Abstract
Carbon
materials
hold
significant
promise
in
electrocatalysis,
particularly
electrochemical
CO
2
reduction
reaction
(eCO
RR)
and
two‐electron
oxygen
(2e
−
ORR).
The
pivotal
factor
achieving
exceptional
overall
catalytic
performance
carbon
catalysts
is
the
strategic
design
of
specific
active
sites
nanostructures.
This
work
presents
a
comprehensive
overview
recent
developments
electrocatalysts
for
eCO
RR
2e
ORR.
creation
through
single/dual
heteroatom
doping,
functional
group
decoration,
topological
defect,
micro‐nano
structuring,
along
with
their
synergistic
effects,
thoroughly
examined.
Elaboration
on
mechanisms
structure‐activity
relationships
these
provided.
In
addition
to
directly
serving
as
electrocatalysts,
this
review
explores
role
matrix
support
finely
adjusting
reactivity
single‐atom
molecular
catalysts.
Finally,
addresses
challenges
prospects
associated
designing
fabricating
providing
valuable
insights
into
future
trajectory
dynamic
field.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(13), С. 9434 - 9443
Опубликована: Март 20, 2024
Electrocatalytic
synthesis
of
hydrogen
peroxide
(H2O2)
in
acidic
media
is
an
efficient
and
eco-friendly
approach
to
produce
inherently
stable
H2O2,
but
limited
by
the
lack
selective
catalysts
under
industrial-relevant
current
densities.
Herein,
we
report
a
diatomic
cobalt
catalyst
for
two-electron
oxygen
reduction
efficiently
H2O2
at
50–400
mA
cm–2
acid.
Electrode
kinetics
study
shows
>95%
selectivity
on
sites.
In
flow
cell
device,
record-high
production
rate
11.72
mol
gcat–1
h–1
exceptional
long-term
stability
(100
h)
are
realized
high
situ
spectroscopic
studies
theoretical
calculations
reveal
that
introducing
second
metal
into
coordination
sphere
site
can
optimize
binding
strength
key
intermediates
due
downshifted
d-band
center
cobalt.
We
also
demonstrate
feasibility
processing
municipal
plastic
wastes
through
decentralized
production.
Advanced Functional Materials,
Год журнала:
2024,
Номер
34(29)
Опубликована: Фев. 13, 2024
Abstract
Defect
engineering
is
an
emerging
technology
for
tailoring
nanomaterials'
characteristics
and
catalytic
performance
in
various
applications.
Recently,
defect‐engineered
nanoparticles
have
emerged
as
highly
researched
materials
applications
because
of
their
exceptional
redox
reaction
capabilities
physicochemical
optical
properties.
The
properties
nanomaterials
can
be
readily
adjusted
by
controlling
the
nature
concentration
defects
within
nanoparticles,
avoiding
need
intricate
design
strategies.
This
review
investigates
defect
nanocatalysts,
including
design,
fabrication,
Initially,
categories
strategies
nanomaterial
impacts
on
nanocatalysts'
electronic
surface
properties,
activity,
selectivity,
stability
are
summarized.
Then,
processes
uses,
gas
sensing,
hydrogen
(H
2
)
evolutions,
water
splitting,
reductions
carbon
dioxide
(CO
nitrogen
to
value‐aided
products,
pollutant
degradation,
biomedical
(oncotherapy,
antibacterial
wound
healing,
biomolecular
sensing)
discussed.
Finally,
limitations
prospective
paths
allowing
logical
optimization
nanocatalytic
long‐term
efficient
also
examined.
comprehensive
gives
unique
insights
into
current
state
nanocatalysts
inspires
future
research
exploiting
shortcomings
improve
customize
performance.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(47), С. 25695 - 25704
Опубликована: Ноя. 9, 2023
In
the
energy
conversion
context,
design
and
synthesis
of
high-performance
metal-free
carbon
nanomaterials
with
topological
defects
for
oxygen
reduction
reaction
(ORR)
are
essential.
Herein,
we
first
report
a
template-assisted
strategy
to
fabricate
defect
electrocatalysts
rich
vacancy
coupling
pentagons
(VP)
as
active
sites
in
two-dimensional
(2D)
nanosheets
(VP/CNs).
Experimental
characterizations
verify
presence
abundant
VP
VP/CNs
electrocatalyst,
ORR
activity
is
linearly
related
amounts
sites.
situ
spectroscopic
results
identify
that
can
catalyze
direct
O-O
bond
cleavage,
bypassing
formation
traditional
*OOH
intermediates,
resulting
fast
kinetics
via
dissociative
pathway.
The
as-prepared
show
outstanding
intrinsic
alkaline
(half-wave
potential
0.86
V
vs
reversible
hydrogen
electrode)
an
almost
99%
efficiency
four-electron
selectivity,
outperforming
using
benchmark
Pt/C.
Density
functional
theory
calculations
further
reveal
cooperative
effect
between
adjacent
significantly
increases
charge
transfer
achieves
lower
barrier
compared
counterpart
or
single
pentagon.
well-designed
pave
new
avenue
rational
high
efficiency.
Advanced Materials,
Год журнала:
2024,
Номер
36(25)
Опубликована: Март 8, 2024
Abstract
Non‐noble
transition
metal
(TM)‐based
compounds
have
recently
become
a
focal
point
of
extensive
research
interest
as
electrocatalysts
for
the
two
electron
oxygen
reduction
(2e
−
ORR)
process.
To
efficiently
drive
this
reaction,
these
TM‐based
must
bear
unique
physiochemical
properties,
which
are
strongly
dependent
on
their
phase
structures.
Consequently,
adopting
engineering
strategies
toward
structure
has
emerged
cutting‐edge
scientific
pursuit,
crucial
achieving
high
activity,
selectivity,
and
stability
in
electrocatalytic
This
comprehensive
review
addresses
intricate
field
applied
to
non‐noble
2e
ORR.
First,
connotation
fundamental
concepts
related
kinetics
thermodynamics
succinctly
elucidated.
Subsequently,
focus
shifts
detailed
discussion
various
approaches,
including
elemental
doping,
defect
creation,
heterostructure
construction,
coordination
tuning,
crystalline
design,
polymorphic
transformation
boost
or
revive
ORR
performance
(selectivity,
stability)
catalysts,
accompanied
by
an
insightful
exploration
phase‐performance
correlation.
Finally,
proposes
fresh
perspectives
current
challenges
opportunities
burgeoning
field,
together
with
several
critical
directions
future
development
electrocatalysts.
Chemical Science,
Год журнала:
2024,
Номер
15(29), С. 11188 - 11228
Опубликована: Янв. 1, 2024
The
oxygen
reduction
reaction
(ORR)
is
a
key
component
for
many
clean
energy
technologies
and
other
industrial
processes.
However,
the
low
selectivity
sluggish
kinetics
of
ORR
catalysts
have
hampered
conversion
efficiency
real
application
these
new
mentioned
before.
Recently,
tremendous
efforts
been
made
in
mechanism
understanding,
electrocatalyst
development
system
design.
Here,
comprehensive
critical
review
provided
to
present
recent
advances
field
electrocatalytic
ORR.
two-electron
four-electron
transfer
catalytic
mechanisms
evaluation
parameters
are
discussed
first.
Then,
up-to-date
synthetic
strategies
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Окт. 21, 2024
Surface
modulation
strategies
have
spurred
great
interest
with
regard
to
regulating
the
morphology,
dispersion
and
flexible
processability
of
materials.
Unsurprisingly,
customized
surfaces
is
primed
offer
a
route
control
their
electronic
functions.
To
regulate
electromagnetic
wave
(EMW)
absorption
applications
by
surface
engineering
an
unmet
challenge.
Thanks
pyrolyzing
surface-anchored
metal-porphyrin,
here
we
report
on
four-nitrogen
atoms-confined
single
metal
site
nitrogen-doped
carbon
layer
(sM(N4)@NC,
M
=
Ni,
Co,
Cu,
Ni/Cu)
(sM=single
metal;
NC=
layer)
that
registers
absorption.
Surface-anchored
metal-porphyrins
are
afforded
attaching
them
onto
polypyrrole
via
prototypical
click
reaction.
Further,
sM(N4)@NC
experimentally
found
elicit
identical
dipole
polarization
loss
mechanism,
overcoming
handicaps
conductivity
loss,
defects,
interfacial
among
current
EMW
absorber
models.
Importantly,
exhibit
effective
bandwidth
6.44
reflection
−51.7
dB,
preceding
state-of-the-art
carbon-based
absorbers.
This
study
introduces
strategy
design
absorbers
based
sites
enable
fine-tunable
controlled
mechanism
atomistic
precision.
In
this
work,
Cheng
et
al.
unique
dipole-dominated
model
excluding
other
redundant
opening
avenue
for
exploring
future
academic
studies
industrially
applicable
absorbing
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
