Advanced Functional Materials,
Год журнала:
2024,
Номер
34(25)
Опубликована: Фев. 1, 2024
Abstract
Although
metal–sulfur
batteries
(M–S
batteries,
M
=
Li,
Na,
K)
are
promising
next‐generation
energy‐storage
devices
because
of
ultrahigh
theoretical
energy
density,
low
cost,
and
environmentally
friendliness,
their
practical
applications
significantly
hindered
by
the
shuttle
effect
polysulfides
growth
alkali
metal
dendrites.
These
issues
can
be
mitigated
using
Janus
atomic‐site
catalysts,
which
possess
maximum
atom
utilization
efficiency
(≈100%),
adjustable
electronic
structures,
tailorable
catalytic
sites,
thereby
effectively
improving
electrochemical
performance
M–S
batteries.
In
this
review,
recent
progress
development
atomic‐sites
on
properties,
synthesis,
characterizations
reviewed.
Then,
advances
in
catalysts
intended
for
accelerating
polysulfide
conversion
regulating
deposition,
briefly
introducing
working
principles
systematically
summarized.
Furthermore,
a
high
emphasis
is
placed
effective
regulation
strategies
rational
design
Finally,
current
challenges
future
research
directions
also
presented
to
develop
high‐efficiency
high‐energy
Nanoscale,
Год журнала:
2023,
Номер
15(39), С. 16056 - 16067
Опубликована: Янв. 1, 2023
Tailoring
the
coordination
environment
is
an
effective
strategy
to
modulate
electronic
structure
and
catalytic
activity
of
atomically
dispersed
transition-metal
(TM)
catalysts,
which
has
been
widely
investigated
for
single-atom
catalysts
but
received
less
attention
emerging
double-atom
(DACs).
Herein,
based
on
first-principles
calculations,
taking
commonly
studied
N-coordinated
graphene-based
DACs
as
references,
we
explored
effect
engineering
behaviors
towards
electrocatalytic
nitrogen
reduction
reaction
(NRR),
realized
through
replacing
one
N
atom
by
B
or
O
form
B,
O,
co-coordinated
DACs.
We
found
that
co-coordination
could
significantly
strengthen
N2
adsorption
alter
pattern
TM
dimer
active
center,
greatly
facilitates
activation.
Moreover,
DACs,
linear
scaling
relationship
between
binding
strengths
key
intermediates
can
be
attenuated.
Consequently,
Mn2
exhibiting
ultralow
limiting
potential
-0.27
V,
climb
peak
volcano.
In
addition,
experimental
feasibility
this
DAC
system
was
also
identified.
Overall,
benefiting
from
effect,
chemical
performance
NRR
boosted.
This
phenomena
understood
adjusted
center
due
changes
its
microenvironment,
affects
strength
(pattern)
pathways,
leading
enhanced
selectivity.
work
highlights
importance
in
developing
other
important
reactions.
ACS Catalysis,
Год журнала:
2024,
Номер
14(9), С. 6816 - 6826
Опубликована: Апрель 18, 2024
The
Fe-embedded
N-doped
graphene
(Fe–N–C)
is
the
most
representative
single
atom
catalyst
(SAC)
that
has
shown
great
potentiality
in
electrocatalysis,
such
as
oxygen
reduction
reaction
(ORR)
and
evolution
(OER).
However,
active
moiety
of
Fe–N–C
still
elusive
due
to
contradictory
experimental
results.
Moreover,
early
simulations
mainly
focus
on
thermodynamic
potential
adsorbates,
while
effect
spin
multiplicity
receives
little
attention.
To
explore
role
we
employ
constant-potential
density
functional
theory
(DFT)
systematically
study
structural
high-spin
(HS)
intermediate-spin
(IS)
FeN4
site
(marked
by
FeN4HS/IS)
OER
ORR
processes.
With
consideration
multiplicity,
our
simulation
shows
spontaneous
oxidation
from
Fe(II)N4IS
Fe(III)N4HS
at
U
=
0.4
V
versus
SHE.
Further
indicates
FeN4IS
undergoes
a
sequential
adsorption
*OH
*OOH
along
with
increase,
which
leads
state
transition
IS
HS.
According
free
energy
analysis,
FeN4HS*OOH
confirmed
be
practical
centers
OER,
FeN4HS*OH
are
assigned
center
low
high
overpotentials.
predicted
activity
agrees
situ
X-ray
absorption
near-edge
spectroscopy
(XANES)
57Fe
Mössbauer
measurement
Xiao
et
al.
[Microporous
Framework
Induced
Synthesis
Single-Atom
Dispersed
Fe-NC
Acidic
Catalyst
its
In
Situ
Reduced
Fe-N4
Active
Site
Identification
Revealed
X-Ray
Absorption
Spectroscopy.
ACS
Catal.
2018,
8,
2824–2832].
Based
geometry
orbital
bond
length
Fe–N
coordination
number
Fe
found
have
significant
impact
d
splitting
thus
induce
turnover
HS/IS
stability
OER/ORR
intermediates.
Our
brings
comprehensive
insights
into
Fe–N–C,
reveals
significance
electrocatalysis
benefits
further
theoretical
design
SACs
perspective
effects.
ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(10), С. 12398 - 12406
Опубликована: Фев. 27, 2024
The
metal-nitrogen-carbon
(M-N-C)-based
catalysts
are
promising
to
replace
PGM
(platinum
group
metal)
accelerate
oxygen
reduction
reaction
due
their
excellent
electrocatalytic
performance.
However,
the
inferior
intrinsic
activity
and
poor
active
site
density
confining
further
improvement
in
Modulating
electronic
structure
reasonably
designing
pore
widely
acknowledged
effective
strategies
boost
of
M-N-C
catalysts.
it
is
a
great
challenge
form
abundant
pores
regulate
via
facile
method.
Herein,
hierarchical,
porous
dual-atom
catalyst
FeNi-NPC-1000
has
been
architectured
by
Na
Single-atom
catalysts
(SACs),
combining
the
advantages
of
multiphase
and
homogeneous
catalysis,
have
been
increasingly
investigated
in
various
catalytic
applications.
Carbon-based
SACs
attracted
much
attention
due
to
their
large
specific
surface
area,
high
porosity,
particular
electronic
structure,
excellent
stability.
As
a
cheap
readily
available
carbon
material,
biochar
has
begun
be
used
as
an
alternative
nanotubes,
graphene,
other
such
expensive
matrices
prepare
SACs.
However,
review
biochar-based
for
environmental
pollutant
removal
energy
conversion
storage
is
lacking.
This
focuses
on
strategies
synthesizing
SACs,
pre-treatment
organisms
with
metal
salts,
insertion
elements
into
biochar,
or
pyrolysis
metal-rich
biomass,
which
are
more
simplistic
ways
Meanwhile,
this
paper
attempts
1)
demonstrate
applications
remediation
based
advanced
oxidation
technology
electrocatalysis;
2)
reveal
mechanism
different
systems;
3)
discuss
stability
SACs;
4)
present
future
developments
challenges
regarding
