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 Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 7, 2025
The
explicit
roles
of
the
hardly
avoidable
oxygen
species
on
carbon
materials
in
various
fields
remain
contentious
due
to
limitations
characterization
techniques,
which
lead
a
lack
fundamental
understanding
surface
chemistry.
This
study
delves
exhaustively
into
comprehension
features
different
oxygen-modified
carbons
through
dynamic
evolution
surficial
functional
groups.
Significant
differences
thermal
stability
and
electronic
properties
among
are
elucidated
via
situ
characterizations
theoretical
calculations,
providing
reliable
benchmark
for
identifying
groups
materials.
chemical
simultaneously
investigated
show
influence
structures,
redox
stability,
scalable
metal
adsorption.
These
findings
not
only
consider
common
misconception
that
produced
under
conditions
possess
identical
but
also
raise
awareness
chemistry
atomic
level.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 5, 2024
The
ligand
engineering
for
single-atom
catalysts
(SACs)
is
considered
a
cutting-edge
strategy
to
tailor
their
electrocatalytic
activity.
However,
the
fundamental
reasons
underlying
reaction
mechanism
and
contemplation
which
actual
active
site
catalytic
depends
on
pyrrolic
pyridinic
N
structure
remain
be
fully
understood.
Herein,
we
first
reveal
relationship
between
oxygen
reduction
(ORR)
activity
manganese
(Mn)
single
atomic
by
precisely
regulated
Abstract
Topological
defects
are
widely
recognized
as
effective
active
sites
toward
a
variety
of
electrochemical
reactions.
However,
the
role
defect
curvature
is
still
not
fully
understood.
Herein,
carbon
nanomaterials
with
rich
topological
tunable
reported.
The
curved
defective
surface
realized
by
controlling
high‐temperature
pyrolytic
shrinkage
process
precursors.
Theoretical
calculations
demonstrate
bending
can
change
local
electronic
structure,
promote
charge
transfer
to
key
intermediates,
and
lower
energy
barrier
for
oxygen
reduction
reaction
(ORR).
Experimental
results
convince
structural
superiority
highly‐curved
sites,
high
kinetic
current
density
22.5
mA
cm
−2
at
0.8
V
versus
RHE
high‐curvature
(HCDC),
≈18
times
that
low‐curvature
(LCDC).
Further
raising
densities
in
HCDC
leads
dual‐regulated
products
(HCHDC),
which
exhibit
exceptionally
outstanding
ORR
activity
both
alkaline
acidic
media
(half‐wave
potentials:
0.88
0.74
V),
outperforming
most
reported
metal‐free
catalysts.
This
work
uncovers
curvature‐activity
relationship
provides
new
guidance
design
advanced
catalysts
via
curvature‐engineering.
Energy & Fuels,
Год журнала:
2024,
Номер
38(12), С. 10589 - 10612
Опубликована: Июнь 7, 2024
The
oxygen
reduction
reaction
(ORR)
holds
significant
importance
in
the
electrochemical
processes
of
energy
conversion
systems.
kinetics
ORR
are
sluggish
as
it
is
involved
multistep
reactions.
It
imperative
to
investigate
electrocatalysts
with
outstanding
performance
and
durability
accelerating
their
kinetics.
Manganese–nitrogen–carbon
(Mn–N–C)
materials
offer
advantages
including
efficient
atom
utilization
easily
tunable
coordination
structures,
rendering
them
promising
candidates
for
enhancing
catalytic
activity.
mini-review
provides
a
concise
overview
fundamental
principles
underlying
ORR.
Then,
three
strategies
regulating
structure
summarized
improve
activity
Mn–N–C
catalysts:
adjusting
number
N
atoms
around
Mn
atoms,
doping
nonmetal
metal
atoms.
Finally,
this
outlines
challenges
prospects
associated
catalyst
This
anticipated
deepen
comprehension
readers
by
presenting
targeted
optimization
methods
regulate
configuration
catalysts.
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.
In
light
of
the
intensifying
global
energy
crisis
and
mounting
demand
for
environmental
protection,
it
is
vital
importance
to
develop
advanced
hydrogen
conversion
systems.
Electrolysis
cells
production
fuel
cell
devices
utilization
are
indispensable
in
conversion.
As
one
electrolysis
cells,
water
splitting
involves
two
electrochemical
reactions,
evolution
reaction
oxygen
reaction.
And
reduction
coupled
with
oxidation
reaction,
represent
core
electrocatalytic
reactions
devices.
However,
inherent
complexity
lack
a
clear
understanding
structure-performance
relationship
these
have
posed
significant
challenges
advancement
research
this
field.
work,
recent
development
revealing
mechanism
systems
reviewed,
including
situ
characterization
theoretical
calculation.
First,
working
principles
applications
operando
measurements
unveiling
systematically
introduced.
Then
application
calculations
design
catalysts
investigation
discussed.
Furthermore,
opportunities
also
summarized
discussed
paving
