Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(28), P. 15528 - 15537
Published: July 10, 2023
Demetalation,
caused
by
the
electrochemical
dissolution
of
metal
atoms,
poses
a
significant
challenge
to
practical
application
single-atom
catalytic
sites
(SACSs)
in
proton
exchange
membrane-based
energy
technologies.
One
promising
approach
inhibit
SACS
demetalation
is
use
metallic
particles
interact
with
SACSs.
However,
mechanism
underlying
this
stabilization
remains
unclear.
In
study,
we
propose
and
validate
unified
which
can
Fe
Metal
act
as
electron
donors,
decreasing
oxidation
state
increasing
density
at
FeN4
position,
thereby
strengthening
Fe-N
bond,
inhibiting
dissolution.
Different
types,
forms,
contents
increase
bond
strength
varying
extents.
A
linear
correlation
between
state,
strength,
amount
supports
mechanism.
Our
screening
particle-assisted
led
78%
reduction
dissolution,
enabling
continuous
operation
for
up
430
h
fuel
cell.
These
findings
contribute
development
stable
SACSs
applications.
Advanced Materials,
Journal Year:
2022,
Volume and Issue:
35(9)
Published: Dec. 19, 2022
Abstract
Rechargeable
zinc–air
batteries
typically
require
efficient,
durable,
and
inexpensive
bifunctional
electrocatalysts
to
support
oxygen
reduction/evolution
reactions
(ORR/OER).
However,
sluggish
kinetics
mass
transportation
challenges
must
be
addressed
if
the
performance
of
these
catalysts
is
enhanced.
Herein,
a
strategy
fabricate
catalyst
comprising
atomically
dispersed
iron
atoms
supported
on
mesoporous
nitrogen‐doped
carbon
(Fe
SAs/NC)
with
accessible
metal
sites
optimized
electronic
metal–support
interactions
developed.
Both
experimental
results
theoretical
calculations
reveal
that
engineered
structures
active
can
regulate
charge
distribution
Fe
centers
optimize
adsorption/desorption
oxygenated
intermediates.
The
SAs/NC
containing
1
N
4
O
achieves
remarkable
ORR
activity
over
entire
pH
range,
half‐wave
potentials
0.93,
0.83,
0.75
V
(vs
reversible
hydrogen
electrode)
in
alkaline,
acidic,
neutral
electrolytes,
respectively.
In
addition,
it
demonstrates
promising
low
overpotential
320
mV
at
10
mA
cm
−2
for
OER
alkaline
conditions.
battery
assembled
exhibits
superior
than
Pt/C+RuO
2
counterpart
terms
peak
power
density,
specific
capacity,
cycling
stability.
These
findings
demonstrate
importance
structure
engineering
directing
catalytic
activity.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(25)
Published: April 11, 2023
The
development
of
rechargeable
zinc-air
batteries
is
heavily
dependent
on
bifunctional
oxygen
electrocatalysts
to
offer
exceptional
reduction/evolution
reaction
(ORR/OER)
activities.
However,
the
design
such
with
high
activity
and
durability
challenging.
Herein,
a
strategy
proposed
create
an
electrocatalyst
comprised
copper-cobalt
diatomic
sites
highly
porous
nitrogen-doped
carbon
matrix
(Cu-Co/NC)
abundantly
accessible
metal
optimal
geometric
electronic
structures.
Experimental
findings
theoretical
calculations
demonstrate
that
synergistic
effect
Cu-Co
dual-metal
metal-N4
coordination
induce
asymmetric
charge
distributions
moderate
adsorption/desorption
behavior
intermediates.
This
exhibits
extraordinary
electrocatalytic
activities
in
alkaline
media,
half-wave
potential
0.92
V
for
ORR
low
overpotential
335
mV
at
10
mA
cm-2
OER.
In
addition,
it
demonstrates
acidic
(0.85
V)
neutral
(0.74
media.
When
applied
battery,
achieves
operational
performance
outstanding
(510
h),
ranking
as
one
most
efficient
reported
date.
work
importance
engineering
isolated
boosting
electrochemical
energy
devices.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(15), P. 4878 - 4932
Published: Jan. 1, 2023
Recently,
the
missing
link
between
homogeneous
and
heterogeneous
catalysis
has
been
found
it
was
named
single-atom
(SAC).
However,
SAC
field
still
faces
important
challenges,
one
of
which
is
controlling
bonding/coordination
single
atoms
support
in
order
to
compensate
for
increase
surface
energy
when
particle
size
reduced
due
atomic
dispersion.
Excellent
candidates
meet
this
requirement
are
carbon
nitride
(CN)-based
materials.
Metal
can
be
firmly
trapped
nitrogen-rich
coordination
sites
CN
materials,
makes
them
a
unique
class
hosts
preparing
catalysts
(SACs).
As
most
promising
two-dimensional
supports
stabilize
isolated
metal
atoms,
materials
have
increasingly
employed
SACs.
Herein,
we
will
cover
recent
advances
single-atoms
supported
by
In
review,
characterization
techniques
challenges
faced
topic
discussed,
commonly
synthetic
methods
delineated
different
Finally,
catalytic
performance
SACs
based
on
nitrides
reviewed
with
special
focus
their
photocatalytic
applications.
particular,
prove
as
non-innocent
support.
The
relationship
two-way,
where
change
electronic
properties
support,
while
features
matrix
tune
activity
reactions.
highlight
frontiers
field,
including
analytical
method
development,
truly
controlled
methods,
allowing
fine
control
loading
multi-element
synthesis,
how
understanding
two-way
exchange
behind
push
next
level.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(7), P. 2759 - 2803
Published: Jan. 1, 2023
The
catalytic
transformation
of
CO
2
into
valuable
fuels/chemicals
is
a
promising
and
economically
profitable
process
because
it
offers
an
alternative
toward
fossil
feedstocks
the
benefit
transforming
cycling
on
scale-up.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(18), P. 10259 - 10267
Published: April 25, 2023
Realizing
efficient
hydrogenation
of
N2
molecules
in
the
electrocatalytic
nitrogen
reduction
reaction
(NRR)
is
crucial
achieving
high
activity
at
a
low
potential
because
it
theoretically
requires
higher
equilibrium
than
other
steps.
Analogous
to
metal
hydride
complexes
for
reduction,
this
step
by
chemical
can
weaken
dependence
initial
process.
However,
strategy
rarely
reported
NRR,
and
catalytic
mechanism
remains
ambiguous
lacks
experimental
evidence.
Here,
we
show
highly
electrocatalyst
(ruthenium
single
atoms
anchored
on
graphdiyne/graphene
sandwich
structures)
with
hydrogen
radical-transferring
mechanism,
which
graphdiyne
(GDY)
generates
radicals
(H•),
effectively
activate
generate
NNH
(•NNH).
A
dual-active
site
constructed
suppress
competing
evolution,
where
preferentially
adsorbs
GDY
Ru
serve
as
adsorption
•NNH
promote
further
NH3
synthesis.
As
result,
selectivity
are
obtained
simultaneously
-0.1
V
versus
reversible
electrode.
Our
findings
illustrate
novel
transfer
that
greatly
reduce
maintain
NRR
provide
powerful
guidelines
design
concept
electrocatalysts.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(40)
Published: June 7, 2023
The
pursuit
of
high
metal
utilization
in
heterogeneous
catalysis
has
triggered
the
burgeoning
interest
various
atomically
dispersed
catalysts.
Our
aim
this
review
is
to
assess
key
recent
findings
synthesis,
characterization,
structure-property
relationship
and
computational
studies
dual-atom
catalysts
(DACs),
which
cover
full
spectrum
applications
thermocatalysis,
electrocatalysis
photocatalysis.
In
particular,
combination
qualitative
quantitative
characterization
with
cooperation
DFT
insights,
synergies
superiorities
DACs
compare
counterparts,
high-throughput
catalyst
exploration
screening
machine-learning
algorithms
are
highlighted.
Undoubtably,
it
would
be
wise
expect
more
fascinating
developments
field
as
tunable
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(26)
Published: April 28, 2023
Artificial
photosynthesis
is
a
promising
strategy
for
converting
carbon
dioxide
(CO2
)
and
water
(H2
O)
into
fuels
value-added
chemical
products.
However,
photocatalysts
usually
suffered
from
low
activity
product
selectivity
due
to
the
sluggish
dynamic
transfer
of
photoexcited
charge
carriers.
Herein,
we
describe
anchoring
Ag
single
atoms
on
hollow
porous
polygonal
C3
N4
nanotubes
(PCN)
form
photocatalyst
Ag1
@PCN
with
Ag-N3
coordination
CO2
photoreduction
using
H2
O
as
reductant.
The
as-synthesized
exhibits
high
CO
production
rate
0.32
μmol
h-1
(mass
catalyst:
2
mg),
(>94
%),
an
excellent
stability
in
long
term.
Experiments
density
functional
theory
(DFT)
reveal
that
strong
metal-support
interactions
(Ag-N3
favor
*CO2
adsorption,
*COOH
generation
desorption,
accelerate
carriers
between
atoms,
thereby
accounting
enhanced
selectivity.
This
work
provides
deep
insight
important
role
enhancing
photoactivity
photoreduction.