The Journal of Physical Chemistry C,
Год журнала:
2024,
Номер
128(46), С. 19468 - 19481
Опубликована: Ноя. 6, 2024
Electrocatalysis
plays
a
crucial
role
in
energy
conversion
and
storage,
providing
an
effective
way
to
achieve
the
goals
of
carbon
neutrality.
The
combination
electrochemical
methods
with
advanced
spectroscopy
techniques
gives
insightful
in-depth
understanding
electrocatalysis
structure–performance
relationship
catalysts.
In
this
review,
recent
advances
are
summarized
focus
on
electronic
structure
electrocatalysts
relevant
dynamical
reaction
processes,
further
research
challenges
developments
outlined
for
field
electrocatalysis.
ABSTRACT
Carbon
electrocatalyst
materials
based
on
lignocellulosic
biomass
with
multi‐components,
various
dimensions,
high
carbon
content,
and
hierarchical
morphology
structures
have
gained
great
popularity
in
electrocatalytic
applications
recently.
Due
to
the
catalytic
deficiency
of
neutral
atoms,
usage
single
lignocellulosic‐based
electrocatalysis
involving
energy
storage
conversion
presents
unsatisfactory
applicability.
However,
atomic‐level
modulation
lignocellulose‐based
can
optimize
electronic
structures,
charge
separation,
transfer
processes,
so
forth,
which
results
substantially
enhanced
performance
carbon‐based
catalysts.
This
paper
reviews
recent
advances
rational
design
as
electrocatalysts
from
an
perspective,
such
self/external
heteroatom
doping
metal
modification.
Then,
through
systematic
discussion
principles
reaction
mechanisms
catalysts,
prepared
catalysts
rechargeable
batteries
are
reviewed.
Finally,
challenges
improving
prospects
diverse
review
contributes
synthesis
strategy
via
modulation,
turn
promotes
lignocellulose
valorization
for
conversion.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 3, 2025
Abstract
High‐temperature
pyrolysis
(HTP,
≥900
°C)
is
a
widely
used
method
for
synthesizing
single‐atom
catalysts
(SACs).
However,
the
high
operational
temperatures
required
HTP
pose
significant
challenges
in
achieving
loading,
primarily
due
to
Ostwald
ripening
effect.
In
this
work,
low‐temperature
trans‐metalation
synthesis
approach
developed
which
involves
exchange
of
cation
between
transition
metal
ions
(M
=
Fe,
Co,
Cu,
Ni,
Mn,
etc)
and
Zn
2+
on
nitrogen‐doped
carbon
(NC)
matrix
within
molten
salt
medium.
This
strategy
effectively
avoids
phase
transformations
enables
direct
formation
mass
loading
(3.7–4.7
wt.%)
atomically
dispersed
M‐N
4
sites.
Both
experimental
theoretical
analyses
confirm
that
cation‐exchange
occurs
at
lower
temperature
threshold
450
°C,
significantly
reducing
energy
barriers
SACs
synthesis.
Furthermore,
synthesized
catalyst
with
Fe
sites
demonstrate
excellent
performance
toward
oxygen
reduction
reaction
fuel
cell
peak
power
density
1.12
W
cm
−2
an
H
2
─O
1.0
bar
80
°C.
ACS Nano,
Год журнала:
2024,
Номер
19(1), С. 1600 - 1610
Опубликована: Дек. 27, 2024
The
development
of
high-performance
bifunctional
single-atom
catalysts
for
use
in
applications,
such
as
zinc–air
batteries,
is
greatly
impeded
by
mild
oxygen
reduction
and
evolution
reactions
(ORR
OER).
Herein,
we
report
a
electrocatalyst
designed
to
overcome
these
limitations.
catalyst
consists
well-dispersed
low-nuclearity
Co
clusters
adjacent
single
atoms
over
nitrogen-doped
carbon
matrix
(CoSA+C/NC).
precisely
tailored
asymmetric
electronic
structures
are
achieved
with
strong
interactions
between
species.
optimize
the
adsorption/desorption
strength
oxygenated
intermediates
on
single-atomic
sites
endow
exceptional
activity
under
alkaline
conditions
half-wave
potential
(E1/2)
0.91
V
an
overpotential
(η)
340
mV
at
10
mA
cm–2.
In
addition,
battery
assembled
CoSA+C/NC
achieves
high
power
density
284.1
mW
cm–2
long
operational
lifespan
400
h,
superior
those
benchmark
Pt/C
+
RuO2.
Experimental
findings
theoretical
analysis
reveal
that
enhanced
stems
from
synergistic
sites.
Consequently,
overbinding
*OH
suppressed
accelerated
removal.
This
work
establishes
design
principle
advanced
electrocatalysts
multiphase
metal
species
bearing
interactions.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 18, 2024
Abstract
High‐efficient
and
durable
electrocatalysts
for
oxygen
reduction
evolution
reaction
(ORR/OER)
are
desirable
to
Zn‐air
batteries
(ZABs).
However,
most
of
catalysts
in
powder
form
with
sole
active
sites
remain
challenging
achieving
the
satisfactory
bifunctional
catalysis
suffer
from
peeling
off
during
long‐term
operation.
Herein,
hybrid
CoFe
constructed
containing
nanoalloys
(≈10
nm),
clusters
(<
2
single
atoms
on
aerophilic
carbon
fiber
membranes
as
binder‐free
air
cathodes
ultra‐long‐life
ZABs.
In
particular,
high
air‐permeability
(0.2
s)
can
prevent
blocking
by
O
bubbles
promote
mass
transfer.
The
theoretical
experimental
results
confirm
that
hydrophilic
4
/CoFeOOH
reconstructed
surface
mainly
responsible
OER.
While
nitrogen
(N)‐doped
matrix,
they
play
a
synergetic
role
optimizing
adsorption
energy
enhance
ORR
activity.
Thus,
as‐prepared
exhibit
an
ultra‐low
ORR/OER
potential
gap
(0.64
V).
When
further
assembled
freestanding
air‐electrodes,
it
exhibits
outstanding
cycling
lifespan
1200
155
h
liquid‐
quasi‐solid‐state
ZABs
respectively,
which
fivefold
twofold
higher
than
those
powder‐based
(240/67
h).
Conversion
of
metal-organic
frameworks
(MOFs)
into
metal-nitrogen-doped
carbon
(M-N-C)
catalysts
requires
a
high-temperature
process
and
longer
processing
time
under
protective
atmosphere.
This
study
utilizes
low-energy
nanosecond
laser
(LP)
technique
to
convert
aqueous
synthesized
2D
leaf-like
Co-MOF
(L-Co-MOF)
nanoscale
cobalt
metal
encapsulated
within
nitrogen-doped
graphitic
matrix
(Co@N-gC,
Co-LP)
in
shorter
period
air
The
laser-induced
results
the
formation
Co@N-gC
with
smaller
Co
particle
size,
uniform
distribution,
better
interaction
support
compared
conventional
pyrolysis
(CP).
LP
result
enhanced
multifunctional
electrocatalytic
activity
over
CP
(Co-CP)
owing
tunable
metal-support
interaction,
higher
charge
transfer,
presence
multiactive
sites.
Under
optimized
conditions
(laser
fluence:
5.76
mJ
cm-2
scan
speed:
10
mm
s-1),
Co-LP-5
catalyst
exhibits
ORR
performance,
onset
half-wave
potentials
0.92
0.76
V,
respectively.
Additionally,
delivers
excellent
water-splitting
OER
HER
overpotentials
380
280
mV,
respectively,
achieving
an
overall
energy
efficiency
77.85%.
Furthermore,
demonstrates
exceptional
durability
48
h
real-time
testing,
outperforming
Co-CP,
proposed
is
viable
for
fabricating
catalysts.
COF
engineering
with
a
built-in,
high
concentration
of
defined
N-doped
sites
overcomes
the
"black-box"
drawback
conventional
trial-and-error
N-doping
methods
(used
in
polymeric
carbon
nitride
and
graphene),
that
hamper
directed
evolution
functional
interfaces
based
on
structure-reactivity
guidelines.
The
cutting-edge
challenge
is
to
dissect
many
complex
interdependent
functions
originate
from
reticular
N-doping,
including
modification
material
optoelectronics,
band
alignments,
interfacial
contacts
co-localization
active-sites,
producing
multiple-set
effectors
can
all
play
role
regulate
photocatalysis.
Herein,
an
ON-OFF
gated
photocatalytic
H