Unraveling
the
configuration–activity
relationship
and
synergistic
enhancement
mechanism
(such
as
real
active
center,
electron
spin-state,
d-orbital
energy
level)
for
triatomic
catalysts,
well
their
intrinsically
bifunctional
oxygen
electrocatalysis,
is
a
great
challenge.
Here
we
present
catalyst
(TAC)
with
trinuclear
structure
that
displays
extraordinary
electrocatalysis
reduction
reaction
(ORR)
evolution
(OER),
greatly
outperforming
counterpart
of
single-atom
diatomic
catalysts.
The
aqueous
Zn-air
battery
(ZAB)
equipped
TAC-based
cathode
exhibits
rechargeable
stability
ultrarobust
cycling
performance
(1970
h/3940
cycles
at
2
mA
cm–2,
125
h/250
10
cm–2
negligible
voltage
decay),
quasi-solid-state
ZAB
outstanding
rechargeability
low-temperature
adaptability
(300
h/1800
−60
°C),
other
state-of-the-art
ZABs.
experimental
theoretical
analyses
reveal
symmetry-breaking
CoN4
configuration
under
incorporation
neighboring
metal
atoms
(Fe
Cu),
which
leads
to
modulation,
low-shift
d
band
weakened
binding
strength
intermediates,
decreased
barrier
electrocatalysis.
This
rational
tricoordination
design
an
in-depth
analysis
indicate
hetero-TACs
can
be
promisingly
applied
in
various
applications.
Advanced Materials,
Год журнала:
2023,
Номер
36(2)
Опубликована: Июль 13, 2023
Single-atom
catalysts
(SACs)
have
attracted
considerable
attention
in
heterogeneous
catalysis
because
of
their
well-defined
active
sites,
maximum
atomic
utilization
efficiency,
and
unique
unsaturated
coordinated
structures.
However,
effectiveness
is
limited
to
reactions
requiring
sites
containing
multiple
metal
atoms.
Furthermore,
the
loading
amounts
single-atom
must
be
restricted
prevent
aggregation,
which
can
adversely
affect
catalytic
performance
despite
high
activity
individual
The
introduction
nanoscale
particles
(NMPs)
into
SACs
(NMP-SACs)
has
proven
an
efficient
approach
for
improving
performance.
A
comprehensive
review
urgently
needed
systematically
introduce
synthesis,
characterization,
application
NMP-SACs
mechanisms
behind
superior
This
first
presents
classifies
different
through
NMPs
enhance
SACs.
It
then
summarizes
currently
reported
synthetic
strategies
state-of-the-art
characterization
techniques
NMP-SACs.
Moreover,
electro/thermo/photocatalysis,
reasons
are
discussed.
Finally,
challenges
perspectives
future
design
advanced
addressed.
Advanced Materials,
Год журнала:
2023,
Номер
35(35)
Опубликована: Июнь 7, 2023
Ever-growing
demands
for
rechargeable
zinc-air
batteries
(ZABs)
call
efficient
bifunctional
electrocatalysts.
Among
various
electrocatalysts,
single
atom
catalysts
(SACs)
have
received
increasing
attention
due
to
the
merits
of
high
utilization,
structural
tunability,
and
remarkable
activity.
Rational
design
SACs
relies
heavily
on
an
in-depth
understanding
reaction
mechanisms,
especially
dynamic
evolution
under
electrochemical
conditions.
This
requires
a
systematic
study
in
mechanisms
replace
current
trial
error
modes.
Herein,
fundamental
oxygen
reduction
is
first
presented
combining
situ
and/or
operando
characterizations
theoretical
calculations.
By
highlighting
structure-performance
relationships,
rational
regulation
strategies
are
particularly
proposed
facilitate
SACs.
Furthermore,
future
perspectives
challenges
discussed.
review
provides
thorough
SACs,
which
expected
pave
avenue
exploring
optimum
effective
ZABs.
ACS Nano,
Год журнала:
2023,
Номер
17(9), С. 8622 - 8633
Опубликована: Апрель 27, 2023
We
have
achieved
the
synthesis
of
dual-metal
single
atoms
and
atomic
clusters
that
co-anchor
on
a
highly
graphitic
carbon
support.
The
catalyst
comprises
Ni4
(and
Fe4)
nanoclusters
located
adjacent
to
corresponding
NiN4
FeN4)
single-atom
sites,
which
is
verified
by
systematic
X-ray
absorption
characterization
density
functional
theory
calculations.
A
distinct
cooperation
between
Fe4
(Ni4)
FeN4
(NiN4)
sites
optimizes
adsorption
energy
reaction
intermediates
reduces
barrier
potential-determining
steps.
This
exhibits
enhanced
oxygen
reduction
evolution
activity
long-cycle
stability
compared
counterparts
without
commercial
Pt/C.
fabricated
Zn-air
batteries
deliver
high
power
long-term
cyclability,
demonstrating
their
prospects
in
storage
device
applications.
Advanced Materials,
Год журнала:
2023,
Номер
35(36)
Опубликована: Май 18, 2023
Abstract
The
electronic
structure
of
transition
metal
complexes
can
be
modulated
by
replacing
partial
ion
to
obtain
tuned
intrinsic
oxygen
reduction
reaction
(ORR)
or
evolution
(OER)
electrocatalytic
activity.
However,
the
anion‐modulated
ORR
activity
is
still
unsatisfactory,
and
construction
hetero‐anionic
remains
challenging.
Herein,
an
atomic
doping
strategy
presented
prepare
CuCo
2
O
4‐x
S
x
/NC‐2
(CCSO/NC‐2)
as
electrocatalysts,
structrual
characterization
results
favorably
demonstrate
substitution
atoms
for
in
CCSO/NC‐2,
which
shows
excellent
catalytic
performance
durability
OER
0.1
m
KOH.
In
addition,
catalyst
assembled
Zinc–air
battery
with
open
circuit
potential
1.43
V
maintains
after
300
h
cyclic
stability.
Theoretical
calculations
differential
charges
illustrate
that
optimizes
kinetics
promotes
electron
redistribution.
superior
CCSO/NC‐2
catalysis
mainly
due
its
unique
modulation
main
body.
introduction
CoO
covalency
constructs
a
fast
transport
channel,
thus
optimizing
adsorption
degree
active
site
Co
intermediates.
Journal of Materials Chemistry A,
Год журнала:
2023,
Номер
11(9), С. 4400 - 4427
Опубликована: Янв. 1, 2023
The
synthetic
strategies,
application
and
future
development
of
non-precious
metal-based
self-supporting
electrodes
for
Zn–air
batteries
have
been
systematically
summarized
according
to
the
recent
research
progress.
Nano Letters,
Год журнала:
2023,
Номер
23(17), С. 8331 - 8338
Опубликована: Авг. 30, 2023
The
great
interest
in
large-scale
electrochemical
water
splitting
toward
clean
hydrogen
has
spurred
large
numbers
of
studies
on
developing
cost-efficient
and
high-performance
bifunctional
electrocatalysts.
Here,
a
Prussian-blue-analogue-derived
method
is
proposed
to
prepare
honeycomb-like
ultrathin
heterogeneous
Co2P-Fe2P
nanosheets
nickel
foam,
showing
low
overpotentials
0.080,
0.088,
0.109
V
for
the
evolution
reaction
(HER)
at
10
mA
cm-2
as
well
0.290,
0.370,
0.730
oxygen
(OER)
50
alkaline,
acidic,
neutral
electrolytes,
respectively.
When
directly
applied
universal-pH
electrolysis,
excellent
performances
are
achieved
especially
ultralow
voltages
1.45
cm-2,
1.66
100
1.79
500
under
alkaline
conditions.
In
situ
Raman
spectroscopy
measurements
demonstrate
that
HER
performance
can
be
attributed
while
ultrahigh
OER
originates
from
reconstruction-induced
oxyhydroxides.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(17), С. 10185 - 10195
Опубликована: Янв. 1, 2024
A
highly
reversible
bifunctional
electrocatalyst
for
flexible
Zn
air
batteries
was
fabricated
featuring
pyridinic-N
exclusively
enriched
CNT
encased
NiFe
interfacial
alloy
nanoparticles
derived
from
an
LDH
template
on
knitted
carbon
fiber
cloth.
Advanced Energy Materials,
Год журнала:
2024,
Номер
14(30)
Опубликована: Май 28, 2024
Abstract
The
oxygen
evolution
reaction
(OER)
and
reduction
(ORR)
are
cornerstone
half
reactions
involved
in
many
renewable
energy
technologies.
High‐density
single‐atom
catalysts
maximize
the
atom
utilization
isolated
active
sites.
Furthermore,
introduction
of
pyri‐N
into
carbon‐based
nanostructures
as
an
electrocatalyst
creates
abundance
Here,
innovative
strategy
is
reported
based
on
atomic
scale
dispersion
Co
atoms
enriched
carbon
nanotube
encapsulated
Ni
nanoparticles
grown
3D
electrospun
nanofiber
nano‐assemblies.
Notably,
SA
Ni‐NCNT/CNF
exhibited
excellent
OER
ORR
activity
terms
low
overpotentials
higher
half‐wave
potentials.
atomically
distributed
allows
maximum
exposure
sites
dominated
multidimensional
skeleton,
synergistic
effects
with
greatly
reduced
delocalization
around
metal
centers
provided
ideal
environment
for
interactions
intermediates,
thus
facilitating
4e
−
pathway,
evidenced
by
DFT
calculations.
Moreover,
Zn‐air
batteries
using
a
air
cathode
high‐power
density
admirable
specific
capacity.
This
studies
may
provide
avenue
rational
modulation
cost‐effective,
large‐scale
synthesis
bifunctional
electrocatalysts
rechargeable
anion
exchange
membrane
fuel
cell.
Nano-Micro Letters,
Год журнала:
2024,
Номер
16(1)
Опубликована: Июль 9, 2024
Combining
single
atoms
with
clusters
or
nanoparticles
is
an
emerging
tactic
to
design
efficient
electrocatalysts.
Both
synergy
effect
and
high
atomic
utilization
of
active
sites
in
the
composite
catalysts
result
enhanced
electrocatalytic
performance,
simultaneously
provide
a
radical
analysis
interrelationship
between
structure
activity.
In
this
review,
recent
advances
single-atomic
site
coupled
are
emphasized.
Firstly,
synthetic
strategies,
characterization,
dynamics
types
clusters/nanoparticles
introduced,
then
key
factors
controlling
discussed.
Next,
several
clean
energy
catalytic
reactions
performed
over
synergistic
illustrated.
Eventually,
encountering
challenges
recommendations
for
future
advancement
energy-transformation
electrocatalysis
outlined.