The Journal of Physical Chemistry C,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 2, 2024
Probing
the
reaction
intermediates
on
electrocatalytic
surface
is
crucial
for
understanding
catalytically
active
sites
and
mechanisms.
Although
pyridinic
nitrogen-doped
carbon
has
been
proposed
as
a
highly
site
technologically
important
oxygen
reduction
(ORR)
in
fuel
cells
metal
air
batteries,
direct
situ
spectroscopic
evidence
center
(nitrogen
or
next
to
nitrogen)
ORR
pathways
remain
lacking.
We
report
chemical
vapor
deposition
of
pyridinic-N-dominated
nondoped
graphene
domains
(GDs)
well-defined
model
electrocatalysts.
By
using
electrochemical
Raman
spectroscopy,
we
reveal
that
both
N-dominated
GDs
generate
common
(*O2–
*OOH)
adsorbed
atoms
at
edges
those
neighboring
N,
respectively,
except
higher
intensities
corresponding
activities
latter.
Spatially
resolved
line
profile
spectroscopy
further
N
more
than
in-plane
containing
graphitic
N.
This
study
provides
general
methodology
establishing
structure–activity
relationships
two-dimensional
electrocatalysts
(spatially
resolved)
spectroscopy.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 29, 2024
Abstract
The
electrochemical
co‐synthesis
of
H₂O₂
and
O₃
holds
substantial
potential
for
environmental
sustainability
energy
conservation.
However,
synthesizing
electrocatalysts
with
appropriate
adsorption
energies
intermediates
in
the
pairwise
electrosynthesis
remains
a
major
challenge.
In
this
study,
boron
nitrogen‐doped
2D
diamonds
(BND)
atomically
dispersed
Pt₁/BND
are
systematically
designed
synthesized
to
facilitate
two‐electron
oxygen
reduction
reaction
(2e⁻
ORR)
ozone
production
(EOP),
respectively.
BND
exhibit
remarkable
activity,
achieving
90.7%
selectivity
attaining
Faradaic
efficiency
(FE)
12.54%
EOP.
Pt
monatomic
species,
loading
0.13%,
predominantly
distributed
along
edges
Pt₁/BND.
Theoretical
calculations
reveal
that
their
superior
properties
primarily
stem
from
phase
transition
graphene
fractions
at
edges,
which
moderate
modulate
electronic
structure
through
synergistic
interactions
between
dopant
elements.
Additionally,
favorable
mass
transfer
properties.
integration
degradation
organic
contaminants
sterilization
further
showcase
practical
utility
electrocatalysts.
Chemical Science,
Год журнала:
2023,
Номер
15(1), С. 95 - 101
Опубликована: Ноя. 9, 2023
Enhancing
the
electrochemical
activity
of
graphene
holds
great
significance
for
expanding
its
applications
in
various
electrochemistry
fields.
In
this
study,
we
have
demonstrated
a
facile
and
quantitative
approach
modulating
defect
density
single-layer
(SLG)
via
an
electrochemically
induced
bromination
process
facilitated
by
cyclic
voltammetry.
This
controlled
engineering
directly
impacts
heterogeneous
electron
transfer
(HET)
rate
SLG.
By
utilizing
Raman
spectroscopy
scanning
microscopy
(SECM),
established
correlation
between
HET
kinetics
both
(nD)
mean
distance
defects
(LD)
The
variation
(k0)
with
manifested
distinctive
three-stage
behavior.
Initially,
k0
increased
slightly
increasing
nD,
then
it
experienced
rapid
increase
as
nD
further
increased.
However,
once
surpassed
critical
value
about
1.8
×
1012
cm-2
(LD
<
4.2
nm),
decreased
rapidly.
Notably,
results
revealed
remarkable
35-fold
enhancement
under
optimal
conditions
compared
to
pristine
research
paves
way
controllable
powerful
strategy
enhance
graphene,
opening
up
new
possibilities
utilization
wide
range
applications.
Frontiers in Chemistry,
Год журнала:
2023,
Номер
11
Опубликована: Окт. 17, 2023
Low-dimensional
carbon-based
(LDC)
materials
have
attracted
extensive
research
attention
in
electrocatalysis
because
of
their
unique
advantages
such
as
structural
diversity,
low
cost,
and
chemical
tolerance.
They
been
widely
used
a
broad
range
electrochemical
reactions
to
relieve
environmental
pollution
energy
crisis.
Typical
examples
include
hydrogen
evolution
reaction
(HER),
oxygen
(OER),
reduction
(ORR),
carbon
dioxide
(CO
2
RR),
nitrogen
(NRR).
Traditional
“trial
error”
strategies
greatly
slowed
down
the
rational
design
electrocatalysts
for
these
important
applications.
Recent
studies
show
that
combination
density
functional
theory
(DFT)
calculations
experimental
is
capable
accurately
predicting
structures
electrocatalysts,
thus
revealing
catalytic
mechanisms.
Herein,
current
well-recognized
collaboration
methods
practice
are
reviewed.
The
commonly
calculation
basic
functionals
briefly
summarized.
Special
paid
descriptors
accepted
bridge
linking
structure
activity
breakthroughs
high-volume
accurate
prediction
electrocatalysts.
Importantly,
correlated
multiple
systematically
describe
complicated
interfacial
electrocatalytic
processes
LDC
catalysts.
Furthermore,
machine
learning
high-throughput
simulations
crucial
assisting
discovery
new
This
review
will
guide
further
development
extended
applications
from
aspect
DFT
computations.
ACS Applied Nano Materials,
Год журнала:
2024,
Номер
7(12), С. 14526 - 14539
Опубликована: Июнь 14, 2024
Carbocatalysts
have
been
widely
explored
in
renewable
energy
systems,
such
as
fuel
cells
and
metal-air
batteries,
their
performance
critically
hinges
upon
the
intricate
balance
between
graphitic
defective
structures.
However,
achieving
this
harmony
while
preserving
high
graphitization
levels
is
still
a
formidable
challenge.
Herein,
an
innovative
graphitic/defective
heteroatom-free
carbon
nanosheet
(GDHfCN)
developed
through
dual
molten
salt
chemical
treatment
of
polyperylene,
which
uniquely
marries
high-density
structures
with
abundant
pentagon
defects.
The
GDHfCN
demonstrates
exceptional
electrocatalytic
for
oxygen
reduction
reaction
(ORR),
half-wave
potential
0.891
V,
low
Tafel
slope
52.1
mV
dec–1,
kinetic
current
density
up
to
106.42
mA
cm–2.
This
nanoscale
configuration
outperforms
catalysts
typically
synthesized
sole
treatment,
limited
by
focus
on
either
or
Moreover,
application
flexible
zinc-air
battery
confirms
its
practical
potential,
exhibiting
remarkable
stability
under
bending
tests.
study
not
only
illustrates
carbocatalysts
but
also
advances
field
electrocatalysis,
marking
significant
stride
development
high-performance
devices.
Traditional
hydrogen
evolution
reaction
(HER)
catalysts
are
generally
noble
metals,
but
their
application
is
limited
due
to
high
cost
and
poor
stability.
Through
research,
carbon-based
have
also
shown
good
HER
performance.
These
advantages
such
as
low
stability,
making
them
a
potential
alternative
traditional
metal
catalysts.
This
chapter
focuses
on
series
of
well-performing
catalysts,
porous
carbons,
low-dimensional
carbon
materials,
metal–organic
framework
(MOF)
atomic
doping
materials
applications,
catalytic
mechanisms
in
HER.
The
strategies
improve
activity
discussed,
including
increasing
specific
surface
area,
with
heteroatoms,
preparing
composite
materials.
It
hoped
that
these
methods
material
synthesis
will
be
helpful
inspire
readers
engage
the
field