Abstract
The
commercial
utilization
of
low‐dimensional
catalysts
has
been
hindered
by
their
propensity
for
agglomeration
and
stacking,
greatly
minimizing
active
sites.
To
circumvent
this
problem,
materials
can
be
assembled
into
systematic
3D
architectures
to
synergistically
retain
the
benefits
constituent
nanomaterials,
with
value‐added
bulk
properties
such
as
increased
surface
area,
improved
charge
transport
pathways,
enhanced
mass
transfer,
leading
higher
catalytic
activity
durability
compared
constituents.
hierarchical
organization
building
blocks
within
structures
also
enables
precise
control
over
catalyst's
morphology,
composition,
chemistry,
facilitating
tailored
design
specific
electrochemical
applications.
Despite
surge
in
metal‐based
assemblies,
there
are
no
reviews
encompassing
different
types
assemblies
from
nanomaterials
electrocatalysis.
Herein,
review
addresses
gap
investigating
various
self‐supported
exploring
how
electrocatalytic
performance
elevated
through
structural
modifications
mechanistic
studies
tailor
them
reactions.
Chemical Society Reviews,
Год журнала:
2024,
Номер
53(5), С. 2693 - 2737
Опубликована: Янв. 1, 2024
Unprecedented
insights
into
electrochemical
surface
dynamics
from
operando
studies
inspire
electronic
and
topographical
strategies,
paving
the
way
for
sustained
electrocatalytic
performance
across
HER,
OER,
ORR,
CO
2
RR
applications.
Advanced Materials,
Год журнала:
2024,
Номер
36(41)
Опубликована: Авг. 15, 2024
Abstract
Modulating
the
electronic
structure
of
catalysts
to
effectively
couple
hydrogen
evolution
reaction
(HER)
and
oxygen
(OER)
is
essential
for
developing
high‐efficiency
anion
exchange
membrane
water
electrolyzer
(AEMWE).
Herein,
a
coral‐like
nanoarray
composed
nanosheets
through
synergistic
layering
effect
cobalt
1D
guiding
vanadium
synthesized,
which
promotes
extensive
contact
between
active
sites
electrolyte.
The
HER
OER
activities
can
be
enhanced
by
modulating
nitridation
phosphorization,
respectively,
enhancing
strength
metal‐H
bond
optimize
adsorption
facilitating
proton
transfer
improve
transformation
oxygen‐containing
intermediates.
Resultantly,
AEMWE
achieves
current
density
500
mA
cm
–2
at
1.76
V
1000
h
in
1.0
M
KOH
70
°C.
energy
consumption
4.21
kWh
Nm
–3
with
producing
cost
$0.93
per
kg
H
2
.
Operando
synchrotron
radiation
Bode
phase
angle
analyses
reveal
that
during
high‐energy
consumed
OER,
dissolution
species
transforms
distorted
Co−O
octahedral
into
regular
structures,
accompanied
shortening
Co−Co
length.
This
structural
facilitates
formation
intermediates,
thus
accelerating
kinetics.
ACS Nano,
Год журнала:
2024,
Номер
18(14), С. 9942 - 9957
Опубликована: Март 29, 2024
Highly
efficient,
cost-effective,
and
durable
electrocatalysts,
capable
of
accelerating
sluggish
reaction
kinetics
attaining
high
performance,
are
essential
for
developing
sustainable
energy
technologies
but
remain
a
great
challenge.
Here,
we
leverage
facile
heterostructure
design
strategy
to
construct
atomically
thin
Os@Pd
metallenes,
with
atomic-scale
Os
nanoclusters
varying
geometries
confined
on
the
surface
layer
Pd
lattice,
which
exhibit
excellent
bifunctional
properties
catalyzing
both
hydrogen
evolution
(HER)
oxygen
reduction
reactions
(ORR).
Importantly,
Os5%@Pd
metallenes
manifest
low
η10
overpotential
only
11
mV
in
1.0
M
KOH
electrolyte
as
well
highly
positive
E1/2
potential
0.92
V
0.1
(ORR),
along
superior
mass
activities
electrochemical
durability.
Theoretical
investigations
reveal
that
strong
electron
redistribution
between
elements
renders
precise
fine-tuning
respective
d-band
centers,
thereby
guiding
adsorption
intermediates
an
appropriate
binding
optimal
HER
ORR.
Transition-metal
dichalcogenides
(TMDs),
such
as
molybdenum
disulfide
(MoS2),
have
emerged
a
generation
of
nonprecious
catalysts
for
the
hydrogen
evolution
reaction
(HER),
largely
due
to
their
theoretical
adsorption
energy
close
that
platinum.
However,
efforts
activate
basal
planes
TMDs
primarily
centered
around
strategies
introducing
numerous
atomic
vacancies,
creating
vacancy–heteroatom
complexes,
or
applying
significant
strain,
especially
acidic
media.
These
approaches,
while
potentially
effective,
present
substantial
challenges
in
practical
large-scale
deployment.
Here,
we
report
gap-state
engineering
strategy
controlled
activation
S
atom
MoS2
through
metal
single-atom
doping,
effectively
tackling
both
efficiency
and
stability
alkaline
water
seawater
splitting.
A
versatile
synthetic
methodology
allows
fabrication
series
single-metal
atom-doped
materials
(M1/MoS2),
featuring
widely
tunable
densities
with
each
dopant
replacing
Mo
site.
Among
these
(Mn1,
Fe1,
Co1,
Ni1),
Co1/MoS2
demonstrates
outstanding
HER
performance
media,
overpotentials
at
mere
159
164
mV
100
mA
cm–2,
Tafel
slopes
41
45
dec–1,
respectively,
which
surpasses
all
reported
TMD-based
benchmark
Pt/C
during
splitting,
can
be
attributed
an
optimal
modulation
associated
sulfur
atoms.
Experimental
data
correlating
doping
density
identity
performance,
conjunction
calculations,
also
reveal
descriptor
linked
near-Fermi
gap
state
modulation,
corroborated
by
observed
increase
unoccupied
3p
states.
Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(35), С. 23577 - 23589
Опубликована: Янв. 1, 2024
The
synergistic
effect
of
PdCu
alloys
on
TiO
2
nanosheets
expands
the
light-absorption
range,
improves
adsorption
CO
and
H
O,
accelerates
photogenerated
electron
migration,
resulting
in
an
increased
CH
4
yield
with
a
selectivity
98.7%.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Авг. 2, 2024
Abstract
Orbital
hybridization
is
a
promising
approach
to
modulating
the
electronic
structure
of
designed
electrocatalysts
boost
reaction
kinetics.
In
contrast
d‐d
hybridization,
p‐d
orbital
between
p‐block
elements
and
d‐block
metals
can
provide
new
opportunities
modulate
properties
thus
promote
catalytic
performance.
Herein,
phosphorus‐doped
osmium
(P‐Os)
catalyst
through
ultrafast
(20
s)
microwave
plasma
engineering.
Theoretical
calculations
verify
d‐p
P
Os,
leading
modulation
d‐band
center
Os
active
site.
Specifically,
neighboring
exhibit
highest
activity,
facilitating
crucial
processes
such
as
H
2
O/H*
adsorption
dissociation.
The
overpotential
P‐Os
in
alkaline
seawater
only
152
mV
at
1
A
cm
−2
,
which
superior
reported
electrocatalysts.
Moreover,
synthesized
catalysts
are
integrated
into
an
anion
exchange
membrane
(AEM)
electrolyzer,
demonstrating
remarkable
AEM
electrolyzer
requires
1.86/2.02
V
achieve
500/1000
mA
current
densities.
Then,
achieved
have
great
potential
for
practical
electrocatalytic
water‐splitting
applications.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Ноя. 25, 2024
Precise
morphological
control
and
identification
of
structure-property
relationships
pose
formidable
challenges
for
high-entropy
alloys,
severely
limiting
their
rational
design
application
in
multistep
tandem
reactions.
Herein,
we
report
the
synthesis
sub-nanometric
metallenes
with
up
to
eight
metallic
elements
via
a
one-pot
wet-chemical
approach.
The
PdRhMoFeMn
exhibit
high
electrocatalytic
hydrogen
evolution
performances
6,
23,
26
mV
overpotentials
at
-10
mA
cm
