ACS Nano,
Journal Year:
2024,
Volume and Issue:
18(41), P. 28433 - 28443
Published: Oct. 4, 2024
Manipulation
of
the
spin
state
holds
great
promise
to
improve
electrochemical
activity
transition
metal-based
catalysts.
However,
underlying
relationship
between
nonplanar
metal
coordination
environment
and
states
remains
be
explored.
Herein,
we
report
precise
regulation
Fe
atomic
d-orbital
energy
level
into
an
irregular
tetrahedral
crystal
field
configuration
by
introducing
P
atoms.
With
increase
number,
magnetic
moment
decreases
linearly
from
3.8
μB
0.2
μB,
high
content
31%
5%.
Significantly,
a
volcanic
curve
Fe-based
catalysts
(Fe-N
Chemical Science,
Journal Year:
2024,
Volume and Issue:
15(36), P. 14585 - 14607
Published: Jan. 1, 2024
The
development
of
high-efficiency
atomic-level
catalysts
for
energy-conversion
and
-storage
technologies
is
crucial
to
address
energy
shortages.
spin
states
diatomic
(DACs)
are
closely
tied
their
catalytic
activity.
Adjusting
the
DACs'
active
centers
can
directly
modify
occupancy
d-orbitals,
thereby
influencing
bonding
strength
between
metal
sites
intermediates
as
well
transfer
during
electro
reactions.
Herein,
we
discuss
various
techniques
characterizing
atomic
strategies
modulating
center
states.
Next,
outline
recent
progress
in
study
effects
DACs
oxygen
reduction
reaction
(ORR),
evolution
(OER),
hydrogen
(HER),
electrocatalytic
nitrogen/nitrate
(eNRR/NO
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(32)
Published: May 30, 2024
Abstract
Rechargeable
Zn–air
batteries
(ZABs)
are
promising
for
energy
storage
and
conversion.
However,
the
high
charging
voltage
low
efficiency
hinder
their
commercialization.
Herein,
these
challenges
addressed
by
employing
precisely
constructed
multifunctional
Fe–Co
diatomic
site
catalysts
(FeCo‐DACs)
integrating
iodide/iodate
redox
into
ZABs
to
create
Zinc–air/iodide
hybrid
(ZAIHBs)
with
highly
efficient
catalyst.
The
strong
coupling
between
3d
orbitals
of
Fe
Co
weakens
excessively
binding
strength
active
sites
intermediates,
enhancing
catalytic
activities
oxygen
reduction/evolution
reaction
redox.
Consequently,
FeCo‐DACs
exhibit
outstanding
bifunctional
activity
a
small
potential
gap
(Δ
E
=
0.66
V)
stability.
Moreover,
an
performance
toward
is
obtained.
Therefore,
FeCo‐DAC‐based
ZAIHBs
up
75%
at
10
mA
cm
−2
excellent
cycling
stability
(72%
after
500
h).
This
research
offers
critical
insights
rational
design
DACs
paves
way
high‐energy
devices.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 21, 2025
Abstract
Advancing
energy
conversion
technologies
requires
cost‐efficient
electrocatalysts
for
the
oxygen
reduction
reaction
(ORR).
Iron
phthalocyanine
(FePc)
emerges
as
a
scalable
and
economical
ORR
electrocatalyst.
However,
Fe–N
4
configuration
in
FePc
still
falls
short
of
satisfied
activity
stability
under
electrocatalytic
conditions.
Here,
an
effective
f‐p‐d
(Eu–O–Fe)
gradient
orbital
coupling
strategy
is
introduced
by
integrating
with
Eu
2
O
3
(FePc/Eu
)
to
enhance
spin
state
performance
Fe
center
through
precisely
designed,
synthetic
approach.
The
Eu─O
bond
promotes
electron
delocalization
shifts
from
low‐spin
intermediate‐spin,
increasing
e
g
occupancy.
This
modification
optimizes
adsorption
oxygen‐containing
intermediates
lowers
barrier.
Notably,
increased
accelerates
charge
transfer
releasing
more
unpaired
electrons,
improving
kinetics.
Furthermore,
f‐band
serves
buffer
layer
compensation
during
ORR,
further
stabilizing
covalency
electronic
atomic
boosting
durability.
one‐batch
synthesis
produces
exceeding
300
g
FePc/Eu
,
achieving
half‐wave
potential
0.931
V
(vs
RHE)
at
cost
less
than
1/15
commercial
Pt/C.
It
demonstrates
exceptional
aluminum–air
batteries,
highlighting
its
significant
application
potential.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(49)
Published: Sept. 13, 2024
Abstract
There
has
been
a
growing
interest
in
developing
catalysts
to
enable
the
reversible
iodine
conversion
reaction
for
high‐performance
aqueous
zinc‐iodine
batteries
(AZIBs).
While
diatomic
(DACs)
have
demonstrated
superior
performance
various
catalytic
reactions
due
their
ability
facilitate
synergistic
charge
interactions,
application
AZIBs
remains
unexplored.
Herein,
we
present,
first
time,
DAC
comprising
Mn−Zn
dual
atoms
anchored
on
nitrogen‐doped
carbon
matrix
(MnZn−NC)
loading,
resulting
AZIB
with
capacity
of
224
mAh
g
−1
at
1
A
and
remarkable
cycling
stability
over
320,000
cycles.
The
electron
hopping
along
Mn−N−Zn
bridge
is
stimulated
via
spin
exchange
mechanism.
This
process
broadens
Mn
3d
xy
band
width
enhances
metallic
character
catalyst,
thus
facilitating
transfer
between
intermediates.
Additionally,
increased
occupancy
within
d‐orbital
Zn
elevates
Zn's
d‐band
center,
thereby
enhancing
chemical
interactions
MnZn−NC
I‐based
species.
Furthermore,
our
mechanism
demonstrates
potential
applicability
other
Metal‐Zn−NC
DACs
spin‐polarized
atoms.
Our
work
elucidates
clear
mechanistic
understanding
provides
new
insights
into
catalyst
design
AZIBs.
ACS Materials Letters,
Journal Year:
2024,
Volume and Issue:
6(7), P. 2858 - 2887
Published: June 7, 2024
Oxygen
reduction
reaction
(ORR),
involving
either
a
two-electron
(2e–)
pathway
or
four-electron
(4e–)
pathway,
is
an
important
in
energy
conversion
and
storage
systems.
It
well-known
that
metal–nitrogen–carbon
(M–N–C)
catalysts,
as
emerging
state-of-the-art
electrocatalysts,
are
applied
to
fuel
cells
via
the
4e–
(e.g.,
Fe–N–C)
while
generating
hydrogen
peroxide
2e–
Co–N–C).
However,
effects
of
MNx
C–N
species
on
catalytic
activity
ORR
require
thorough
clarification.
Especially,
real
active
sites
M–N–C
configuration
long-standing
conundrum.
In
this
review,
latest
advanced
catalysts
were
categorized
according
pathways
moieties.
Then,
coordination
atoms,
N-coordinated
structures,
pH
discussed.
The
detection
quantification
by
situ
Raman
spectroscopy
electrochemical
techniques
summarized.
Finally,
opportunities
challenges
for
with
efficient
highlighted.
ChemPlusChem,
Journal Year:
2024,
Volume and Issue:
89(11)
Published: July 16, 2024
Abstract
The
two‐electron
oxygen
reduction
reaction
(2e‐ORR)
for
the
sustainable
synthesis
of
hydrogen
peroxide
(H
2
O
)
has
demonstrated
considerable
potential
local
production
this
environmentally
friendly
chemical
oxidant
on
small,
medium,
and
large
scales.
This
method
offers
a
promising
alternative
to
energy‐intensive
anthraquinone
approach,
placing
primary
emphasis
development
efficient
electrocatalysts.
Improving
efficiency
electrocatalysts
uncovering
their
catalytic
mechanisms
are
essential
steps
in
achieving
high
2e‐ORR
activity,
selectivity,
stability.
comprehensive
review
summarizes
recent
advancements
in‐situ
H
production,
providing
detailed
overview
field.
In
particular,
delves
into
design,
fabrication,
investigation
active
sites
contributing
selectivity.
Additionally,
it
highlights
range
including
pure
metals
alloys,
transition
metal
compounds,
single‐atom
catalysts,
carbon‐based
catalysts
pathway.
Finally,
addresses
significant
challenges
opportunities
electrosynthesis,
as
well
future
research
directions.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(41)
Published: Aug. 17, 2024
Dual-atom
catalysts
(DACs)
with
atomically
dispersed
dual-sites,
as
an
extension
of
single-atom
(SACs),
have
recently
become
a
new
hot
topic
in
heterogeneous
catalysis
due
to
their
maximized
atom
efficiency
and
dual-site
diverse
synergy,
because
the
synergistic
diversity
dual-sites
achieved
by
asymmetric
microenvironment
tailoring
can
efficiently
boost
catalytic
activity
optimizing
electronic
structure
DACs.
Here,
this
work
first
summarizes
frequently-used
experimental
synthesis
characterization
methods
Then,
four
mechanisms
(cascade
mechanism,
assistance
co-adsorption
mechanism
bifunction
mechanism)
key
modulating
(active
site
strategy,
transverse/axial-modification
engineering,
distance
engineering
strain
engineering)
are
elaborated
comprehensively.
The
emphasis
is
placed
on
effects
DACs
oxygen/carbon
dioxide
reduction
reaction.
Finally,
some
perspectives
outlooks
also
addressed.
In
short,
review
useful
strategy
speed
up
high-performance
electrocatalysts
for
different
reactions.
