Cuδ+ Site-Enhanced Adsorption and Crown Ether-Reconfigured Interfacial D2O Promote Electrocatalytic Dehalogenative Deuteration
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 28, 2025
Electrocatalytic
dehalogenative
deuteration
is
a
sustainable
method
for
precise
deuteration,
whereas
its
Faradaic
efficiency
(FE)
limited
by
high
overpotential
and
severe
D2
evolution
reaction
(DER).
Here,
Cuδ+
site-adjusted
adsorption
crown
ether-reconfigured
interfacial
D2O
are
reported
to
cooperatively
increase
the
FE
of
up
84%
at
−100
mA
cm–2.
sites
strengthen
aryl
iodides,
promoting
mass
transfer
thus
accelerating
kinetics
toward
deuteration.
The
ethers
disrupt
hydration
effect
K·D2O
reconstruct
hydrogen
bond
with
D2O,
lowering
content
electric
double
layer
hindering
interaction
between
cathode,
inhibiting
competitive
DER.
A
linear
relationship
matched
sizes
alkali
metal
cations
demonstrated
universally
increasing
FEs.
This
also
suitable
various
halides
easily
reducible
functional
group
compatibility
improved
FEs
Язык: Английский
Bimetallic effects in the carbon dioxide electroreduction
Chemical Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
This
review
systematically
summarizes
the
latest
advances
in
bimetallic
effects
for
reduction
of
CO
2
to
multi-carbon
products,
discussing
structure–activity
relationships
typical
catalysts
reaction.
Язык: Английский
High‐Entropy Materials: from Bulk to Sub‐nano
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 12, 2025
Abstract
High‐entropy
materials
(HEMs),
characterized
by
their
unique
compositions
involving
multiple
principal
elements
and
inherent
configurational
disorder,
have
emerged
as
a
focal
point
of
material
science
research
since
introduction,
owing
to
exceptional
structural
stability
superior
performance.
The
distinctive
features
HEMs,
including
the
high‐entropy
effect,
lattice
distortion,
sluggish
diffusion,
cocktail
enabled
wide‐ranging
applications
in
fields
such
energy
storage,
catalysis,
electronic
devices,
beyond.
This
review
systematically
documents
evolution
HEMs
synthesis,
from
traditional
melting‐based
methods
for
bulk
production
recent
breakthroughs
addressing
limitations
elemental
immiscibility,
ultimately
enabling
precise
multi‐path
synthesis
nano‐
sub‐nano
materials.
It
comprehensively
examines
controllable
strategies
across
various
dimensional
scales,
principles
composition‐structure
design,
regulation
multidimensional
morphologies,
multifunctional
properties
materials'
multi‐component
characteristics.
Furthermore,
this
work
prospectively
explores
emerging
that
could
drive
future
development
with
particular
emphasis
on
potential
synergies
between
high‐throughput
experimentation,
data‐driven
approaches,
chiral
factors,
entropy‐driven
strategies,
advanced
high‐resolution
characterization
techniques.
Язык: Английский
Density Functional Theory Simulations of Skaergaardite (CuPd) with a Self-Consistent Hubbard U-Correction
Chemistry,
Год журнала:
2025,
Номер
7(2), С. 56 - 56
Опубликована: Апрель 2, 2025
The
electronic
and
phonon
bands
of
Skaergaardite
are
investigated
using
density
functional
theory
(DFT)
as
implemented
in
Quantum
ESPRESSO.
is
a
copper
palladium
mineral
(CuPd)
found
the
Skaergaard
intrusion
with
CsCl-type
(B2)
structure.
Due
to
its
porous
structure,
it
presents
large
surface
area
available
for
interactions,
which
makes
promising
catalyst.
PBE-GGA
Hubbard-like
localized
term
(DFT+U)
combined
ultrasoft
norm-conserving
pseudopotentials,
conventional
approach
dense
Monkhorst–Pack
grid
k-points
12
×
applied.
valence
mainly
constituted
by
3d
orbitals
Cu
4d
Pd
pseudo-gap
can
be
recognized.
With
respect
DFT,
DFT+U
causes
general
downward
shift
band.
acoustic
optical
branches
separated
few
cm−1
gap
at
about
150
show
state
curve
typical
ordered
materials.
These
results
highlight
reliability
studying
bimetallic
systems
scarce
experimental
benchmarks,
offering
insights
into
behavior
potential
applications
material
science
such
reduction
reactions
hydrogen
storage.
Язык: Английский
Promoting CO2 electroreduction to C2H4 product by promoting water molecules activation on MgO/CuO catalyst
Journal of Energy Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 1, 2025
Язык: Английский
Flexible Single‐Atom Cesium Sites on Amorphous MgO Nano‐Cushions for Enhanced CO2‐Involved Multi‐Step Reactions
Small,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 24, 2025
Abstract
Single
atomic
sites
(SAs)
face
challenges
in
catalyzing
complex
chemical
processes
involving
multiple
intermediates
due
to
rigid
coordination
environments,
steric
hindrances,
and
limited
activation
behaviors.
Herein,
an
alloying‐mediated
element
repartition
method
is
developed
synthesize
flexible
cesium
single‐atom
catalysts,
anchoring
Cs
single
on
precisely
controlled
amorphous‐MgO/crystalline
NbC
hetero‐phase
nano‐supports.
The
amorphousMgO(a‐MgO)
equipped
1
‐a‐MgO/NbC
achieves
91%
yield
the
cyclization
of
CO
2
with
2‐aminobenzonitrile
within
a
gas–liquid–solid
triphasic
system,
outperforming
its
counterpart
fabricated
crystalline
MgO,
‐c‐MgO/NbC
catalyst
(only
23%).
shows
excellent
tolerance
various
functional
groups
sustainable
catalysis,
especially
removing
traditional
requirement
for
high‐pressure
conditions
additives.
Operando
spectroscopic
characterizations
theoretical
calculations
demonstrate
that
sandwich‐structural
enhances
consecutive
through
vertically
adsorbed
configurations
during
C‐N
coupling
N‐heterocyclic
ring
formation.
SAs
supported
by
a‐MgO
nano‐cushions
allow
adaptability
dynamic
transformations
via
tensile
Cs‐O
compressive
Mg─O
bonds,
ultimately
reducing
energy
barriers
critical
rearrangement
isomerization
steps.
This
study
provides
valuable
insights
into
designing
SACs
overcome
limitations
support
interfaces,
thereby
enhancing
performance
toward
multi‐intermediate
conversion
heterogeneous
catalytic
transformations.
Язык: Английский