Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: May 15, 2025
Direct
methane
conversion
to
value-added
chemicals
under
mild
conditions
presents
a
promising
route
toward
net-zero
carbon
emissions.
However,
this
process
encounters
significant
challenges
in
efficiently
activating
inert
C-H
bonds
and
preventing
excessive
oxidation
CO2.
Herein,
we
propose
coverage-dependent
strategy
that
leverages
the
correlation
between
coverage
C-C
coupling
selectivity,
thereby
enhancing
both
activity
selectivity.
By
tuning
Lewis
acidity
of
well-defined
atomic
3d
transition
metal-modified
ceria,
from
weak
moderate,
it
boosts
adsorption
capacity
promotes
its
dissociative
activation.
Additionally,
incorporating
nickel
cocatalyst
improves
charge
separation
through
efficient
hole
extraction.
The
optimal
noble-metal-free
catalyst
(Ni1-CeO2)
delivers
exceptional
room-temperature
performance,
achieving
production
rate
243
μmol·g-1·h-1
with
approximately
90%
ethane
selectivity
over
an
ultralong
test
(>350
h),
outperforming
previously
reported
catalysts.
This
work
provides
new
insights
into
regulation
via
optimization
chemisorbed
paves
way
for
design
advanced
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(10), P. 7707 - 7716
Published: May 2, 2024
Nonthermal
plasma
(NTP)
offers
the
potential
for
converting
CH4
with
CO2
into
liquid
products
under
mild
conditions,
but
controlling
selectivity
and
manipulating
intermediate
species
remain
significant
challenges.
Here,
we
demonstrate
effectiveness
of
Cu/UiO-66-NH2
catalyst
in
promising
conversion
oxygenates
within
a
dielectric
barrier
discharge
NTP
reactor
ambient
conditions.
The
10%
achieved
an
impressive
53.4%
overall
selectivity,
C2+
accounting
∼60.8%
total
products.
In
situ
plasma-coupled
Fourier-transform
infrared
spectroscopy
(FTIR)
suggests
that
Cu
facilitates
cleavage
surface
adsorbed
COOH
(*COOH),
generating
*CO
enabling
its
migration
to
particles.
This
surface-bound
then
undergoes
C–C
coupling
hydrogenation,
leading
ethanol
production.
Further
analysis
using
CO
diffuse
reflection
FTIR
1H
nuclear
magnetic
resonance
indicates
generated
is
more
effective
than
gas-phase
(g)
promoting
formation.
work
provides
valuable
mechanistic
insights
production
during
plasma-catalytic
oxidation
These
findings
hold
broader
implications
rational
design
efficient
catalysts
this
reaction,
paving
way
advancements
sustainable
fuel
chemical
ACS Applied Materials & Interfaces,
Journal Year:
2025,
Volume and Issue:
17(9), P. 14119 - 14128
Published: Feb. 24, 2025
Photocatalytic
oxidative
dehydrogenation
of
ethane
offers
a
promising
approach
for
producing
ethylene
under
mild
conditions.
However,
achieving
high
yields
and
selectivity
is
challenging
due
to
the
C-H
bond
activation
barrier
in
tendency
overoxidation
CO2.
In
this
study,
we
demonstrate
that
TiO2
with
highly
dispersed
AuPd
nanoparticles
serves
as
an
efficient
selective
photocatalyst
O2
flow
reactor.
The
optimized
Au0.33Pd0.67/TiO2
achieves
up
20.3
mmol
g-1
h-1
91.5%
selectivity,
resulting
5.9%
apparent
quantum
efficiency
at
365
nm.
Detailed
characterizations
reveal
Au0.33Pd0.67
cocatalyst
plays
crucial
role
facilitating
photocarrier
separation
regulating
formation
active
oxygen
species.
effectively
activates
lattice
TiO2,
which
localized
oxidant
promote
dissociation
through
photoassisted
Mars-van
Krevelen
mechanism.
Additionally,
facilitates
dioxygen
reduction
ensures
rapid
replenishment
lattice,
thereby
yield
formation.
This
work
provides
valuable
insights
designing
composite
photocatalysts
dehydrogenation.
Small,
Journal Year:
2024,
Volume and Issue:
20(29)
Published: Feb. 16, 2024
Direct
photocatalytic
methane
oxidation
into
value-added
products
provides
a
promising
strategy
for
utilization.
However,
the
inefficient
generation
of
reactive
oxygen
species
(ROS)
partly
limits
activation
CH
Advanced Science,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 21, 2025
Partial
oxidation
of
methane
(POM)
is
achieved
by
forming
air-methane
microbubbles
in
saltwater
to
which
an
alternating
electric
field
applied
using
a
copper
oxide
foam
electrode.
The
solubility
increased
putting
it
contact
with
water
containing
dissolved
KCl
or
NaCl
(3%).
Being
fully
dispersed
as
(20-40
µm
diameter),
reacts
more
hydroxyl
radicals
(OH·)
at
the
gas-water
interface.
voltage
(100
mV)
generates
two
synergistic
POM
processes
dominated
Cl-
→
Cl·
+
e-
and
O2
-•
under
positive
negative
potentials,
respectively.
By
tuning
frequency
amplitude,
extent
path
process
can
be
precisely
controlled
so
that
than
90%
methanol
selectively
formed
compared
byproducts,
dichloromethane,
acetic
acid.
conversion
yield
estimated
57%
rate
approximately
887
µM
h-1.
This
method
appears
have
potential
for
removing
from
air
seawater
converting
higher-concentration
sources
into
value-added
methanol.
