Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 28, 2025
Abstract
CH
3
OH
is
the
most
desired
product
of
photocatalytic
4
conversion.
The
prominent
metal‐decorated
photocatalyst
challenging
in
both
high
yield
and
selectivity
for
products
due
to
over‐oxidation
by
•OH
mechanism.
Here,
interstitial
Zn
fabricated
into
i
O
induce
formation
atom
island
rapid
single
electron
reduction
2
•OOH
instead
selective
combination
with
methyl
OOH.
AuPd
alloy
simultaneously
decorated
on
surface
tuning
OOH
adsorption
OH.
synergy
achieve
a
tandem
reaction
pathway
(CH
→CH
OOH→CH
OH)
an
unprecedented
2444
mmol
g
−1
h
(or
8800
µmol
cat
)
98.3%
selectivity,
which
bypasses
mechanism
An
apparent
quantum
efficiency
18.53%
at
370
nm
conversion
are
super
reported
systems.
Thus,
this
work
provides
new
strategy
synergetic
metal
photocatalysts
through
mediate
oxidation
ACS Nano,
Год журнала:
2023,
Номер
17(20), С. 20560 - 20569
Опубликована: Окт. 4, 2023
Inefficient
charge
separation
and
slow
interfacial
reaction
dynamics
significantly
hamper
the
efficiency
of
photocatalytic
CO2
reduction.
Herein,
a
facile
EDC/NHS-assisted
linking
strategy
was
developed
to
enhance
in
heterojunction
photocatalysts.
Using
this
approach,
we
successfully
synthesized
amide-bonded
carbon
quantum
dot-g-C3N4
(CQD-CN)
The
formation
amide
covalent
bonds
between
CN
CQDs
CN-CQD
facilitates
efficient
carrier
migration,
adsorption,
activation.
Exploiting
these
advantages,
photocatalysts
exhibit
high
selectivity
with
CO
CH4
evolution
rates
79.2
2.7
μmol
g-1
h-1,
respectively.
These
are
about
1.7
3.6
times
higher
than
those
CN@CQD
bulk
CN,
Importantly,
demonstrate
exceptional
stability,
even
after
12
h
continuous
testing.
presence
COOH*
signal
is
identified
as
crucial
intermediate
species
conversion
CO.
This
study
presents
bonding
engineering
for
developing
high-performance
solar-driven
reduction
CO2.
ACS Catalysis,
Год журнала:
2024,
Номер
14(2), С. 955 - 964
Опубликована: Янв. 5, 2024
Photocatalytic
oxidation
of
methane
to
methanol
is
an
attractive
process
under
mild
conditions,
nevertheless
confronting
significant
challenges
in
achieving
high
conversion
and
selectivity
simultaneously.
Herein,
we
propose
a
strategy
for
the
direct
rapid
generation
hydroxyl
radicals
(•OH)
from
O2
(O2
→
*OOH
•OH)
by
rational
design
Au–Pd/ZnO
photocatalyst,
skipping
water-soluble
H2O2
avoiding
diffusion.
For
photocatalytic
at
ambient
temperature,
yield
CH3OH
over
optimized
1.0%
AuPd0.5/ZnO
catalyst
were
as
81.0
μmol·h–1
88.2%,
respectively,
exceeding
that
most
reported
systems.
The
formation
Au–Pd
alloys
could
improve
adsorption
cleavage
O–O
bond
*OOH,
facilitating
efficient
•OH
increasing
selectivity.
This
work
provides
some
guidance
delicate
composite
photocatalysts
selective
utilization.
Nature Communications,
Год журнала:
2025,
Номер
16(1)
Опубликована: Янв. 20, 2025
Defect
engineering
can
create
various
vacancy
configurations
in
catalysts
by
finely
tuning
the
local
electronic
and
geometric
structures
of
active
sites.
However,
achieving
precise
control
identification
these
defects
remains
a
significant
challenge,
origin
catalysts,
especially
clustered
or
associated
ones,
largely
unknown.
Herein,
we
successfully
achieve
controllable
fabrication
quantitative
triple
O-Ti-O
associate
(VOVTiVO)
nanosized
Ni-doped
TiO2.
Experimental
theoretical
analyses
demonstrate
that
terminal
hydroxyls
adsorbed
at
unsaturated
cationic
sites
play
an
essential
role
boosting
VOVTiVO
formation,
which
enhances
H2O
dissociation
facilitates
dissociative
OH*
deprotonation
for
defect
site
regeneration.
In
contrast,
single
VO
be
easily
saturated
bridging
hydroxyl
accumulation,
leading
to
gradual
decrease
number
The
TiO2
is
evidenced
its
comparable
catalytic
performance
hydrogen
evolution
reaction
hydrodechlorination
reactions.
Our
work
highlights
importance
vacancy-associated
presents
notable
approach
designing
highly
selective
efficient
H2O-involved
enhance
manipulating
configurations,
but
controlling
them
challenging.
authors
report
vacancies
TiO2,
boost
reactions
through
water
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
62(4)
Опубликована: Ноя. 30, 2022
Direct
photocatalytic
oxidation
of
methane
to
liquid
oxygenated
products
is
a
sustainable
strategy
for
valorization
at
room
temperature.
However,
in
this
reaction,
noble
metals
are
generally
needed
function
as
cocatalysts
obtaining
adequate
activity
and
selectivity.
Here,
we
report
atomically
dispersed
nickel
anchored
on
nitrogen-doped
carbon/TiO2
composite
(Ni-NC/TiO2
)
highly
active
selective
catalyst
photooxidation
CH4
C1
oxygenates
with
O2
the
only
oxidant.
Ni-NC/TiO2
exhibits
yield
198
μmol
4
h
selectivity
93
%,
exceeding
that
most
reported
high-performance
photocatalysts.
Experimental
theoretical
investigations
suggest
single-atom
Ni-NC
sites
not
enhance
transfer
photogenerated
electrons
from
TiO2
isolated
Ni
atoms
but
also
dominantly
facilitate
activation
form
key
intermediate
⋅OOH
radicals,
which
synergistically
lead
substantial
enhancement
both
ACS Catalysis,
Год журнала:
2023,
Номер
13(6), С. 3768 - 3774
Опубликована: Март 2, 2023
Oxidation
of
methane
into
valuable
chemicals,
such
as
C2+
molecules,
has
been
long
sought
after
but
the
dilemma
between
high
yield
and
selectivity
desired
products
remains.
Herein,
is
upgraded
through
photocatalytic
oxidative
coupling
(OCM)
over
a
ternary
Ag–AgBr/TiO2
catalyst
in
pressurized
flow
reactor.
The
ethane
35.4
μmol/h
with
79%
obtained
under
6
bar
pressure.
These
are
much
better
than
most
previous
benchmark
performance
OCM
processes.
results
attributed
to
synergy
Ag
AgBr,
where
serves
an
electron
acceptor
promotes
charge
transfer
AgBr
forms
heterostructure
TiO2
not
only
facilitate
separation
also
avoid
overoxidation
process.
This
work
thus
demonstrates
efficient
strategy
for
conversion
by
both
rational
design
reactor
engineering
conversion.
Advanced Energy Materials,
Год журнала:
2023,
Номер
13(36)
Опубликована: Авг. 13, 2023
Abstract
The
conversion
of
methane
to
value‐added
chemicals
by
traditional
reforming
processes
suffers
from
intensive
energy
consumption
due
its
particularly
strong
C─H
bonds.
Thus,
it
is
urgent
optimize
the
driving
force
structure
for
accelerating
integration
sustainable
energy.
In
this
review,
advances
in
energy‐driven
are
systematically
summarized
provide
a
scientific
understanding
operation/storage
concepts,
reactor
design,
technological
maturity,
system
optimization,
and
remaining
issues.
Furthermore,
essence,
economic
evaluations,
balance,
social
impacts
driven
carefully
discussed,
paving
path
future
course
research
development.
Diversifying
mix
can
play
an
important
role
industries,
being
used
as
crucial
step
transition
energy,
especially
combination
solar/nuclear
with
fossil
fuels
produce
chemicals.
Additionally,
review
intends
bridge
studies
development,
ultimate
goal
offering
robust
framework
understand
current
status
guidance
design
solutions
greener
future.
