Advanced Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 20, 2025
Abstract
Precisely
optimizing
the
electronic
metal
support
interaction
(EMSI)
of
electrocatalysts
and
tuning
structures
active
sites
are
crucial
for
accelerating
water
adsorption
dissociation
kinetics
in
alkaline
hydrogen
evolution
reaction
(HER).
Herein,
an
effective
strategy
is
applied
to
modify
structure
Ru
nanoparticles
(Ru
NPs
)
by
incorporating
single
atoms
SAs
Cr
atomic
pairs
(RuCr
APs
onto
a
nitrogen‐doped
carbon
(N–C)
through
optimized
EMSI.
The
resulting
catalyst,
‐RuCr
‐N‐C,
shows
exceptional
performance
HER,
achieving
six
times
higher
turnover
frequency
(TOF)
13.15
s⁻¹
at
overpotential
100
mV,
compared
that
commercial
Pt/C
(2.07
s⁻¹).
Additionally,
catalyst
operates
lower
current
density
10
mA·cm⁻
2
(η
=
31
mV),
outperforming
34
mV).
Experimental
results
confirm
RuCr
modified
main
facilitating
rate‐determining
steps
dissociation.
Moreover,
Ru–Cr
also
plays
vital
role
modulating
desorption.
This
study
presents
synergistic
approach
rationally
combining
atoms,
pairs,
with
EMSI
effects
advance
development
efficient
HER.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(14)
Published: Feb. 9, 2023
Oxygen
vacancies-enriched
black
TiO2
is
one
promising
support
for
enhancing
hydrogen
evolution
reaction
(HER).
Herein,
oxygen
vacancies
enriched
supported
sub-nanometer
Pt
clusters
(Pt/TiO2
-OV
)
with
metal
interactions
designed
through
solvent-free
microwave
and
following
low-temperature
electroless
approach
the
first
time.
High-temperature
strong
reductants
are
not
required
then
can
avoid
aggregation
of
decorated
species.
Experimental
theoretical
calculation
verify
that
created
exhibit
synergistic
effects
optimizing
kinetics.
Based
on
it,
Pt/TiO2
presents
remarkable
electrocatalytic
performance
18
mV
to
achieve
10
mA
cm-2
coupled
small
Tafel
slope
12
dec-1
.
This
work
provides
quick
synthetic
strategy
preparing
titanium
dioxide
based
nanomaterials.
Energy & Environmental Science,
Journal Year:
2023,
Volume and Issue:
16(9), P. 4009 - 4019
Published: Jan. 1, 2023
Unique
PtMoPdRhNi
high-entropy
alloy
nanocrystals
(NCs)
catalysts
assembled
by
radial
nanosheets
with
multiple
active
sites
different
local
chemical
environments
and
the
interaction
of
d–d
electron
for
superior
HER
performance.
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.
Small,
Journal Year:
2023,
Volume and Issue:
19(29)
Published: March 22, 2023
Abstract
Platinum
is
one
of
the
best‐performing
catalysts
for
hydrogen
evolution
reaction
(HER).
However,
high
cost
and
scarcity
severely
hinder
large‐scale
application
Pt
electrocatalysts.
Constructing
highly
dispersed
ultrasmall
entities
thereby
a
very
effective
strategy
to
increase
utilization
mass
activities,
reduce
costs.
Herein,
composed
mixture
single
atoms,
clusters,
nanoparticles
are
synthesized
on
mesoporous
N‐doped
carbon
nanospheres.
The
presence
demonstrated
by
combining
among
others
aberration‐corrected
annular
dark‐field
scanning
transmission
electron
microscopy,
X‐ray
absorption
spectroscopy,
electrochemical
CO
stripping.
best
catalyst
exhibits
excellent
geometric
HER
activity,
respectively
≈4
26
times
higher
than
that
commercial
Pt/C
reference
supported
nonporous
nanofibers
with
similar
loadings.
Noteworthily,
after
optimization
geometrical
electrode
loading,
ultrahigh
activities
(56
±
3
A
mg
−1
11.7
0.6
Cat
at
−50
mV
vs.
reversible
electrode),
which
≈1.5
58
highest
single‐atom
cluster‐based
reported
so
far.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: June 13, 2024
Single-atom
electrocatalysts
(SACs)
are
a
class
of
promising
materials
for
driving
electrochemical
energy
conversion
reactions
due
to
their
intrinsic
advantages,
including
maximum
metal
utilization,
well-defined
active
structures,
and
strong
interface
effects.
However,
SACs
have
not
reached
full
commercialization
broad
industrial
applications.
This
review
summarizes
recent
research
achievements
in
the
design
crucial
electrocatalytic
on
sites,
coordination,
substrates,
as
well
synthesis
methods.
The
key
challenges
facing
activity,
selectivity,
stability,
scalability,
highlighted.
Furthermore,
it
is
pointed
out
new
strategies
address
these
increasing
activity
enhancing
utilization
improving
optimizing
local
environment,
developing
fabrication
techniques,
leveraging
insights
from
theoretical
studies,
expanding
potential
Finally,
views
offered
future
direction
single-atom
electrocatalysis
toward
commercialization.
Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: July 6, 2024
Abstract
Catalyst
systems
populated
by
high-density
single
atoms
are
crucial
for
improving
catalytic
activity
and
selectivity,
which
can
potentially
maximize
the
industrial
prospects
of
heterogeneous
single-atom
catalysts
(SACs).
However,
achieving
high-loading
SACs
with
metal
contents
above
10
wt%
remains
challenging.
Here
we
describe
a
general
negative
pressure
annealing
strategy
to
fabricate
ultrahigh-loading
up
27.3–44.8
13
different
metals
on
typical
carbon
nitride
matrix.
Furthermore,
our
approach
enables
synthesis
high-entropy
(HESACs)
that
exhibit
coexistence
multiple
high
contents.
In-situ
aberration-corrected
HAADF-STEM
(AC-STEM)
combined
ex-situ
X-ray
absorption
fine
structure
(XAFS)
demonstrate
treatment
accelerates
removal
anionic
ligand
in
precursors
boosts
bonding
species
N
defective
sites,
enabling
formation
dense
N-coordinated
sites.
Increasing
loading
platinum
(Pt)
SAC
41.8
significantly
enhances
propane
oxidation
towards
liquid
products,
including
acetone,
methanol,
acetic
acid
et
al.
This
work
presents
straightforward
universal
many
low-cost
efficient
transformations.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(19)
Published: Jan. 30, 2024
Abstract
The
integration
of
graphene
and
metal–organic
frameworks
(MOFs)
has
numerous
implications
across
various
domains,
but
fabricating
such
assemblies
is
often
complicated
time‐consuming.
Herein,
a
one‐step
preparation
graphene‐MOF
assembly
presented
by
directly
impregnating
vertical
(VG)
arrays
into
the
zeolitic
imidazolate
framework
(ZIF)
precursors
under
ambient
conditions.
This
approach
can
effectively
assemble
multiple
ZIFs,
including
ZIF‐7,
ZIF‐8,
ZIF‐67,
resulting
in
their
uniform
dispersion
on
VG
with
adjustable
sizes
shapes.
Hydrogen
defects
surface
are
critical
inducing
high‐efficiency
ZIF
assembly,
acting
as
reactive
sites
to
interact
facilitate
crystallisation.
versatility
VG‐ZIF‐67
further
demonstrated
exploring
process
MOF
amorphization.
Surprisingly,
this
leads
an
amorphous
thin‐film
coating
formed
(named
VG‐IL‐amZIF‐67),
which
preserves
short‐range
molecular
bonds
crystalline
ZIF‐67
while
sacrificing
long‐range
order.
Such
unique
film‐on‐graphene
architecture
maintains
essential
characteristics
functionalities
within
disordered
arrangement,
making
it
well‐suited
for
electrocatalysis.
In
electrochemical
oxygen
reduction,
VG‐IL‐amZIF‐67
exhibits
exceptional
activity,
selectivity,
stability
produce
H
2
O
acid
media.