
reduction
reaction
(ORR)
is
crucial.
Herein,
a
one‐step
nitrogen
doping/extraction
strategy
proposed
to
fabricate
3D
nitrogen‐doped
aerogels
(NCA‐Cl)
with
rich
pentagonal
topological
defects.
The
NCA‐Cl
electrocatalyst
exhibits
superb
ORR
activity,
displaying
half‐wave
potential
0.89
V
vs
RHE
0.74
under
alkaline
(0.1
m
KOH)
acidic
HClO
4
)
media,
respectively,
thanks
balanced
*
OOH
intermediate
adsorption
desorption
induced
by
defects
dopants.
aqueous
zinc‐air
battery
(ZAB)
equipped
cathode
delivers
peak
power
density
206.6
mW
cm
−2
,
specific
capacity
810.6
mAh
g
−1
durability
400
h,
flexible
ZAB
also
performed
convincingly.
This
work
provides
an
effective
formation
enhancement
electrocatalytic
activity
carbon‐based
catalysts.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 17, 2025
Abstract
The
5–10
nm
exciton
diffusion
distance
for
most
organic
semiconductors
is
much
less
than
the
particle
size
of
2D
covalent
frameworks
(COFs).
As
a
result,
local
structure
change
in
small
domain
COFs,
rather
whole
particles,
could
effectively
promote
charge
transfer
photocatalysis.
Herein,
three‐component
condensation
used
to
preparing
four
mixed
imine‐
and
thiazole‐linked
donor‐acceptor
(D–A)
COFs.
In
contrast
100%
imine
ca.
90%
10%
materials
have
77–95%
higher
photocatalytic
hydrogen
peroxide
(H
2
O
)
production
rate
pure
water
due
more
prolonged
lifetime
excitation
state.
particular,
USTB‐10‐S
exhibits
H
generation
5041
µmol
g
−1
h
.
Coupling
with
benzyl
alcohol
as
sacrificial
reagent,
its
further
increased
16152
,
superior
COF‐based
photocatalysts.
This
work
illustrates
proof‐of‐concept
that
COFs
tiny
amount
able
significantly
enhance
separation
thus
performance,
inspiring
development
defect
engineering
field
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 14, 2025
Abstract
Single‐atom
site
electrocatalysts
(SACs),
with
maximum
atom
efficiency,
fine‐tuned
coordination
structure,
and
exceptional
reactivity
toward
catalysis,
energy,
environmental
purification,
have
become
the
emerging
frontier
in
recent
decade.
Along
significant
breakthroughs
activity
selectivity,
limited
stability
durability
of
SACs
are
often
underemphasized,
posing
a
grand
challenge
meeting
practical
requirements.
One
pivotal
obstacle
to
construction
highly
stable
is
heavy
reliance
on
empirical
rather
than
rational
design
methods.
A
comprehensive
review
urgently
needed
offer
concise
overview
progress
stability/durability,
encompassing
both
deactivation
mechanism
mitigation
strategies.
Herein,
this
first
critically
summarizes
degradation
induction
factors
at
atomic‐,
meso‐
nanoscale,
mainly
based
but
not
oxygen
reduction
reaction.
Subsequently,
potential
stability/durability
improvement
strategies
by
tuning
catalyst
composition,
morphology
surface
delineated,
including
robust
substrate
metal‐support
interaction,
optimization
active
stability,
fabrication
porosity
modification.
Finally,
challenges
prospects
for
discussed.
This
facilitates
fundamental
understanding
provides
efficient
principles
aimed
overcoming
difficulties
beyond.
Electrocatalytic
and
photocatalytic
hydrogen
evolution
reaction
(HER)
via
water-splitting
are
played
a
significant
role
in
solving
environmental
energy
crisis.
Two-dimensional
(2D)
nanomaterials
regarded
as
promising
materials
the
electrocatalytic
HER
field
due
to
its
large
surface
area,
good
hydrophilicity
brilliant
electronic
conductivity.
However,
several
drawbacks,
such
low
crystalline
quality,
productivity
limited
intrinsic
active
sites
restrict
industrial
applications.
Herein,
facile
green
one-step
method
prepare
Ni
particles
coated
by
carbon
2D
nanosheet
(2D
Ni/C-m)
through
molten
salt
(NaCl)-facilitated
pyrolysis
is
proposed.
Benefit
from
excellent
electrical
conductivity,
holey
synergistic
effect
between
composition
structure
of
prepared
Ni/C-m
catalyst.
The
areas
Ni/C-0.75
catalyst
shows
much
better
activities
among
samples.
exhibits
potential
-110
mV
-375
at
-10
mA
cm-2
-200
cm-2,
which
compare
that
Pt/C
(η200
=
-339
mV).
also
speed
78
umol
h-1
with
Eosin
Y
photosensitizer.
Additionally,
wonderful
stability
process
electro/photocatalytic
HER.
These
results
provide
new
insight
fabricate
Ni-based
catalysts
for
electro/photo-catalytic
evolution.
ABSTRACT
High‐entropy
materials
(HEMs)
have
emerged
as
a
pioneering
paradigm
in
recent
years,
drawing
substantial
interest
due
to
their
unique
combination
of
diverse
elemental
constituents
and
homogeneous
solid‐solution
structure.
This
novel
material
class
not
only
opens
up
extensive
potential
for
discovery
through
broad
spectrum
combinations
but
also
facilitates
fine‐tuning
properties
thanks
its
distinctive
microstructural
characteristics.
HEMs
garnered
considerable
attention
across
various
applications,
particularly
catalysis.
The
virtually
infinite
variations
compositional
within
these
multi‐elemental
systems
enable
meticulous
optimization
the
catalytic
performance.
Additionally,
high‐entropy
structure
potentially
enhances
structural,
thermal,
chemical
stability,
which
is
vital
ensuring
functionality
under
harsh
conditions.
Herein,
we
thoroughly
explore
exceptional
attributes
HEMs,
designing
strategies
transition
metal‐based
catalysis,
three
major
fields
HEMs:
electrocatalysis,
photocatalysis,
thermocatalysis.
discussion
aspires
provide
valuable
perspectives
into
advancements
innovations
catalyst
design
development.
Zinc-air
batteries
(ZABs)
are
highly
promising
for
flexible
electronics
due
to
their
high
energy
density
and
cost-effective.
However,
practical
application
is
impeded
by
the
sluggish
kinetics
of
oxygen
evolution
reduction
reactions
(OER/ORR).
This
study
presents
a
novel
design
featuring
BaO
nanoparticles
anchored
on
layered
perovskite
PrBaMn1.5Co0.5O6-δ
(PBMC)
nanofibers,
fabricated
through
plasma
method.
Notably,
treatment
induces
selective
exsolution
A-site
Ba
onto
surface,
while
simultaneously
driving
transformation
PBMC
from
simple
perovskite,
resulting
in
unique
BaO/PBMC
heterostructure.
Theoretical
calculations
demonstrate
that
construction
heterojunction
regulates
interfacial
electronic
redistribution,
thereby
lowering
barriers
both
OER
ORR.
Consequently,
air
electrode
exhibits
superior
peak
power
enhanced
stability
solid-state
ZABs,
compared
pristine
cathode.
Selective
coupled
with
phase
transition,
alkaline-earth
metal
oxide/perovskite
heterostructure,
may
offer
new
insights
conversion
technologies.