Inorganic Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 15, 2025
Developing
new
photocatalysts
for
the
selective
oxidation
of
thioethers
to
high-value-added
sulfoxides
under
low-oxygen
mild
conditions
is
a
promising
but
challenging
strategy.
Here,
polyoxometalate-based
metal–organic
framework
(POMOF),
CoBW12–TPT,
was
successfully
synthesized,
wherein
continuous
π···π
stacking
interactions
and
direct
coordination
bonds
not
only
strengthen
framework's
stability
also
accelerate
electron
transfer.
A
series
experiments
theoretical
studies,
including
control
experiments,
kinetic
electrochemical
spectroscopic
analyses,
paramagnetic
resonance,
revealed
synergistic
catalytic
effect
among
Co(II)
metal
centers,
BW12O405–,
photosensitizer
TPT.
CoBW12–TPT
applied
in
photocatalytic
sulfoxides.
Under
irradiation,
photoinduced
transfer
POMOF
leads
generation
superoxide
radicals
from
O2,
which
controls
sulfoxide
compounds
desulfurization
reaction
shows
good
activity.
In
particular,
it
can
be
construction
some
drug
molecules
such
as
Modafinil
Albendazole
Oxide.
ACS Nano,
Год журнала:
2023,
Номер
17(17), С. 16993 - 17003
Опубликована: Авг. 22, 2023
Effective
photodynamic
therapy
(PDT)
requires
photosensitizers
(PSs)
to
massively
generate
type
I
reactive
oxygen
species
(ROS)
in
a
less
oxygen-dependent
manner
the
hypoxia
tumor
microenvironment.
Herein,
we
present
cascade
strategy
boost
ROS,
especially
hydroxyl
radical
(OH·-),
generation
with
an
aggregation-induced
emission
(AIE)
photosensitizer-albumin
complex
for
hypoxia-tolerant
PDT.
The
cationic
AIE
PS
TPAQ-Py-PF6
(TPA
=
triphenylamine,
Q
anthraquinone,
Py
pyridine)
contains
three
important
moieties
cooperatively
enhance
free
generation:
AIE-active
TPA
unit
ensures
effective
triplet
exciton
aggregate,
anthraquinone
moiety
possesses
redox
cycling
ability
promote
electron
transfer,
while
methylpyridinium
cation
further
increases
intramolecular
charge
transfer
and
separation
processes.
Inserting
into
hydrophobic
domain
of
bovine
serum
albumin
nanoparticles
(BSA
NPs)
could
greatly
immobilize
its
molecular
geometry
increase
generation,
electron-rich
microenvironment
BSA
ultimately
leads
OH·-
generation.
Both
experimental
theoretical
results
confirm
effectiveness
our
cationization
immobilization
enhancing
In
vitro
vivo
experiments
validate
excellent
antitumor
PDT
performance
NPs,
superior
conventional
polymeric
encapsulation
approach.
Such
multidimensional
specially
boosting
shall
hold
great
potential
related
applications.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Март 21, 2024
Abstract
Photodynamic
therapy
(PDT)
is
a
promising
cancer
treatment
but
has
limitations
due
to
its
dependence
on
oxygen
and
high-power-density
photoexcitation.
Here,
we
report
polymer-based
organic
photosensitizers
(PSs)
through
rational
PS
skeleton
design
precise
side-chain
engineering
generate
•O
2
−
•OH
under
oxygen-free
conditions
using
ultralow-power
808
nm
photoexcitation
for
tumor-specific
photodynamic
ablation.
The
designed
skeletons
can
electron-hole
pairs
sensitize
H
O
into
with
photoexcitation,
achieving
NIR-photoexcited
oxygen-independent
production.
Further,
compared
commonly
used
alkyl
side
chains,
glycol
oligomer
as
the
chain
mitigates
recombination
offers
more
molecules
around
generated
from
hydrophobic
skeletons,
which
yield
4-fold
stronger
production,
thus
allowing
an
high
PDT
effect.
Finally,
feasibility
of
developing
activatable
PSs
in
female
mice
further
demonstrated
irradiation
15
mW
cm
−2
.
study
not
only
provides
insights
mechanism
also
general
guideline
develop
NIR
PDT.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(25)
Опубликована: Апрель 20, 2023
NIR-II-emitting
photosensitizers
(PSs)
have
attracted
great
research
interest
due
to
their
promising
clinical
applications
in
imaging-guided
photodynamic
therapy
(PDT).
However,
it
is
still
challenging
realize
highly
efficient
PDT
on
NIR-II
PSs.
In
this
work,
we
develop
a
chlorination-mediated
π-π
organizing
strategy
improve
the
of
PS
with
conjugation-extended
A-D-A
architecture.
The
significant
dipole
moment
carbon-chlorine
bond
and
strong
intermolecular
interactions
chlorine
atoms
bring
compact
stacking
chlorine-substituted
PS,
which
facilitates
energy/charge
transfer
promotes
photochemical
reactions
PDT.
Consequently,
resultant
emitting
exhibits
leading
performance
yield
reactive
oxygen
species
higher
than
that
previously
reported
long-wavelength
These
findings
will
enlighten
future
design
PSs
enhanced
efficiency.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(12)
Опубликована: Янв. 23, 2024
We
herein
present
an
approach
of
photo-induced
disproportionation
for
preparation
Type-I
photodynamic
agents.
As
a
proof
concept,
BODIPY-based
photosensitizers
were
rationally
designed
and
prepared.
The
intermolecular
electron
transfer
between
homotypic
chromophores
leads
to
the
reaction,
resulting
in
formation
charged
intermediates,
cationic
anionic
radicals.
radicals
efficiently
oxidize
cellularimportant
coenzyme,
tetrahydrobiopterin
(BH
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(9), С. 6252 - 6265
Опубликована: Фев. 20, 2024
Conventional
photodynamic
therapy
(PDT)
is
often
limited
in
treating
solid
tumors
due
to
hypoxic
conditions
that
impede
the
generation
of
reactive
oxygen
species
(ROS),
which
are
critical
for
therapeutic
efficacy.
To
address
this
issue,
a
fractionated
PDT
protocol
has
been
suggested,
wherein
light
irradiation
administered
stages
separated
by
dark
intervals
permit
recovery
during
these
breaks.
However,
current
photosensitizers
used
incapable
sustaining
ROS
production
intervals,
leading
suboptimal
outcomes
(Table
S1).
circumvent
drawback,
we
have
synthesized
novel
photosensitizer
based
on
triple-anthracene
derivative
designed
prolonged
generation,
even
after
cessation
exposure.
Our
study
reveals
unique
action
derivatives,
facilitating
direct
and
effective
disruption
biomolecules
significantly
improving
efficacy
S2).
Moreover,
existing
lack
imaging
capabilities
monitoring,
constraints
fine-tuning
parameters
also
serves
as
an
afterglow
agent,
emitting
sustained
luminescence
postirradiation.
This
function
allows
precise
optimization
between
sessions
aids
determining
timing
subsequent
irradiation,
thus
enabling
meticulous
control
over
parameters.
Utilizing
our
photosensitizer,
formulated
regimen
effectively
eliminates
orthotopic
pancreatic
tumors.
investigation
highlights
promise
employing
long-persistent
activity
advanced
approaches
overcome
limitations
tumor
treatment.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Апрель 6, 2024
Abstract
Single-atom
catalysts
(SACs)
have
attracted
interest
in
photodynamic
therapy
(PDT),
while
they
are
normally
limited
by
the
side
effects
on
normal
tissues
and
interference
from
Tumor
Microenvironment
(TME).
Here
we
show
a
TME-activated
situ
synthesis
of
SACs
for
efficient
tumor-specific
water-based
PDT.
Upon
reduction
upregulated
GSH
TME,
C
3
N
4
-Mn
obtained
TME
with
Mn
atomically
coordinated
into
cavity
nanosheets.
This
overcomes
toxicity
random
distribution
catalyst
release
healthy
tissues.
Based
Ligand-to-Metal
charge
transfer
(LMCT)
process,
exhibit
enhanced
absorption
red-light
region.
Thereby,
water-splitting
process
is
induced
under
660
nm
irradiation,
which
initiates
O
2
-independent
generation
highly
toxic
hydroxyl
radical
(·OH)
cancer-specific
Subsequently,
·OH-initiated
lipid
peroxidation
demonstrated
to
devote
effective
cancer
cell
death.
The
synthesized
facilitate
precise
conversion
inert
H
reactive
·OH,
facilitates
female
mice.
strategy
achieves
therapy,
not
only
avoiding
but
also
overcoming
tumor
hypoxia.
