The
construction
of
highly
efficient
and
self-supported
electrocatalysts
with
abundant
active
sites
for
pH-universal
hydrogen
evolution
reaction
(HER)
alkaline
water
splitting
is
significantly
challenging.
Herein,
Co
MoC
nanoparticles
embedded
in
nitrogen-doped
carbon
nanofibers
(Co-MoC/NCNFs)
which
display
a
bamboo-like
morphology
are
prepared
by
electrospinning
followed
the
carbonization
method.
electrospun
possesses
an
ultrasmall
size
(≈5
nm)
can
provide
more
during
electrocatalysis,
while
introduction
greatly
optimizes
electronic
structure
MoC.
Both
endow
Co-MoC/NCNFs
superior
HER
performances
over
wide
pH
range,
low
overpotentials
86,
116,
145
mV
to
achieve
current
density
10
mA
cm
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Ноя. 15, 2023
Regulating
electron
transport
rate
and
ion
concentrations
in
the
local
microenvironment
of
active
site
can
overcome
slow
kinetics
unfavorable
thermodynamics
CO2
electroreduction.
However,
simultaneous
optimization
both
is
hindered
by
synthetic
constraints
poor
mechanistic
understanding.
Here
we
leverage
laser-assisted
manufacturing
for
synthesizing
CuxO
bipyramids
with
controlled
tip
angles
abundant
nanograins,
elucidate
mechanism
relationship
between
transport/ion
electrocatalytic
performance.
Potassium/OH-
adsorption
tests
finite
element
simulations
corroborate
contributions
from
strong
electric
field
at
sharp
tip.
In
situ
Fourier
transform
infrared
spectrometry
differential
electrochemical
mass
unveil
dynamic
evolution
critical
*CO/*OCCOH
intermediates
product
profiles,
complemented
theoretical
calculations
that
thermodynamic
improved
coupling
Cu+/Cu2+
interfaces.
Through
modulating
concentrations,
achieve
high
Faradaic
efficiency
81%
~900
mA
cm-2
C2+
products
via
CO2RR.
Similar
enhancement
also
observed
nitrate
reduction
reaction
(NITRR),
achieving
81.83
mg
h-1
ammonia
yield
per
milligram
catalyst.
Coupling
CO2RR
NITRR
systems
demonstrates
potential
valorizing
flue
gases
wastes,
which
suggests
a
practical
approach
carbon-nitrogen
cycling.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июль 17, 2024
Abstract
Electrocatalytic
alkynes
semi-hydrogenation
to
produce
alkenes
with
high
yield
and
Faradaic
efficiency
remains
technically
challenging
because
of
kinetically
favorable
hydrogen
evolution
reaction
over-hydrogenation.
Here,
we
propose
a
hierarchically
nanoporous
Cu
50
Au
alloy
improve
electrocatalytic
performance
toward
alkynes.
Using
Operando
X-ray
absorption
spectroscopy
density
functional
theory
calculations,
find
that
modulate
the
electronic
structure
Cu,
which
could
intrinsically
inhibit
combination
H*
form
H
2
weaken
alkene
adsorption,
thus
promoting
alkyne
hampering
Finite
element
method
simulations
experimental
results
unveil
catalysts
induce
local
microenvironment
abundant
K
+
cations
by
enhancing
electric
field
within
nanopore,
accelerating
water
electrolysis
more
H*,
thereby
conversion
As
result,
electrocatalyst
achieves
highly
efficient
94%
conversion,
100%
selectivity,
92%
over
wide
potential
window.
This
work
provides
general
guidance
rational
design
for
high-performance
transfer
catalysts.
Journal of The Electrochemical Society,
Год журнала:
2024,
Номер
171(5), С. 056509 - 056509
Опубликована: Май 1, 2024
The
quest
for
economical
and
sustainable
electrocatalysts
to
facilitate
the
hydrogen
evolution
reaction
(HER)
is
paramount
in
addressing
pressing
challenges
associated
with
carbon
dioxide
emissions.
Molybdenum
carbide-based
nanomaterials
have
emerged
as
highly
promising
HER
due
their
Pt-like
catalytic
proficiency,
exceptional
stability,
versatility
of
crystal
phases.
Within
this
comprehensive
review,
we
explore
diverse
methodologies
synthesizing
molybdenum
carbides,
including
solid-gas,
solid-solid,
solid-liquid
phase
reactions.
In
addition,
a
thorough
elucidation
generation
process
through
water
electrolysis
provided.
Furthermore,
spectrum
innovative
strategies
aimed
at
augmenting
performance
carbides
milieu
introduced,
encompassing
cutting-edge
techniques
such
phase-transition
engineering,
construction
heterostructures,
hetero-atom
doping,
integration
hybrid
structures
materials,
defect
meticulous
surface
modification.
review
culminates
by
underscoring
current
prospects
advancement
production,
dedicated
focus
on
catalysts.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 3, 2025
Electrochemical
conversion
has
been
regarded
as
an
ideal
technology
for
achieving
clean
and
sustainable
energy,
showing
significant
promise
in
addressing
the
increasingly
serious
energy
crisis
environmental
pollution.
Ru-containing
electrocatalysts
(RUCE)
outperform
other
precious
metals
due
to
elevated
intrinsic
activity
superior
cost-effectiveness,
developing
into
a
promising
candidate
electrochemical
reactions.
A
challenge
field
of
catalyst
discovery
lies
its
heavy
reliance
on
empirical
methods,
rather
than
approaches
that
are
rooted
rational
design
principles.
This
review
first
concentrates
catalytically
active
sites
critical
factors
governing
catalytic
performance
durability.
Then,
comprehensive
summary
multifunctional
modification
strategies
ranging
from
nanoscale
atomic
scale
is
explored
control
structure
improve
performance.
By
unveiling
roles
each
component
modified
RUCE
at
level,
their
identified
discussed
establish
structure-performance
relationship
catalysts.
Finally,
challenges
perspectives
Ru-based
materials
hydrogen,
oxygen,
nitrogen
reactions
presented
inspire
further
efforts
toward
understanding
meet
ever-growing
demand
future.
