Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(13)
Опубликована: Янв. 16, 2024
Abstract
Activation
of
ubiquitous
C(sp
3
)−H
bonds
is
extremely
attractive
but
remains
a
great
challenge.
Heterogeneous
photocatalysis
offers
promising
and
sustainable
approach
for
activation
has
been
fast
developing
in
the
past
decade.
This
Minireview
focuses
on
mechanism
strategies
heterogeneous
photocatalytic
activation.
After
introducing
mechanistic
insights,
including
precise
design
active
sites,
regulation
reactive
radical
species,
improving
charge
separation
reactor
innovations
are
discussed.
In
addition,
recent
advances
hydrocarbons,
alcohols,
ethers,
amines
amides
by
summarized.
Lastly,
challenges
opportunities
outlined
to
encourage
more
efforts
development
this
exciting
field.
Angewandte Chemie,
Год журнала:
2024,
Номер
136(34)
Опубликована: Июнь 11, 2024
Abstract
Light‐driven
photoredox
catalysis
presents
a
promising
approach
for
the
activation
and
conversion
of
methane
(CH
4
)
into
high
value‐added
chemicals
under
ambient
conditions.
However,
C−H
bond
dissociation
energy
CH
absence
well‐defined
sites
on
catalysts
significantly
limit
highly
efficient
toward
multicarbon
(C
2+
hydrocarbons,
particularly
ethylene
2
H
).
Herein,
we
demonstrate
bimetallic
design
Ag
nanoparticles
(NPs)
Pd
single
atoms
(SAs)
ZnO
cascade
C
with
highest
production
rate
compared
previous
works.
Mechanistic
studies
reveal
that
synergistic
effect
NPs
SAs,
upon
effecting
key
bond‐breaking
‐forming
events,
lowers
overall
barrier
process
both
resulting
6
,
constituting
truly
catalytic
system
to
facilitate
generation.
This
work
offers
novel
perspective
advancement
photocatalytic
directional
hydrocarbons
through
subtle
catalyst
strategy.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Май 24, 2024
Abstract
Photocatalytic
coupling
of
methane
to
ethane
and
ethylene
(C
2
compounds)
offers
a
promising
approach
utilizing
the
abundant
resource.
However,
state-of-the-art
photocatalysts
usually
suffer
from
very
limited
C
formation
rates.
Here,
we
report
our
discovery
that
anatase
TiO
nanocrystals
mainly
exposing
{101}
facets,
which
are
generally
considered
less
active
in
photocatalysis,
demonstrate
surprisingly
better
performances
than
those
high-energy
{001}
facet.
The
palladium
co-catalyst
plays
pivotal
role
Pd
2+
site
on
accounts
for
selective
formation.
We
unveil
facet
favors
hydroxyl
radicals
aqueous
phase
near
surface,
where
they
activate
molecules
into
methyl
radicals,
participates
facilitating
adsorption
radicals.
This
work
provides
strategy
design
efficient
nanocatalysts
photocatalytic
by
reaction-space
separation
optimize
heterogeneous-homogeneous
reactions
at
solid-liquid
interfaces.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(13)
Опубликована: Янв. 16, 2024
Abstract
Activation
of
ubiquitous
C(sp
3
)−H
bonds
is
extremely
attractive
but
remains
a
great
challenge.
Heterogeneous
photocatalysis
offers
promising
and
sustainable
approach
for
activation
has
been
fast
developing
in
the
past
decade.
This
Minireview
focuses
on
mechanism
strategies
heterogeneous
photocatalytic
activation.
After
introducing
mechanistic
insights,
including
precise
design
active
sites,
regulation
reactive
radical
species,
improving
charge
separation
reactor
innovations
are
discussed.
In
addition,
recent
advances
hydrocarbons,
alcohols,
ethers,
amines
amides
by
summarized.
Lastly,
challenges
opportunities
outlined
to
encourage
more
efforts
development
this
exciting
field.
