Scientific Reports,
Journal Year:
2025,
Volume and Issue:
15(1)
Published: March 14, 2025
Precisely
regulating
active
sites
is
vital
for
promoting
the
oxygen
reduction
reaction
(ORR)
activity.
Here
we
reported
highly
Ni-Pd
co-doped
N-coordinated
graphene
towards
ORR
achieved
by
edge
termination
and
O
doping.
Our
first-principles
calculations
demonstrated
that
effectively
boost
activity,
armchair-edge
was
energetically
more
favorable
than
zigzag-edge
termination.
Notably,
after
doping
center,
armchair
edge-terminated
site
exhibited
better
lowest
overpotential
only
0.31
V.
This
improvement
in
activity
attributed
to
shift
of
d-band
center
Ni
atom
toward
Fermi-level
Pd
away
from
Fermi-level,
thus
*OH
adsorption
strength.
work
paves
way
developing
graphene-based
dual-atom
catalysts
through
engineering.
Chemical Science,
Journal Year:
2024,
Volume and Issue:
15(14), P. 5082 - 5112
Published: Jan. 1, 2024
This
review
systematically
introduces
how
to
regulate
the
electronic
structure
and
geometric
configuration
of
atomic
catalysts
achieve
high-efficiency
electrocatalysis
performances
by
analyzing
detailed
electrocatalytic
applications
mechanisms.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
63(3)
Published: Nov. 24, 2023
Abstract
Modulating
the
surface
and
spatial
structure
of
host
is
associated
with
reactivity
active
site,
also
enhances
mass
transfer
effect
CO
2
electroreduction
process
(CO
RR).
Herein,
we
describe
development
two‐step
ligand
etch–pyrolysis
to
access
an
asymmetric
dual‐atomic‐site
catalyst
(DASC)
composed
a
yolk–shell
carbon
framework
(Zn
1
Mn
‐SNC)
derived
from
S,N‐coordinated
Zn−Mn
dimers
anchored
on
metal–organic
(MOF).
In
Zn
‐SNC,
electronic
effects
S/N−Zn−Mn−S/N
configuration
are
tailored
by
strong
interactions
between
dual
sites
co‐coordination
S/N
atoms,
rendering
structural
stability
atomic
distribution.
H‐cell,
‐SNC
DASC
shows
low
onset
overpotential
50
mV
high
Faraday
efficiency
97
%
applied
343
mV,
thus
outperforming
counterparts,
in
flow
cell,
it
reaches
current
density
500
mA
cm
−2
at
−0.85
V,
benefitting
accessibility
sites.
DFT
simulations
showed
that
diatomic
site
optimal
adsorption
strength
COOH*
lowers
reaction
energy
barrier,
boosting
intrinsic
RR
activity
DASC.
The
structure‐property
correlation
found
this
study
suggests
new
ideas
for
highly
accessible
catalysts.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(37)
Published: May 6, 2024
Abstract
The
exploitation
of
highly
activity
oxygen
evolution
reaction
(OER)
electrocatalysts
is
critical
for
the
application
electrocatalytic
water
splitting.
Triggering
lattice
mechanism
(LOM)
expected
to
provide
a
promising
pathway
overcome
sluggish
OER
kinetics,
however,
effectively
enhancing
involvement
remains
challenging.
In
this
study,
fabrication
B,
Fe
co‐doped
CoP
(B,
Fe─CoP)
nanofibers
reported,
which
serve
as
efficient
electrocatalyst
through
phosphorization
and
boronation
treatment
Fe‐doped
Co
3
O
4
nanofibers.
Experimental
results
combined
with
theoretical
calculations
reveal
that
simultaneous
incorporation
both
B
can
more
trigger
participation
in
CoFe
oxyhydroxides
reconstructed
from
Fe─CoP
compared
incorporating
only
or
Fe.
Therefore,
optimized
exhibit
superb
low
overpotentials
361
376
mV
at
1000
mA
cm
−2
alkaline
freshwater
natural
seawater,
respectively.
present
work
provides
significant
guidelines
innovative
design
concepts
development
following
LOM
pathway.
Advanced Science,
Journal Year:
2024,
Volume and Issue:
11(33)
Published: July 1, 2024
Abstract
Modifying
the
coordination
or
local
environments
of
single‐,
di‐,
tri‐,
and
multi‐metal
atom
(SMA/DMA/TMA/MMA)‐based
materials
is
one
best
strategies
for
increasing
catalytic
activities,
selectivity,
long‐term
durability
these
materials.
Advanced
sheet
supported
by
metal
atom‐based
have
become
a
critical
topic
in
fields
renewable
energy
conversion
systems,
storage
devices,
sensors,
biomedicine
owing
to
maximum
utilization
efficiency,
precisely
located
centers,
specific
electron
configurations,
unique
reactivity,
precise
chemical
tunability.
Several
offer
excellent
support
are
attractive
applications
energy,
medical
research,
such
as
oxygen
reduction,
production,
hydrogen
generation,
fuel
selective
detection,
enzymatic
reactions.
The
strong
metal–metal
metal–carbon
with
metal–heteroatom
(i.e.,
N,
S,
P,
B,
O)
bonds
stabilize
optimize
electronic
structures
atoms
due
interfacial
interactions,
yielding
activities.
These
provide
models
understanding
fundamental
problems
multistep
This
review
summarizes
substrate
structure‐activity
relationship
different
active
sites
based
on
experimental
theoretical
data.
Additionally,
new
synthesis
procedures,
physicochemical
characterizations,
biomedical
discussed.
Finally,
remaining
challenges
developing
efficient
SMA/DMA/TMA/MMA‐based
presented.
Nano-Micro Letters,
Journal Year:
2024,
Volume and Issue:
16(1)
Published: Feb. 29, 2024
Abstract
The
exploration
of
sustainable
energy
utilization
requires
the
implementation
advanced
electrochemical
devices
for
efficient
conversion
and
storage,
which
are
enabled
by
usage
cost-effective,
high-performance
electrocatalysts.
Currently,
heterogeneous
atomically
dispersed
catalysts
considered
as
potential
candidates
a
wide
range
applications.
Compared
to
conventional
catalysts,
metal
atoms
in
carbon-based
have
more
unsaturated
coordination
sites,
quantum
size
effect,
strong
metal–support
interactions,
resulting
exceptional
catalytic
activity.
Of
these,
dual-atomic
(DACs)
attracted
extensive
attention
due
additional
synergistic
effect
between
two
adjacent
atoms.
DACs
advantages
full
active
site
exposure,
high
selectivity,
theoretical
100%
atom
utilization,
ability
break
scaling
relationship
adsorption
free
on
sites.
In
this
review,
we
summarize
recent
research
advancement
DACs,
includes
(1)
comprehensive
understanding
synergy
atomic
pairs;
(2)
synthesis
DACs;
(3)
characterization
methods,
especially
aberration-corrected
scanning
transmission
electron
microscopy
synchrotron
spectroscopy;
(4)
energy-related
last
part
focuses
great
catalysis
small
molecules,
such
oxygen
reduction
reaction,
CO
2
hydrogen
evolution
N
reaction.
future
challenges
opportunities
also
raised
prospective
section.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(10), P. 6893 - 6904
Published: March 1, 2024
Owing
to
the
electrical
conductivity
and
periodic
porosity,
conductive
metal–organic
framework
(cMOF)
ultrathin
films
open
new
perspectives
photocatalysis.
The
space-selective
assembly
of
catalytic
sites
photosensitizers
in/on
cMOF
is
favorable
for
promoting
separation
photogenerated
carriers
mass
transfer.
However,
controllable
integration
functional
units
into
film
rarely
reported.
Herein,
via
synergistic
effect
steric
hindrance
an
electrostatic-driven
strategy,
dinuclear-metal
molecular
catalysts
(DMC)
perovskite
(PVK)
quantum
dot
were
immobilized
channels
onto
surface
films,
respectively,
affording
[DMC@cMOF]-PVK
photocatalysts.
In
this
unique
heterostructure,
not
only
facilitated
charge
transfer
from
PVK
DMC
but
also
guaranteed
Using
H2O
as
electron
donor,
realized
a
133.36
μmol·g–1·h–1
CO
yield
in
photocatalytic
CO2
reduction,
much
higher
than
DMC-PVK.
excellent
light
transmission
multilayers
integrated
increase
per
unit
area,
10-layer
device
1115.92
μmol·m–2
4
h,
which
was
8-fold
that
powder
counterpart.
This
work
lightens
development
cMOF-based
composite
paves
novel
avenue
photocatalyst.
Nano-Micro Letters,
Journal Year:
2024,
Volume and Issue:
17(1)
Published: Sept. 25, 2024
Abstract
Green
hydrogen
from
water
splitting
has
emerged
as
a
critical
energy
vector
with
the
potential
to
spearhead
global
transition
fossil
fuel-independent
society.
The
field
of
catalysis
been
revolutionized
by
single-atom
catalysts
(SACs),
which
exhibit
unique
and
intricate
interactions
between
atomically
dispersed
metal
atoms
their
supports.
Recently,
bimetallic
SACs
(bimSACs)
have
garnered
significant
attention
for
leveraging
synergistic
functions
two
ions
coordinated
on
appropriately
designed
BimSACs
offer
an
avenue
rich
metal–metal
metal–support
cooperativity,
potentially
addressing
current
limitations
in
effectively
furnishing
transformations
involve
synchronous
proton–electron
exchanges,
substrate
activation
reversible
redox
cycles,
simultaneous
multi-electron
transfer,
regulation
spin
states,
tuning
electronic
properties,
cyclic
states
low
energies.
This
review
aims
encapsulate
growing
advancements
bimSACs,
emphasis
pivotal
role
generation
via
splitting.
We
subsequently
delve
into
advanced
experimental
methodologies
elaborate
characterization
SACs,
elucidate
discuss
local
coordination
environment.
Overall,
we
present
comprehensive
discussion
deployment
bimSACs
both
evolution
reaction
oxygen
reaction,
half-reactions
electrolysis
process.
Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: Nov. 1, 2024
Double-atom
catalysts
(DACs)
have
opened
distinctive
paradigms
in
the
field
of
rapidly
developing
atomic
catalysis
owing
to
their
great
potential
for
promoting
catalytic
performance
various
reaction
systems.
However,
increasing
loading
and
extending
service
life
metal
active
centres
represents
a
considerable
challenge
efficient
utilization
DACs.
Here,
we
rationally
design
asymmetric
nitrogen,
sulfur-coordinated
diatomic
iron
on
highly
defective
nitrogen-doped
carbon
nanosheets
(denoted
A-Fe
