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
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(38), P. 20627 - 20648
Published: April 17, 2021
Abstract
The
electrochemical
carbon
dioxide
reduction
reaction
(CO
2
RR)
provides
an
attractive
approach
to
convert
renewable
electricity
into
fuels
and
feedstocks
in
the
form
of
chemical
bonds.
Among
different
CO
RR
pathways,
conversion
is
considered
one
most
promising
candidate
reactions
because
its
high
technological
economic
feasibility.
Integrating
catalyst
electrolyte
design
with
understanding
catalytic
mechanism
will
yield
scientific
insights
promote
this
technology
towards
industrial
implementation.
Herein,
we
give
overview
recent
advances
challenges
for
selective
CO.
Multidimensional
engineering
are
also
summarized.
Furthermore,
studies
on
large‐scale
production
highlighted
facilitate
industrialization
.
To
conclude,
remaining
future
directions
application
generate
highlighted.
Advanced Functional Materials,
Journal Year:
2020,
Volume and Issue:
30(25)
Published: April 3, 2020
Abstract
Functionalized
carbon
nanomaterials,
as
significant
options
for
renewable
energy
systems,
are
widely
utilized
in
diversified
electrochemical
reactions
virtue
of
property
advantages.
The
inevitable
defect
sites
architectures
greatly
affect
physicochemical
properties
thus
engineering
has
recently
become
a
vital
research
orientation
carbon‐based
electrocatalysts.
intentionally
introduced
intrinsic
the
frameworks
can
directly
serve
potential
active
owing
to
altered
surface
charge
state,
modulated
adsorption
free
key
intermediates,
well
diminished
bandgap.
Furthermore,
synergistic
between
defects
and
heteroatom
dopants/captured
atomic
metal
species
further
optimize
electronic
structure
adsorption/desorption
behavior,
making
catalysts
comparable
commercial
precious
electrocatalysis.
With
pressing
demands,
common
configurations,
construction
strategies,
structure–activity
relationships,
characterization
methods
defect‐involved
catalytic
centers
systematically
summarized.
Such
theoretical
experimental
evidences
defect‐induced
activity
reveal
relevant
mechanism,
thereby
providing
necessary
guidance
design
highly
efficient
electrocatalysts
promoting
their
applications.
Advanced Materials,
Journal Year:
2020,
Volume and Issue:
32(44)
Published: July 14, 2020
Abstract
Electrocatalysis
is
at
the
center
of
many
sustainable
energy
conversion
technologies
that
are
being
developed
to
reduce
dependence
on
fossil
fuels.
The
past
decade
has
witnessed
significant
progresses
in
exploitation
advanced
electrocatalysts
for
diverse
electrochemical
reactions
involved
electrolyzers
and
fuel
cells,
such
as
hydrogen
evolution
reaction
(HER),
oxygen
reduction
(ORR),
CO
2
(CO
RR),
nitrogen
(NRR),
(OER).
Herein,
recent
research
advances
made
porous
these
five
important
reviewed.
In
discussions,
an
attempt
highlight
advantages
multiobjective
optimization
surface
active
sites
including
not
only
their
density
accessibility
but
also
intrinsic
activity.
First,
current
knowledge
about
electrocatalytic
briefly
summarized.
Then,
mechanisms
above‐mentioned
(HER,
ORR,
RR,
NRR,
OER),
challenges
faced
by
reactions,
efforts
meet
using
examined.
Finally,
future
directions
synthetic
strategies
leading
materials,
insights
into
sites,
standardized
tests
performance
requirements
discussed.
Energy & Environmental Science,
Journal Year:
2020,
Volume and Issue:
13(8), P. 2275 - 2309
Published: Jan. 1, 2020
This
review
discusses
how
morphology
and
interface
engineering
promote
electrocatalytic
CO2
reduction,
providing
general
design
principles
to
fabricate
advanced
electrode
catalysts.
Chemical Society Reviews,
Journal Year:
2021,
Volume and Issue:
50(21), P. 11785 - 11843
Published: Jan. 1, 2021
Since
the
discovery
of
N-doped
carbon
nanotubes
as
first
carbon-based
metal-free
electrocatalyst
(C-MFEC)
for
oxygen
reduction
reaction
(ORR)
in
2009,
C-MFECs
have
shown
multifunctional
electrocatalytic
activities
many
reactions
beyond
ORR,
such
evolution
(OER),
hydrogen
(HER),
dioxide
(CO2RR),
nitrogen
(NRR),
and
peroxide
production
(H2O2PR).
Consequently,
attracted
a
great
deal
interest
various
applications,
including
metal-air
batteries,
water
splitting
devices,
regenerative
fuel
cells,
solar
chemical
production,
purification,
to
mention
few.
By
altering
electronic
configuration
and/or
modulating
their
spin
angular
momentum,
both
heteroatom(s)
doping
structural
defects
(e.g.,
atomic
vacancy,
edge)
been
demonstrated
create
catalytic
active
sites
skeleton
graphitic
materials.
Although
certain
made
be
comparable
or
even
better
than
counterparts
based
on
noble
metals,
transition
metals
hybrids,
further
research
development
are
necessary
order
translate
practical
applications.
In
this
article,
we
present
timely
comprehensive,
but
critical,
review
recent
advancements
field
within
past
five
years
so
by
discussing
types
catalyzed
C-MFECs.
An
emphasis
is
given
potential
applications
energy
conversion
storage.
The
structure-property
relationship
mechanistic
understanding
will
also
discussed,
along
with
current
challenges
future
perspectives.
Advanced Energy Materials,
Journal Year:
2020,
Volume and Issue:
10(9)
Published: Jan. 31, 2020
Abstract
Due
to
their
high
conductivity
and
low
cost,
carbon
materials
have
attracted
great
attention
in
the
field
of
energy
storage,
especially
as
anode
material
for
sodium
ion
batteries.
Current
research
focuses
on
introducing
external
defects
through
heteroatom
engineering
improve
storage
performance
materials.
However,
there
is
still
a
lack
systematic
investigation
effects
intrinsic
prevalent
performance.
Herein,
template‐assisted
method
was
used
design
with
different
degrees
explore
properties.
The
experimental
results
show
that
facilitates
adsorption
behavior
Na
+
during
surface
induction
capacitance
process.
Among
them,
best
exhibits
reversible
capacity
(221
mAh
g
−1
at
1
A
)
excellent
rate
In
addition,
density
functional
theory
calculations
also
existence
can
optimize
distribution
electron
density,
thereby
increasing
Na‐adsorption
capacity.
This
work
makes
an
important
contribution
understanding
role
