Advanced Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Июль 25, 2024
Over
the
last
decade,
carbon-based
metal-free
electrocatalysts
(C-MFECs)
have
become
important
in
electrocatalysis.
This
field
is
started
thanks
to
initial
discovery
that
nitrogen
atom
doped
carbon
can
function
as
a
electrode
alkaline
fuel
cells.
A
wide
variety
of
nanomaterials,
including
0D
dots,
1D
nanotubes,
2D
graphene,
and
3D
porous
carbons,
has
demonstrated
high
electrocatalytic
performance
across
applications.
These
include
clean
energy
generation
storage,
green
chemistry,
environmental
remediation.
The
applicability
C-MFECs
facilitated
by
effective
synthetic
approaches,
e.g.,
heteroatom
doping,
physical/chemical
modification.
methods
enable
creation
catalysts
with
properties
useful
for
sustainable
transformation
storage
(e.g.,
cells,
Zn-air
batteries,
Li-O
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(45), С. 31253 - 31261
Опубликована: Янв. 1, 2024
The
widespread
utilization
of
noble
metal-based
catalysts
for
the
oxygen
evolution
reaction
(OER)
is
hindered
by
their
rarity
and
substantial
expense,
posing
significant
challenges
large-scale
applications.
Abstract
The
electrochemical
activation
of
inert
CO
2
molecules
through
C─C
coupling
reactions
under
ambient
conditions
remains
a
significant
challenge
but
holds
great
promise
for
sustainable
development
and
the
reduction
emission.
Lewis
pairs
can
capture
react
with
,
offering
novel
strategy
electrosynthesis
high‐value‐added
C2
products.
Herein,
an
electron‐beam
irradiation
is
presented
rapidly
synthesizing
metal–organic
framework
(MOF)
well‐defined
(i.e.,
Cu‐
N
pyridinic
).
synthesized
MOFs
exhibit
total
product
faradic
efficiency
70.0%
at
−0.88
V
versus
RHE.
In
situ
attenuated
reflection
Fourier
transform
infrared
Raman
spectra
reveal
that
electron‐deficient
acidic
Cu
sites
electron‐rich
basic
in
ligand
facilitate
targeted
chemisorption,
activation,
conversion
molecules.
DFT
calculations
further
elucidate
electronic
interactions
key
intermediates
reaction.
work
not
only
advances
pair‐site
as
new
platform
conversion,
also
provides
pioneering
insights
into
underlying
mechanisms
irradiated
synthesis
advanced
nanomaterials.
Abstract
Electroreduction
of
carbon
dioxide
(CO
2
)
is
a
key
strategy
for
achieving
net‐zero
emissions.
Copper
(Cu)‐based
electrocatalysts
have
shown
promise
CO
conversion
into
valuable
chemicals
but
are
hindered
by
limited
C
2+
product
selectivity
due
to
competing
hydrogen
evolution
and
ineffective
dimerization
adsorbed
intermediate
(
*
CO).
Here,
functional‐group‐directed
reported
enhance
using
single‐walled
nanotubes
(SWCNTs)
as
supports.
The
catalytic
performance
Cu
nanoparticles
strongly
influenced
the
type
density
functional
groups
on
SWCNTs.
Optimized
Cu/amine‐functionalized
SWCNTs
achieved
Faradaic
efficiency
66.2%
partial
current
−270
mA
cm
−2
products
within
flow
cell,
outperforming
Cu/SWCNTs
Cu/cyano‐functionalized
Density
theory
calculations
revealed
that
electron‐donating
amine
can
facilitate
electron
transfer
from
graphite
sheet
atoms,
thereby
shifting
d‐band
center
upward.
This
shift
enhances
its
hydrogenation
derivative
adsorption
promotes
water
splitting,
leading
an
increased
tendency
generation
products.
In
situ
infrared
Raman
spectroscopy
confirm
enhancement
CHO
coverage,
facilitating
C─C
coupling.
work
provides
molecular
framework
exploring
interactions
between
active
metals
in
electrolysis,
offering
insights
designing
catalysts
broad
range
electrocatalytic
processes.
Nano-Micro Letters,
Год журнала:
2025,
Номер
17(1)
Опубликована: Апрель 18, 2025
Abstract
Natural
biomass-derived
carbon
material
is
one
promising
alternative
to
traditional
graphene-based
catalyst
for
oxygen
electrocatalysis.
However,
their
electrocatalytic
performance
were
constrained
by
the
limited
modulating
strategy.
Herein,
using
N-doped
commercial
coconut
shell-derived
activated
(AC)
as
model,
controllably
enhanced
sp
2
-C
domains,
through
an
flash
Joule
heating
process,
effectively
improve
edge
defect
density
and
overall
graphitization
degree
of
AC
catalyst,
which
tunes
electronic
structure
N
configurations
accelerates
electron
transfer,
leading
excellent
reduction
reaction
(half-wave
potential
0.884
V
RHE
,
equivalent
20%
Pt/C,
with
a
higher
kinetic
current
5.88
mA
cm
−2
)
evolution
activity
(overpotential
295
mV
at
10
).
In
Zn-air
battery,
shows
outstanding
cycle
stability
(over
1200
h)
peak
power
121
mW
surpassing
Pt/C
RuO
catalysts.
Density
functional
theory
simulation
reveals
that
catalytic
arises
from
axial
regulation
local
domains.
This
work
establishes
robust
strategy
domain
modulation,
offering
broad
applicability
in
natural
biomass-based
catalysts
