Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(28)
Опубликована: Май 9, 2024
The
single-atom
Fe-N-C
catalyst
has
shown
great
promise
for
the
oxygen
reduction
reaction
(ORR),
yet
intrinsic
activity
is
not
satisfactory.
There
a
pressing
need
to
gain
deeper
understanding
of
charge
configuration
and
develop
rational
modulation
strategies.
Herein,
we
have
prepared
Fe
with
co-coordination
N
O
(denoted
as
Fe-N/O-C)
adjacent
defect,
proposing
strategy
optimize
d-orbital
spin-electron
filling
sites
by
fine-tuning
first
coordination
shell.
Fe-N/O-C
exhibits
significantly
better
ORR
compared
its
counterpart
commercial
Pt/C,
much
more
positive
half-wave
potential
(0.927
V)
higher
kinetic
current
density.
Moreover,
using
catalyst,
Zn-air
battery
proton
exchange
membrane
fuel
cell
achieve
peak
power
densities
up
490
1179
mW
cm
Carbon Energy,
Год журнала:
2022,
Номер
4(6), С. 1021 - 1079
Опубликована: Июль 14, 2022
Abstract
Currently,
more
than
86%
of
global
energy
consumption
is
still
mainly
dependent
on
traditional
fossil
fuels,
which
causes
resource
scarcity
and
even
emission
high
amounts
carbon
dioxide
(CO
2
),
resulting
in
a
severe
“Greenhouse
effect.”
Considering
this
situation,
the
concept
“carbon
neutrality”
has
been
put
forward
by
125
countries
one
after
another.
To
achieve
goals
neutrality,”
two
main
strategies
to
reduce
CO
emissions
develop
sustainable
clean
can
be
adopted.
Notably,
these
are
crucial
for
synthesis
advanced
single‐atom
catalysts
(SACs)
energy‐related
applications.
In
review,
we
highlight
unique
SACs
conversion
into
high‐efficiency
energy,
example,
through
photocatalytic,
electrocatalytic,
thermal
catalytic
hydrogenation
technologies,
convert
hydrocarbon
fuels
(CO,
CH
4
,
HCOOH,
3
OH,
multicarbon
[C
2+
]
products).
addition,
introduce
technologies
devices
replace
polluting
such
as
photocatalytic
electrocatalytic
water
splitting
produce
hydrogen
oxygen
reduction
reaction
(ORR)
fuel
cells.
Impressively,
several
representative
examples
(including
d
‐,
ds
p
f
‐blocks)
conversion,
H
ORR
discussed
describe
methods,
characterization,
corresponding
activity.
Finally,
review
concludes
with
description
challenges
outlooks
future
applications
contributing
toward
neutrality.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(39), С. 18144 - 18152
Опубликована: Сен. 22, 2022
Fe–N–C
electrocatalysts
have
emerged
as
promising
substitutes
for
Pt-based
catalysts
the
oxygen
reduction
reaction
(ORR).
However,
their
real
catalytic
active
site
is
still
under
debate.
The
underlying
roles
of
different
types
coordinating
N
including
pyridinic
and
pyrrolic
in
performance
require
thorough
clarification.
In
addition,
how
to
understand
pH-dependent
activity
another
urgent
issue.
Herein,
we
comprehensively
studied
13
N-coordinated
FeNxC
configurations
corresponding
ORR
through
simulations
which
mimic
realistic
electrocatalytic
environment
on
basis
constant-potential
implicit
solvent
models.
We
demonstrate
that
contributes
a
higher
than
N,
FeN4C
exhibits
highest
acidic
media.
Meanwhile,
situ
transformation
*O-FeN4C
*OH-FeN4C
clarifies
origin
alkaline
These
findings
can
provide
indispensable
guidelines
rational
design
better
durable
catalysts.
eScience,
Год журнала:
2022,
Номер
2(4), С. 399 - 404
Опубликована: Май 18, 2022
Robust
oxygen
reduction
reaction
(ORR)
catalysts
are
essential
for
energy
storage
and
conversion
devices,
but
their
development
remains
challenging.
Herein,
we
design
a
single-atom
catalyst
featuring
isolated
Co
anchored
on
nitrogen-doped
carbon
(Co-SAC/NC)
via
highly
efficient
“plasma-bombing”
strategy.
With
high
loading
(up
to
2.5
wt%),
the
well-dispersed
single
atoms
in
Co-SAC/NC
give
it
robust
ORR
performance
an
alkaline
medium.
It
also
demonstrates
excellent
battery
when
implemented
as
air-cathode
zinc-air
(ZAB).
Theoretical
calculations
reveal
that
Co–N4
moiety
experiences
“extraction/recovery”
structural
evolution
during
process,
reaction's
rate-determining
step
is
formation
of
OOH∗
(reaction
intermediate).
This
work
provides
new
strategy
designing
high-performance
ZABs
other
energy-conversion
devices.
Advanced Functional Materials,
Год журнала:
2022,
Номер
32(32)
Опубликована: Май 22, 2022
Abstract
Dual–single‐atom
catalysts
with
synergistic
effect
of
adjacent
atomic
metal
sites
show
a
great
potential
for
oxygen
reduction
reaction
(ORR).
Herein,
dynamical
synthetic
strategy
is
demonstrated
the
rational
design
dual‐atom
catalyst
((Zn,
Cu)
−
NC)
non‐covalent
Cu
and
Zn
as
nitrogen‐doped
carbon
support.
Owing
to
interaction
pair
sites,
(Zn,
NC
exhibits
significant
performances
ORR,
surpassing
individual
or
site.
The
theoretical
calculations
reveal
that
can
highly
activate
linear
O
2
molecule
via
between
pairs,
providing
more
effective
overlap
3d
orbitals
2p
orbital.
Therefore,
ORR
activity
optimized
improvement
adsorption
configuration
energy
.
Further,
both
liquid
quasi‐solid
zinc
air
batteries
cathodes
achieve
remarkable
density
stability.
This
research
proposes
facile
construct
single‐atom
presents
an
insightful
understanding
interplay
heteronuclear
atoms
in
catalysts.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(14)
Опубликована: Янв. 16, 2023
Abstract
Oxygen
reduction
reaction
(ORR)
is
vital
for
clean
and
renewable
energy
technologies,
which
require
no
fossil
fuel
but
catalysts.
Platinum
(Pt)
the
best‐known
catalyst
ORR.
However,
its
high
cost
scarcity
have
severely
hindered
devices
(e.g.,
cells)
large‐scale
applications.
Recent
breakthroughs
in
carbon‐based
metal‐free
electrochemical
catalysts
(C‐MFECs)
show
great
potential
earth‐abundant
carbon
materials
as
low‐cost
electrocatalysts
towards
ORR
acidic
media.
This
article
provides
a
focused,
critical
review
on
C‐MFECs
media
with
an
emphasis
advances
structure
design
synthesis,
fundamental
understanding
of
structure‐property
relationship
electrocatalytic
mechanisms,
their
applications
proton
exchange
membrane
cells.
Current
challenges
future
perspectives
this
emerging
field
are
also
discussed.
Nature Communications,
Год журнала:
2022,
Номер
13(1)
Опубликована: Авг. 29, 2022
The
controllable
anchoring
of
multiple
isolated
metal
atoms
into
a
single
support
exhibits
scientific
and
technological
opportunities,
while
the
synthesis
catalysts
with
remains
challenge
has
been
rarely
reported.
Herein,
we
present
general
route
for
up
to
eleven
metals
as
highly
dispersed
single-atom
centers
on
porous
nitride-doped
carbon
supports
developed
movable
type
printing
method,
label
them
high-entropy
catalysts.
Various
tunable
multicomponent
are
successfully
synthesized
same
method
by
adjusting
only
templates
carbonization
parameters.
To
prove
utility,
quinary
(FeCoNiCuMn)
is
investigated
oxygen
reduction
reaction
catalyst
much
more
positive
activity
durability
than
commercial
Pt/C
catalyst.
This
work
broadens
family
opens
way
investigate
efficient
compositions.
Advanced Materials,
Год журнала:
2023,
Номер
35(30)
Опубликована: Апрель 18, 2023
Metal-organic
frameworks
(MOFs)
offer
versatile
templates/precursors
to
prepare
supported
metal
catalysts.
However,
the
afforded
catalysts
usually
exhibit
microporous
structures
and
unsuitable
wettability,
which
will
restrict
accessibility
of
active
sites
in
liquid-phase
reactions.
Herein,
an
etching-functionalization
strategy
is
developed
for
construction
a
tannic-acid-functionalized
MOF
with
unique
hollow-wall
3D-ordered
macroporous
(H-3DOM)
structure.
The
functional
can
be
further
employed
as
ideal
precursor
synthesis
cobalt
on
oxygen/nitrogen-co-doped
carbon
composites
H-3DOM
structures,
hydrophilic
surface.
structure
improve
external
surface
area
maximize
exposure
sites.
Moreover,
oxygen-containing
groups
enhance
wettability
guarantee
more
electrochemically
accessible
aqueous
electrolyte.
Benefitting
from
these
outstanding
characteristics,
H-3DOM-Co/ONC
exhibits
high
electrocatalytic
activity
oxygen
reduction
reaction,
superior
its
counterparts
without
hierarchically
ordered
functionalization.