Advanced Energy Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 28, 2024
Abstract
Developing
cost‐effective,
high‐efficiency,
and
stable
electrocatalysts
for
the
hydrogen
evolution
reaction
(HER)
in
alkaline
electrolytes
is
of
critical
importance
realizing
renewable
technologies.
However,
sluggish
HER
kinetics
unsatisfied
stability
remain
challenges
their
practical
applications.
Herein,
a
hierarchically
porous
phosphorized
Pt‐Ni
nanohexapod/N‐doped
graphene
aerogel
(P‐PtNiNH/NGA)
constructed
by
an
oxidation‐phosphorization‐controlled
reconfiguration
strategy
presented.
It
enables
fast
water
dissociation
abundant
supply
ions,
strong
electron
interaction
optimal
intermediate
adsorption,
excellent
anchoring
effect
NGA
to
avoid
aggregation
Ostwald
ripening
PtNiNHs,
thus
exhibiting
superior
activity
exceptional
toward
HER.
The
P‐Pt
1
Ni
2
NH/NGA
exhibits
ultralow
overpotential
15
mV
at
current
density
10
mA
cm
−2
,
low
Tafel
slope
37
dec
−1
long‐term
stability,
which
are
commercial
Pt/C.
Moreover,
shows
high
mass
13.4
µg
large
TOF
value
13.5
s
100
mV,
8.8
times
9.0
higher
than
Pt/C
(under
same
Pt
loading
≈9.1
).
This
work
inspiration
catalyst
design
obtain
ideal
performance.
Nature Communications,
Год журнала:
2025,
Номер
16(1)
Опубликована: Янв. 22, 2025
The
H2-evolution
kinetics
play
a
pivotal
role
in
governing
the
photocatalytic
hydrogen-evolution
process.
However,
achieving
precise
regulation
of
H-adsorption
and
H-desorption
equilibrium
(Hads/Hdes)
still
remains
great
challenge.
Herein,
we
propose
fine-tuning
d-p
hybridization
strategy
to
precisely
optimize
Hads/Hdes
Ni-Bx
modified
CdS
photocatalyst
(Ni-Bx/CdS).
X-ray
absorption
fine-structure
spectroscopy
theoretical
calculations
reveal
that
increasing
B-atom
amount
cocatalyst
gradually
strengthens
orbital
interaction
between
Ni3d
B2p,
resulting
consecutive
d-band
broadening
controllable
center
on
Ni
active
sites.
above
optimization
allows
for
modulation
dynamics
Ni-Bx/CdS,
ultimately
demonstrating
remarkable
activity
13.4
mmol
g-1
h-1
(AQE
=
56.1
%).
femtosecond
transient
further
confirms
rapid
electron-transfer
Ni-Bx/CdS
photocatalyst.
This
work
provides
insights
into
optimal
design
prospective
catalysts.
A
is
proposed
sites,
H-adsorption/desorption
balance
improving
H2
evolution
efficiency.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Сен. 19, 2024
Abstract
High
entropy
materials
(HEMs)
compositing
of
at
least
five
elements
have
gained
widespread
attention
in
the
field
electrocatalysis
due
to
their
tunable
activities
and
high
stability.
These
intrinsic
properties
can
be
further
highlighted
when
size
HEMs
comes
nanoscale.
In
nanostructured
HEMs,
fascinating
including
large
composition
space,
multi‐element
synergy,
configuration
are
expected
endow
nano‐HEMs
with
excellent
catalytic
activity
stability,
thus
providing
greater
potential
for
design
advanced
electrocatalysts.
this
review,
differentiated
detail
dimensions
common
synthesis
methods
summarized.
Additionally,
from
perspective
complex
nanostructure‐performance
relationship,
applications
systems,
water‐splitting
(hydrogen
evolution
reaction
(HER),
oxygen
(OER)),
hydrogen
oxidation
(HOR),
reduction
(ORR),
carbon
dioxide
(CO
2
RR),
nitrogen
(NRR)
alcohol
(AOR)
discussed.
Finally,
main
challenges
faced
by
underscored.
This
review
is
provide
more
insights
into
understanding
developing
efficient
electrocatalytic
practical
applications.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 28, 2024
Abstract
The
high
entropy
alloy
(HEA)
possesses
distinctive
thermal
stability
and
electronic
characteristics,
which
exhibits
substantial
potential
for
diverse
applications
in
electrocatalytic
reactions.
nanosize
of
HEA
also
has
a
significant
impact
on
its
catalytic
performance.
However,
accurately
controlling
synthesizing
small
nanomaterials
remains
challenge,
especially
the
ultrasmall
nanoparticles.
Herein,
we
firstly
calculate
illustrate
size
structure
as
well
adsorption
energies
crucial
intermediates
involved
typical
processes,
such
hydrogen
evolution
reaction
(HER),
oxygen
reduction
(ORR),
CO
2
electroreduction
(CO
RR)
NO
3
−
(NO
RR).
Under
guidance
theoretical
calculations,
synthesize
range
PtRuPdCoNi
nanoparticles
with
adjustable
sizes
(1.7,
2.3,
3.0,
3.9
nm)
using
one‐step
spatially
confined
approach,
without
any
further
treatment.
Experimentally,
smaller
HEAs
is
more
favorable
HER
ORR
performances,
aligning
predictions.
Specifically,
sized
at
1.7
nm
(HEA‐1.7)
endows
16
mV
overpotential
current
density
10
mA
cm
−2
,
yielding
mass
activity
31.9
A
mg
NM
−1
noble
metal
HER,
significantly
outperforming
commercial
Pt/C
catalyst.
This
strategy
can
be
easily
applicable
to
other
reactions
(e.g.
)
attributed
richness
components
adjustability,
presenting
promising
platform
various
advanced
catalysts.
High-entropy
alloy
(HEA)
nanoparticles
are
rising
as
promising
catalysts
but
face
challenges
in
both
facile
synthesis
and
correlation
of
the
structure
with
properties.
Herein,
utilizing
highly
reductive
carbon-centered
isopropyl
alcohol
radicals
generated
by
UV
irradiation,
we
report
a
simple
yet
robust
wet
chemical
method
to
synthesize
HEA
under
ambient
conditions.
These
isopropanol
verified
electron
paramagnetic
resonance
spectroscopy
impose
very
large
overpotentials
reduce
diverse
metal
ions
into
five
seven
different
elements.
Specially,
PtPdIrRhAuAgCu
on
reduced
electrochemical
graphene
oxide
(rEGO)
support
(PtPdIrRhAuAgCu-rEGO)
demonstrate
superior
activity
for
hydrogen
evolution
reaction
(HER)
across
entire
pH
range,
small
11,
30,
31
mV
deliver
current
density
-10
mA
cm-2
1
M
KOH,
phosphate
buffer
saline,
0.5
H2SO4,
respectively.
The
excellent
HER
performance
PtPdIrRhAuAgCu-rEGO
surpasses
that
commercial
Pt/C
most
contemporary
literature.
Density
functional
theory
calculations
using
random
structures
mimicking
disordering
confirm
its
imply
possible
between
d-band
centers
nearest
atoms
face-centered
cubic
hollow
site.
