Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(28)
Published: Feb. 15, 2024
Abstract
Photocatalytic
oxygen
(O
2
)
reduction
to
hydrogen
peroxide
(H
O
is
considered
be
a
promising
method
for
energy
storage.
However,
it
suffers
from
the
rapid
recombination
of
carriers,
limited
solubility
and
slow
diffusion
,
self‐decomposition
H
in
traditional
diphase
systems.
Here,
self‐floating
carbon
dots/conjugated
microporous
polymer
(CDs/CMP)
photocatalytic
system
established
production
organic
synthesis.
Due
D–π–A
structure,
porous
hydrophobicity,
CMP
induced
intramolecular
charge
transfer,
exposed
abundant
reaction
sites,
enhanced
adsorption.
CDs
act
as
“bridges”
electron
transmission
regulate
surface
hydrophobicity
CMP,
further
improving
transfer
optimizing
interface.
CDs/CMP
exhibits
high
8542.6
µmol
g
−1
h
concurrent
furoic
acid
at
2.22
m
.
This
rate
≈90%
higher
than
that
system,
exceeding
all
previously
reported
photocatalysts
triphase
Notably,
achieves
relative
separation
suppressing
generated
self‐decomposition.
Theoretical
calculations
situ
characterizations
reveal
mechanism
evolution.
provides
insights
into
exploring
application
metal‐free
heterogeneous
reactions.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
34(24)
Published: Feb. 19, 2024
Abstract
Photosynthesis
of
hydrogen
peroxide
(H
2
O
)
is
regarded
as
an
economically
efficient
and
environmentally
friendly
synthesis
method.
However,
the
scalability
photocatalytic
H
production
(PHP)
hindered
by
sluggish
reaction
kinetics
rapid
recombination
photogenerated
charge
carriers.
In
this
study,
organic
amine‐constrained
ions
intercalated
carbon
nitride/CdSe‐diethylenetriamine
(K
+
/I
−
‐CN/CdSe‐D)
S‐scheme
heterojunction
synthesized
using
organic–inorganic
hybrid
approach
employed
for
PHP
first
time.
The
optimization
interface
I
K
contributed
to
enhanced
light
absorption
capabilities
reduced
interlayer
transfer
distance.
Concurrently,
synergy
C─Se
bonds
at
effectively
modulated
electron
pathways.
coordination
environment
mechanism
are
thoroughly
investigated
extended
X‐ray
fine
structure
in
situ
irradiated
photoelectron
spectroscopy.
rate
40%K
‐CN/CdSe‐D
reached
2240.23
µmol
h
−1
g
pure
water.
This
study
highlights
significance
dual
tuning
chemical
ionic
intercalation
effective
strategy
enhancing
,
paving
way
further
advancements
technology.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(18), P. 12386 - 12394
Published: March 19, 2024
Difluoromethylation
reactions
are
increasingly
important
for
the
creation
of
fluorine-containing
heterocycles,
which
core
groups
in
a
diverse
range
biologically
and
pharmacologically
active
ingredients.
Ideally,
this
typically
challenging
reaction
could
be
performed
photocatalytically
under
mild
conditions.
To
achieve
separation
redox
processes
would
required
efficient
generation
difluoromethyl
radicals
reduction
oxygen.
A
covalent
organic
framework
photocatalytic
material
was,
therefore,
designed
with
dual
reactive
centers.
Here,
anthracene
was
used
as
site
benzothiadiazole
an
oxidation
site,
distributed
tristyryl
triazine
framework.
Efficient
charge
ensured
by
superior
electron-donating
-accepting
abilities
centers,
creating
long-lived
photogenerated
electron–hole
pairs.
Photocatalytic
difluoromethylation
16
compounds
high
yields
remarkable
functional
group
tolerance
demonstrated;
included
bioactive
molecules
such
xanthine
uracil.
The
structure–function
relationship
dual-active-center
photocatalyst
investigated
through
electron
spin
resonance,
femtosecond
transient
absorption
spectroscopy,
density
theory
calculations.
