Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 26, 2024
Abstract
Efficiently
regulating
reaction
pathways
for
photoreduction
CO
2
to
achieve
required
products
is
enormously
strenuous.
The
design
of
active
sites
adsorption,
activation,
and
tuning
pivotal
address
this
grand
challenge.
Herein,
highly
selective
are
developed
HCOOH
based
on
asymmetrically
coupling
different
ratios
Ni
Co
loaded
crystalline
carbon
nitride
(CCN)
by
an
alloying
synthesis
strategy,
which
confirmed
high‐resolution
transmission
electron
microscopy
(HRTEM)
imaging,
X‐ray
diffraction
(XRD)
patterns,
photoelectron
spectroscopy
(XPS)
spectra.
In
situ
Fourier
transform
infrared
spectra
suggest
that
the
key
intermediate
*OCHO
pathway
prefers
form
sites,
while
*COOH
tends
generate
characteristic
peaks
intensity
two
intermediates
stronger
with
synergistic
effects
NiCo
bimetallic,
further
verified
theory
calculations.
Accordingly,
a
selectivity
98.5%
(194.5
µmol
g⁻
1
h⁻
)
or
85.4%
(144.8
g
−1
h
can
be
achieved
optimized
x
y
alloy,
under
sacrificial
agent‐free
conditions.
Hydrogen
spillover-based
binary
(HSBB)
system
has
attracted
significant
attention
in
alkaline
hydrogen
evolution
reaction
(HER).
Accelerating
spillover
the
HSBB
is
crucial
for
HER
activity.
Herein,
a
highly
efficient
developed
by
anchoring
nano-Ru
on
oxygen
vacancy
(Vo)
rich
amorphous/crystal
ZrO
Angewandte Chemie International Edition,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 31, 2025
Abstract
Carbon
black
has
been
extensively
employed
as
the
support
for
noble
metal
catalysts
electrocatalysis
applications.
However,
nearly
catalytic
inertness
and
weak
interaction
with
species
of
carbon
are
two
major
obstacles
that
hinder
further
improvement
performance.
Herein,
we
report
a
surface
functionalization
strategy
by
decorating
transition
oxide
clusters
on
commercial
to
offer
specific
activity
enhanced
species.
In
case
NiO
x
cluster‐decorated
black,
strongly
coupled
cluster‐cluster
heterostructure
consisting
Pt
(Pt−NiO
/C)
is
formed
delivers
greatly
alkaline
hydrogen
evolution
kinetics.
The
can
not
only
accelerate
process
co‐catalyst,
but
also
optimize
adsorption
H
intermediates
stabilize
clusters.
Notably,
anion
exchange
membrane
water
electrolyzer
Pt−NiO
/C
cathode
catalyst
(with
loading
50
μ
g
cm
−2
)
most
competitive
electrochemical
performance
reported
date,
requiring
1.90
V
reach
current
density
2
A
.
results
demonstrate
significance
carbonaceous
supports
toward
development
advanced
electrocatalysts.
Angewandte Chemie,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 31, 2025
Abstract
Carbon
black
has
been
extensively
employed
as
the
support
for
noble
metal
catalysts
electrocatalysis
applications.
However,
nearly
catalytic
inertness
and
weak
interaction
with
species
of
carbon
are
two
major
obstacles
that
hinder
further
improvement
performance.
Herein,
we
report
a
surface
functionalization
strategy
by
decorating
transition
oxide
clusters
on
commercial
to
offer
specific
activity
enhanced
species.
In
case
NiO
x
cluster‐decorated
black,
strongly
coupled
cluster‐cluster
heterostructure
consisting
Pt
(Pt−NiO
/C)
is
formed
delivers
greatly
alkaline
hydrogen
evolution
kinetics.
The
can
not
only
accelerate
process
co‐catalyst,
but
also
optimize
adsorption
H
intermediates
stabilize
clusters.
Notably,
anion
exchange
membrane
water
electrolyzer
Pt−NiO
/C
cathode
catalyst
(with
loading
50
μ
g
cm
−2
)
most
competitive
electrochemical
performance
reported
date,
requiring
1.90
V
reach
current
density
2
A
.
results
demonstrate
significance
carbonaceous
supports
toward
development
advanced
electrocatalysts.
Abstract
The
design
of
efficient
alkaline
hydrogen
evolution
reaction
(HER)
electrocatalysts
is
crucial
for
the
development
green
production.
In
this
work,
we
report
modulation
HER
activity
Ru
nanoparticles
by
functionalization
using
para‐substituted
phenylacetylenes
(R
=
Cl,
H,
C
2
H
5
,
and
OCH
3
),
which
have
different
electron
donating/withdrawing
capabilities.
A
close
correlation
between
Hammett
substituent
constant
functionalized
revealed,
underlying
mechanism
investigated.
Guided
such
correlation,
4‐ethylphenylacetylene‐modified
(Ru─EPA)
with
a
low
overpotential
17.7
mV
at
current
density
10
mA
cm
−2
in
solution
developed.
mechanistic
understanding
gained
work
will
provide
important
guidelines
future
high‐performance
nanostructured
electrocatalyst.
Abstract
Ruthenium
(Ru)
–based
catalysts
have
been
considered
a
promising
candidate
for
efficient
sustainable
hydrogen
and
chlor‐alkali
co‐production.
Theoretical
calculations
disclosed
that
the
hollow
sites
on
Ru
surface
strong
adsorption
energies
of
H
Cl
species,
which
inevitably
leads
to
poor
activity
cathodic
evolution
reaction
(HER)
anodic
chlorine
(CER),
respectively.
Furthermore,
it
confirmed
anchoring
Lewis
acid
oxide
nanoparticles
such
as
MgO
can
induce
formation
onion‐like
charge
distribution
atoms
around
nanoparticles,
thereby
exposing
Ru‐bridge
at
interface
excellent
accelerate
both
HER
CER.
Under
guidance
theoretical
calculations,
novel
dispersed
(MgO
x
‐Ru)
electrocatalyst
is
successfully
prepared.
In
strongly
alkaline
saline
media,
‐Ru
recorded
CER
electrocatalytic
with
very
low
overpotential
19
mV
74
current
density
10
mA
cm
−2
,
More
stirringly,
electrochemical
test
electrodes
under
simulated
electrolysis
conditions
demonstrated
superior
performance
industrial
commercial
20
wt%
Pt/C
dimensionally
stable
anode
(DSA).
ACS Applied Energy Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 27, 2025
Dual-atom
catalysts
(DACs)
have
gained
great
attention
as
highly
efficient
materials
for
the
hydrogen
evolution
reaction
(HER)
due
to
their
synergistic
dual-site
effects
and
high
atomic
utilization.
This
review
explores
how
microenvironmental
regulation,
including
electronic
structure
optimization
coordination
design,
influences
DAC
performance.
Both
homonuclear
heteronuclear
types
of
DACs
are
analyzed
in
detail
terms
site
interactions
structural
configurations.
Moreover,
recent
advancements
HER
applications
under
various
pH
conditions
discussed,
highlighting
enhanced
catalytic
activity
mechanism.
Despite
challenges
synthesis
characterization,
represent
a
promising
frontier
developing
offer
guidance
future
research
scalable
applications.
Hydrogen,
as
an
environmentally
sustainable
energy
carrier,
offers
substantial
potential
for
addressing
the
global
crisis.
The
development
of
highly
efficient
catalysts
to
accelerate
hydrogen
evolution
reaction
(HER)
is
critical
realization
electrochemical
production
via
water
splitting.
Herein,
a
novel
heterogeneous
catalyst
consisting
PtNi
nanoalloys
with
Pt-enriched
surfaces
obtained,
which
are
uniformly
distributed
within
nitrogen-doped
hollow
carbon
nanoshells
derived
from
complex
Ni-EDTA
(ethylene
diamine
tetraacetate).
Remarkably,
fabricated
NE-PtNiNC
demonstrates
exceptional
HER
performance,
exhibiting
ultra-low
overpotential
3
mV
at
10
mA
cm-2
and
6.8-fold
higher
mass
activity
compared
commercial
Pt/C
catalyst,
positioning
it
one
most
advanced
date.
Additionally,
shows
outstanding
stability
over
200
h
exhibits
promising
practical
deployment
in
two-electrode
electrolysis
systems.
Theoretical
analyses
further
reveal
that
Pt-skin@PtNi
structure,
its
lowest
d-band
center,
fosters
more
pronounced
overlap
5d
electron
cloud
surface
Pt
sites.
This
interaction
results
increased
density
on
skin,
facilitating
dissociation
significantly
enhancing
intrinsic
durability.
The
electrochemical
synthesis
of
hydrogen
peroxide
(H2O2)
via
the
two-electron
oxygen
reduction
reaction
(2e-
ORR)
is
a
promising
alternative
to
conventional
anthraquinone
method.
However,
due
local
alkalinization
near
catalyst
surface,
restricted
replenishment
and
insufficient
activated
water
molecule
supply
limit
formation
key
*OOH
intermediate.
Herein,
pulsed
electrocatalysis
approach
based
on
structurally
optimized
S/N/O
tridoped
hollow
carbon
bowl
has
been
proposed
overcome
this
challenge.
In
an
H-type
electrolytic
cell,
method
achieves
superior
H2O2
yield
rate
55.6
mg
h-1
mgcat.-1,
approximately
1.6
times
higher
than
potentiostatic
(34.2
mgcat.-1),
while
maintaining
Faradaic
efficiency
above
94.6%.
situ
characterizations,
finite
element
simulations,
density
functional
theory
analyses
unveil
that
application
potentials
mitigates
OH-
concentration,
enhances
activation
proton
generation,
facilitates
production
within
bowl-like
structure.
These
effects
synergistically
accelerate
kinetics
intermediate
by
efficient
generation
*O2
*H2O
intermediates,
leading
yields.
This
work
develops
strategy
tune
catalytic
environments
for
diverse
applications.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 24, 2025
The
electrocatalytic
conversion
of
carbon
dioxide
(CO2)
to
ethylene
(C2H4)
holds
great
promise
for
sustainable
chemical
synthesis,
yet
achieving
industrially
relevant
production
rates
remains
a
significant
challenge.
Through
computational
screening,
we
have
identified
praseodymium
(Pr)
single-atom
alloy
embedded
in
copper
(Cu)
catalyst
(Pr@Cu)
that
exhibits
superior
CO2
activation
and
remarkably
low
energy
barrier
asymmetric
*CO-*CHO
coupling,
primarily
by
facilitating
the
*CHO
intermediate
formation.
Our
optimized
catalyst,
Pr@Cu-2
(6
wt
%
Pr),
achieves
C2H4
Faradaic
efficiency
(FE)
64.2%
at
-1.6
V
versus
reversible
hydrogen
electrode
(RHE)
under
high
current
density
1200
mA
cm-2
reduction
reaction
(CO2RR).
Furthermore,
when
integrated
into
100
cm2
membrane
assembly
(MEA)
electrolyzer,
demonstrates
robust
performance,
maintaining
continuous
rate
21.3
mL
min-1
20
A
over
200
h.
This
work
provides
fundamental
insights
role
Pr
alloys
CO2RR
highlights
their
potential
scalable
electrosynthesis.
