Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 7, 2025
Abstract
Seawater
electrolysis
is
pivotal
for
sustainable
hydrogen
production,
yet
chloride‐induced
catalyst
corrosion
severely
hinders
its
efficiency.
Here,
a
(Mo,
Co)P
x
electrocatalyst
via
two‐step
hydrothermal‐phosphorization
strategy
engineered,
enabling
in
situ
formation
of
dynamic
dual‐anion
(MoO
4
2
⁻/PO
3
⁻)
Cl
−
‐rejection
interface.
This
tailored
interface
effectively
blocks
adsorption
while
preserving
hydroxyl
accessibility,
significantly
enhancing
resistance
alkaline
seawater.
The
optimized
delivers
exceptional
oxygen
evolution
reaction
performance
seawater
electrolysis,
achieving
ultralow
overpotentials
213
and
360
mV
to
reach
current
densities
10
1000
mA
cm
−2
,
respectively.
Remarkably,
the
with
an
situ‐generated
rejection
layer
demonstrates
durability,
exhibiting
only
20mV
degradation
during
480‐h
stability
test
under
high‐current
conditions.
In
Raman
spectroscopy,
attenuated
total
reflectance
surface‐enhanced
infrared
absorption
density
functional
theory
calculations
demonstrate
that
not
enhances
but
also
promotes
rapid
surface
reconstruction
Co
species
interfacial
water
adsorption,
thereby
suppressing
competitive
chlorine
reactions.
work
provides
rational
designing
durable
electrocatalysts
situ‐engineered
anion‐rejection
interfaces,
advancing
efficient
electrolysis.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 12, 2025
The
bifunctional
mechanism,
involving
multiactive
compositions
to
simultaneously
dissociate
water
molecules
and
optimize
intermediate
adsorption,
has
been
widely
used
in
the
design
of
catalysts
boost
electrolysis
for
sustainable
hydrogen
energy
production
but
remains
debatable
due
difficulties
accurately
identifying
reaction
process.
Here,
we
proposed
concept
well-defined
Lewis
pairs
single-atom
catalysts,
with
a
unique
acid-base
nature,
comprehensively
understand
exact
role
an
alkaline
evolution
reaction.
By
facilely
adjusting
active
moieties,
induced
synergistic
effect
between
(M-P/S/Cr
pairs,
M
=
Ru,
Ir,
Pt)
can
significantly
facilitate
cleavage
H-OH
bond
accelerate
removal
intermediates,
thereby
switching
rate-determining
step
from
Volmer
Heyrovsky
step.
Moreover,
representative
Ru-P
deliver
impressive
266
h
durability
at
high
industrial
current
density
2
A
cm-2
without
activity
decay
anion-exchange
membrane
electrolysis,
be
extended
modify
commercial
noble-metal-based
performance
enhancement.
This
work
not
only
sheds
light
on
important
mechanism
scale
also
offers
universal
descriptor
rational
advanced
catalysts.
Advanced Sustainable Systems,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 5, 2025
Abstract
As
a
pivotal
bio‐based
building
block,
2,5‐furandicarboxylic
acid
(FDCA)
holds
immense
and
broad
application
potential
in
the
chemistry
industry.
Its
polymeric
derivative,
polyethylene
furandicarboxylate
(PEF),
emerges
as
an
appealing
alternative
to
conventional
petroleum‐based
terephthalate
(PET).
The
electrochemical
route
for
oxidizing
5‐hydroxymethylfurfural
(HMF)
into
FDCA
presents
significant
advantages
over
thermochemical
processes,
without
requirements
of
high
temperature,
pressure,
chemical
oxidants,
precious
metal
catalysts,
featuring
higher
energy
efficiency.
Furthermore,
electrosynthesis
at
anode
can
be
synergistically
integrated
with
selective
reduction
reactions
cathode,
enabling
simultaneous
production
two
desirable
value‐added
products
further
enhancing
overall
utilization
This
work
reviews
advancements
electrocatalytic
HMF
(EHTF),
encompassing
catalyst
design,
reaction
mechanisms,
coupling
strategies,
reactor
configurations.
It
also
indicates
challenges
opportunities
EHTF
provides
insights
future
development
directions.
Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 4, 2025
Electrocatalysts
can
efficiently
convert
earth-abundant
simple
molecules
into
high-value-added
products.
In
this
context,
heterostructures,
which
are
largely
determined
by
the
interface,
have
emerged
as
a
pivotal
architecture
for
enhancing
activity
of
electrocatalysts.
review,
atomistic
understanding
heterostructured
electrocatalysts
is
considered,
focusing
on
reaction
kinetic
rate
and
electron
configuration,
gained
from
both
empirical
studies
theoretical
models.
We
start
fundamentals
microkinetic
model,
adsorption
energy
theory,
electric
double
layer
model.
The
importance
heterostructures
to
accelerate
electrochemical
processes
via
modulating
configuration
interfacial
reactive
microenvironment
highlighted,
considering
rectification,
space
charge
region,
built-in
field,
synergistic
interactions,
lattice
strain,
geometric
effect.
conclude
review
summarizing
challenges
perspectives
in
field
electrocatalysts,
such
determination
transition
state
energy,
their
dynamic
evolution,
refinement
approaches,
use
machine
learning.
Proceedings of the National Academy of Sciences,
Год журнала:
2025,
Номер
122(8)
Опубликована: Фев. 20, 2025
Electrocatalytic
reduction
(ECR)
of
furfural
represents
a
sustainable
route
for
biomass
valorization.
Unfortunately,
traditional
Cu-catalyzed
ECR
suffers
from
diversified
product
distribution
and
industrial-incompatible
production
rates,
mainly
caused
by
the
intricate
mechanism-performance
relationship.
Here,
we
manipulate
hydrogenation
pathways
on
Cu
introducing
ceria
as
an
auxiliary
component,
which
enables
mechanism
switching
proton-coupled
electron
transfer
to
electrochemical
hydrogen-atom
(HAT)
thus
high-speed
furfural-to-furfuryl
alcohol
electroconversion.
Theoretical
kinetic
analyses
show
that
oxygen-vacancy-rich
delivers
efficient
formation-diffusion-hydrogenation
chain
H*
diminishing
adsorption.
Spectroscopic
characterizations
indicate
Cu/ceria
interfacial
perimeter
enriches
local
furfural,
synergistically
lowering
barrier
rate-determining
HAT
step
across
perimeter.
Our
catalyst
realizes
high-rate
HAT-dominated
electrosynthesis
single-product
furfuryl
alcohol,
achieving
high
rate
19.1
±
0.4
mol
h-1
m-2
Faradaic
efficiency
97
1%
at
economically
viable
partial
current
density
over
0.1
A
cm-2.
results
demonstrate
highly
biofeedstock
valorization
with
enhanced
techno-economic
feasibility.
Nano Letters,
Год журнала:
2025,
Номер
25(9), С. 3383 - 3390
Опубликована: Фев. 19, 2025
In
order
to
study
the
catalytic
behavior
of
a
metastable-phase
catalyst
in
electrocatalytic
hydrogenation,
we
report
new
noble-metal-free
core–shell
with
metastable
hexagonal
closest
packed
(hcp)
phase
Ni
as
shell
and
face-centered-cubic
(fcc)
Cu
core
(Cu@hcp
NPs)
for
hydrogenation
nitrobenzene
(Ph-NO2)
aniline
(Ph-NH2).
Using
H2O
hydrogen
source,
it
achieves
up
99.63%
Ph-NO2
conversion
∼100%
Ph-NH2
selectivity,
an
improved
activity
turnover
frequency
(TOF:
6640
h–1),
much
higher
than
those
hcp
NPs
(5183.7
h–1)
commercial
Pt/C
(3537.6
h–1).
It
can
also
deliver
variety
aminoarenes
outstanding
selectivity
excellent
functional
group
compatibility
several
groups.
Mechanistic
studies
have
shown
that
introduction
enhances
Ni's
ability
dissociate
water
situ
produce
H*
improves
rate,
resulting
rapid
final
product
Ph-NH2.
