Advanced Materials,
Journal Year:
2020,
Volume and Issue:
32(28)
Published: June 3, 2020
Abstract
Topological
defects,
with
an
asymmetric
local
electronic
redistribution,
are
expected
to
locally
tune
the
intrinsic
catalytic
activity
of
carbon
materials.
However,
it
is
still
challenging
deliberately
create
high‐density
homogeneous
topological
defects
in
networks
due
high
formation
energy.
Toward
this
end,
efficient
NH
3
thermal‐treatment
strategy
presented
for
thoroughly
removing
pyrrolic‐N
and
pyridinic‐N
dopants
from
N‐enriched
porous
particles,
defects.
The
resultant
systematically
investigated
by
near‐edge
X‐ray
absorption
fine
structure
measurements
density
states
analysis,
defect
mechanism
revealed
reactive
molecular
dynamics
simulations.
Notably,
as‐prepared
materials
possess
enhanced
electrocatalytic
CO
2
reduction
performance,
yielding
a
current
2.84
mA
cm
−2
Faradaic
efficiency
95.2%
generation.
Such
result
among
best
performances
reported
metal‐free
electrocatalysts.
Density
functional
theory
calculations
suggest
that
edge
pentagonal
sites
dominating
active
centers
lowest
free
energy
(Δ
G
)
reduction.
This
work
not
only
presents
deep
insights
engineering
carbon‐based
but
also
improves
understanding
on
Solar RRL,
Journal Year:
2020,
Volume and Issue:
4(8)
Published: Jan. 14, 2020
Photocatalytic
CO
2
reduction
to
produce
valuable
chemicals
and
fuels
using
solar
energy
provides
an
appealing
route
alleviate
global
environmental
problems.
Searching
for
photocatalysts
with
high
activity
selectivity
conversion
is
the
key
achieving
this
goal.
Among
various
proposed
photocatalysts,
metal‐free
materials,
such
as
graphene,
nitrides,
carbides,
conjugated
organic
polymers,
have
gained
extensive
research
interest
photocatalytic
reduction,
due
their
earth
abundance,
cost‐effectiveness,
good
electrical
conductivity,
friendliness.
They
exhibit
prominent
catalytic
activity,
impressive
selectivity,
long
durability
of
fuels.
Herein,
recent
progress
on
photocatalysis
systematically
reviewed.
Opportunities
challenges
modification
nonmetallic
catalysts
enhance
transformation
are
presented.
Theoretical
calculations
possible
mechanisms
pathways
well
potential
in
situ
operando
techniques
mechanistic
understanding
also
summarized
discussed.
Based
aforementioned
discussions,
suitable
future
directions
perspectives
design
development
efficient
provided.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(18), P. 10375 - 10383
Published: Feb. 19, 2021
We
reported
the
selective
electrochemical
reduction
of
oxygen
(O2
)
to
hydroxyl
radicals
(.
OH)
via
3-electron
pathway
with
FeCo
alloy
encapsulated
by
carbon
aerogel
(FeCoC).
The
graphite
shell
exposed
-COOH
is
conducive
2-electron
for
H2
O2
generation
stepped
1-electron
towards
.
OH.
electrocatalytic
activity
can
be
regulated
tuning
local
electronic
environment
electrons
coming
from
inner
alloy.
new
strategy
OH
overcomes
rate-limiting
step
over
electron
transfer
initiated
reduction-/oxidation-state
cycle
in
Fenton
process.
Fast
and
complete
removal
ciprofloxacin
was
achieved
within
5
min
this
proposed
system,
apparent
rate
constant
(kobs
up
1.44±0.04
min-1
,
which
comparable
state-of-the-art
advanced
oxidation
processes.
degradation
almost
remains
same
after
50
successive
runs,
suggesting
satisfactory
stability
practical
applications.
Advanced Energy Materials,
Journal Year:
2020,
Volume and Issue:
10(23)
Published: May 5, 2020
Abstract
Although
the
maximized
dispersion
of
metal
atoms
has
been
realized
in
single‐atom
catalysts,
further
improving
intrinsic
activity
catalysts
is
vital
importance.
Here,
decoration
isolated
Ru
into
an
edge‐rich
carbon
matrix
reported
for
electrocatalytic
hydrogen
evolution
reaction.
The
developed
catalyst
displays
high
catalytic
performance
with
low
overpotentials
63
and
102
mV
achieving
current
densities
10
50
mA
cm
−2
,
respectively.
Its
mass
about
9.6
times
higher
than
that
commercial
Pt/C‐20%
at
overpotential
100
mV.
Experimental
results
density
functional
theory
calculations
suggest
edges
enhance
local
electric
field
site
accelerate
reaction
kinetics
evolution.
present
work
may
provide
insights
behavior
guide
design
advanced
electrocatalysts.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(5), P. 1723 - 1772
Published: Jan. 1, 2023
Defective
two-dimensional
(2D)
materials
show
huge
potential
for
energy-related
fields.
This
review
overviews
the
formation/evolution
mechanisms
and
engineering
strategies
of
defects
in
2D
materials,
which
enable
enhanced
electrode
reaction
kinetics.
Advanced Materials,
Journal Year:
2020,
Volume and Issue:
32(28)
Published: June 3, 2020
Abstract
Topological
defects,
with
an
asymmetric
local
electronic
redistribution,
are
expected
to
locally
tune
the
intrinsic
catalytic
activity
of
carbon
materials.
However,
it
is
still
challenging
deliberately
create
high‐density
homogeneous
topological
defects
in
networks
due
high
formation
energy.
Toward
this
end,
efficient
NH
3
thermal‐treatment
strategy
presented
for
thoroughly
removing
pyrrolic‐N
and
pyridinic‐N
dopants
from
N‐enriched
porous
particles,
defects.
The
resultant
systematically
investigated
by
near‐edge
X‐ray
absorption
fine
structure
measurements
density
states
analysis,
defect
mechanism
revealed
reactive
molecular
dynamics
simulations.
Notably,
as‐prepared
materials
possess
enhanced
electrocatalytic
CO
2
reduction
performance,
yielding
a
current
2.84
mA
cm
−2
Faradaic
efficiency
95.2%
generation.
Such
result
among
best
performances
reported
metal‐free
electrocatalysts.
Density
functional
theory
calculations
suggest
that
edge
pentagonal
sites
dominating
active
centers
lowest
free
energy
(Δ
G
)
reduction.
This
work
not
only
presents
deep
insights
engineering
carbon‐based
but
also
improves
understanding
on
