PNAS Nexus,
Journal Year:
2024,
Volume and Issue:
4(1)
Published: Dec. 23, 2024
Modulating
the
electronic
structure
of
noble
metals
via
metal-support
interaction
(EMSI)
has
been
proven
effectively
for
facilitating
molecular
oxygen
activation
and
catalytic
oxidation
reactions.
Nevertheless,
investigation
fundamental
mechanisms
underlying
activity
enhancement
primarily
focused
on
metal
oxides
as
supports,
especially
in
degradation
volatile
organic
compounds.
In
this
study,
a
novel
Pt
catalyst
supported
nitrogen-doped
carbon
encapsulating
FeNi
alloy,
featuring
ultrafine
nanoparticles,
was
synthesized.
This
demonstrated
exceptional
(92%),
recyclability,
water
tolerance
deep
formaldehyde
at
room
temperature.
Structural
analyses
theoretical
calculations
revealed
directional
electron
transfer
from
alloy
to
Pt,
even
there
is
no
direct
contact
between
them.
penetration
effect,
mediated
by
carbon,
conferred
electron-rich
properties
leading
elongating
O-O
bond
length
(1.405
Å).
Consequently,
efficient
removal
achieved
with
an
ultra-low
loading.
offers
perspective
modulating
engineering
unique
EMSI
effect
nonoxide
support
active
species,
thereby
enabling
air
purification.
Advanced Science,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 18, 2025
Abstract
Engineering
stable
and
efficient
noble
metal
ensembles
with
multi‐type
active
sites
while
understanding
the
role
of
each
site
at
atomic
level
remains
a
significant
challenge
in
heterogeneous
catalysis.
Herein,
sub‐nanometric
Pt
ensemble
catalyst
diverse
array
is
constructed
via
dual‐confinement
strategy,
which
exhibits
superior
activity
durability
minimal
loading
(0.13
wt.%).
Simultaneously,
roles
different
scale
are
determined
through
situ
characterization
methods
density
functional
theory
(DFT)
calculations.
Specifically,
top
predominantly
serve
as
pivotal
centers
for
O═O
bond
activation,
whereas
Pt−O−Si
interfacial
primarily
govern
activation
H─OH
C─H
bonds.
The
reactive
oxygen
species
(O
2
−
,
O
2−
−OH)
generated
from
H
synergistically
enhance
formaldehyde
(HCHO)
oxidation
shorten
reaction
pathway.
This
study
sheds
light
on
better
rational
design
precise
synthesis
multi‐site
or
discerning
distinct
contributions
various
catalytic
sites.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 4, 2024
Abstract
Transition
metal
oxide
shows
great
potential
in
catalytic
formaldehyde
(HCHO)
pollution
degradation
at
room
temperature,
while
it
is
still
difficult
to
overcome
the
efficiency
attenuation
caused
by
limited
reactive
oxygen
species
(ROS)
generation
during
catalysis.
An
elastic
spongy
catalyst
with
Cu‐modified
polydimethylsiloxane
(PDMS)
organic
skeleton
(PDMS@Cu)
supported
hydroxy‐modified
MnO
x
(MnO
‐OH)
prepared
hereon,
named
PDMS@Cu/MnO
‐OH.
Deformation
of
carrier
causes
contact‐separation
friction
between
Cu
and
PDMS
generate
electrostatically
induced
nonuniform
charges,
which
provide
enriched
electrons
transient
electric
field
(EF)
enhance
ROS
HCHO
oxidation.
In
dynamic
tests
(∼12
ppm
weight
hourly
space
velocity
(WHSV)
120
000
mL
g
cat.
−1
h),
‐OH
achieved
∼100%
removal
efficiency,
an
HCHO‐to‐CO
2
conversion
82.47%,
32.47%
higher
than
that
without
non‐uniform
electrostatic
sustained
complete
real‐time
within
24
h
temperature.
Coupled
Density
Functional
Theory
(DFT)
calculations
COMSOL
physics
simulations,
pathway
surface
charges
EF
enhancing
oxidation
unveiled,
offering
a
theoretical
foundation
novel
strategy
for
efficient
long‐term
indoor
pollutant
under
action
sustainably
charges.