Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(19)
Published: Feb. 21, 2024
Abstract
Designing
effective
electrocatalysts
tailored
for
targeted
reactions
requires
fundamental
insights
into
the
structure
dependence
of
reaction
microenvironment.
Herein,
inspired
by
finite
element
simulations,
N,O
co‐doped
carbon
nanosheets
featuring
a
hierarchical
micro/mesoporous
to
form
an
oxygen‐rich
and
local
alkaline‐like
microenvironment
two‐electron
oxygen
reduction
(2e
−
ORR)
in
neutral
medium
are
designed.
The
situ
ex
test
results
confirmed
that
architecture
can
elevate
pH
accelerate
generation
intermediates
(*O
2
,
*OOH),
leading
high‐efficiency
H
O
production.
Utilizing
this
favorable
microenvironment,
N,O‐CNS
0.5
demonstrated
exceptional
electrosynthesis
performance
media,
achieving
superior
yield
rate
(6705
mmol
g
catalyst
−1
h
flow
cell).
Additionally,
comparative
experiments
density‐functional
theory
calculations
provided
confirmation
bi‐doping
N
as
active
origin
responsible
electrochemical
2e
ORR.
This
study
synergistically
manipulates
sites,
providing
opportunity
efficient
electro‐production
medium.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
unknown
Published: May 9, 2023
Metal-free
carbon-based
materials
are
considered
one
of
the
most
promising
two-electron
oxygen
reduction
reaction
(2e–
ORR)
electrocatalysts
for
green
synthesis
hydrogen
peroxide
(H2O2).
However,
reported
carbon
perform
much
more
effectively
in
alkalis
than
acids.
Herein,
by
creatively
using
fullerene
(C60)
as
precursor
subject
to
ammonia
treatment,
we
designed
and
synthesized
a
pentagonal
defect-rich
nitrogen-doped
nanomaterial
(PD/N–C).
It
achieves
outstanding
ORR
activity,
2e–
selectivity,
stability
acidic
electrolytes,
surpassing
benchmark
PtHg4
alloy
catalyst.
Impressively,
flow
cell
based
on
PD/N–C
catalyst
nearly
100%
Faraday
efficiency
with
remarkable
H2O2
yield,
representing
best
improvement
among
all
metal-free
catalysts.
Experimental
theoretical
results
reveal
that
such
superb
performance
originates
from
synergism
between
defects
nitrogen
dopants.
This
work
presents
an
effective
strategy
design
construction
highly
efficient
acid-resistant
production
beyond.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(38)
Published: Feb. 13, 2023
Abstract
Carbon‐based
single‐atom
catalysts
(SACs)
are
considered
to
be
a
perfect
platform
for
studying
the
structure–activity
relationship
of
different
reactions
due
adjustability
their
coordination
environment.
Multi‐heteroatom
doping
has
been
demonstrated
as
an
effective
strategy
tuning
environment
carbon‐based
SACs
and
enhancing
catalytic
performance
in
electrochemical
reactions.
Herein,
recently
developed
strategies
multi‐heteroatom
doping,
focusing
on
regulation
active
sites
by
heteroatoms
shells,
summarized.
In
addition,
correlation
between
activity
investigated
through
representative
experiments
theoretical
calculations
various
Finally,
concerning
certain
shortcomings
current
multi‐heteroatoms,
some
suggestions
put
forward
promote
development
field
electrocatalysis.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
34(52)
Published: March 25, 2022
Abstract
Electrocatalysts
are
the
core
components
of
many
sustainable
energy
conversion
technologies
that
considered
most
potential
solution
to
worldwide
and
environmental
crises.
The
reliability
structure
composition
pledges
electrocatalysts
can
achieve
predictable
stable
performance.
However,
during
electrochemical
reaction,
influenced
directly
by
applied
potential,
electrolyte,
adsorption/desorption
reactive
species,
triggering
structural
compositional
corrosion,
which
affects
catalytic
behaviors
(performance
degradation
or
enhancement)
invalidates
established
structure–activity
relationship.
Therefore,
it
is
necessary
elucidate
corrosion
behavior
mechanism
formulate
targeted
corrosion‐resistant
strategies
use
reconstruction
synthesis
techniques
guide
preparation
efficient
electrocatalysts.
Herein,
recent
developments
in
electrocatalyst
chemistry
outlined,
including
mechanisms,
mitigation
strategies,
syntheses/reconstructions
based
on
typical
materials
important
electrocatalytic
reactions.
Finally,
opportunities
challenges
also
proposed
foresee
possible
development
this
field.
It
believed
contribution
will
raise
more
awareness
regarding
nanomaterial
beyond.
Nano-Micro Letters,
Journal Year:
2023,
Volume and Issue:
15(1)
Published: March 28, 2023
Hydrogen
peroxide
(H2O2)
is
a
high-demand
organic
chemical
reagent
and
has
been
widely
used
in
various
modern
industrial
applications.
Currently,
the
prominent
method
for
preparation
of
H2O2
anthraquinone
oxidation.
Unfortunately,
it
not
conducive
to
economic
sustainable
development
since
complex
process
involves
unfriendly
environment
potential
hazards.
In
this
context,
numerous
approaches
have
developed
synthesize
H2O2.
Among
them,
photo/electro-catalytic
ones
are
considered
as
two
most
promising
manners
on-site
synthesis
These
alternatives
that
only
water
or
O2
required.
Namely,
oxidation
(WOR)
oxygen
reduction
(ORR)
reactions
can
be
further
coupled
with
clean
energy.
For
generation,
design
catalysts
extremely
important
extensively
conducted
an
aim
obtain
ultimate
catalytic
performance.
This
article
overviews
basic
principles
WOR
ORR,
followed
by
summary
recent
progresses
achievements
on
performance
photo/electro-catalysts
generation.
The
related
mechanisms
these
highlighted
from
theoretical
experimental
aspects.
Scientific
challenges
opportunities
engineering
generation
also
outlined
discussed.
