Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
60(41), С. 22368 - 22375
Опубликована: Авг. 12, 2021
Abstract
The
salts
{[Ln
2
Ln*(Hhmq)
3
(OAc)
(hfac)
]
+
[Ln*(hfac)
(OAc)(MeOH)]
−
}
(Hhmq=2‐methanolquinolin‐8‐oxide,
hfac=hexafluoroacetylacetonate;
Ln,
Ln*=Er,
Gd,
Yb)
feature
a
discrete
heteronuclear
cation
consisting
of
two
types
lanthanide
atoms.
quinolinoxy
O‐atom
serves
as
μ
‐bridge
to
Ln
atoms
and
all
three
atoms,
with
metal⋅⋅⋅metal
distances
being
around
3.7
Å.
For
1
(
[Yb
Er]
),
near‐infrared
downshifted
luminescence
is
switched
competitive
upconversion
upon
irradiation
by
980
nm
laser
under
an
extremely
low
excitation
power
(0.288
W
cm
−2
)
through
introduction
fluoride
ions.
stability
after
addition
was
confirmed
powder
X‐ray
diffraction
multistage
mass
spectrometry,
associated
the
H
NMR
6
[La
Eu]
).
More
importantly,
at
least
20‐fold
enhancement
quantum
yield
in
non‐deuterated
solvents
room
temperature
densities
(2
highest
among
few
molecular
examples
reported.
Chemical Society Reviews,
Год журнала:
2021,
Номер
50(4), С. 2839 - 2891
Опубликована: Янв. 1, 2021
Supramolecular
cancer
nanotheranostics
have
shown
promising
potentials
in
early-stage
diagnosis
and
personal
therapy.
Herein,
we
summarize
the
progress
of
supramolecular
provide
guidance
for
designing
new
targeted
theranostic
agents.
Advanced Materials,
Год журнала:
2023,
Номер
36(4)
Опубликована: Авг. 29, 2023
Photodynamic
therapy
(PDT),
which
utilizes
type
I
photoreactions,
has
great
potential
as
an
effective
cancer
treatment
because
of
its
hypoxia-tolerant
superiority
over
the
commonly
used
II
pathway.
A
few
photosensitizers
are
exploited;
however,
they
majorly
induce
cytotoxicity
and
possess
poor
tumor
specificity
low-efficient
theranostics.
To
resolve
this
issue,
herein
aminopeptidase
N
(APN)-activated
phototheranostic
probe
(CyA)
is
reported
for
anti-hypoxic
PDT
in
conjunction
with
immunotherapy
treatment.
CyA
can
specifically
activate
near-infrared
fluorescence,
photoacoustic
signals,
phototoxicity
following
APN-induced
substrate
cleavage
subsequent
generation
active
molecules
(such
CyBr).
endows
specific
imaging
capabilities
toward
cells
overexpressing
APN
under
both
normoxia
hypoxia.
In
addition,
locally
activatable
induces
systemic
antitumor
immune
responses.
More
importantly,
integration
localized
activated
evokes
enhanced
therapeutic
effects
improved
inhibition
efficiency
live
mice
compared
individual
treatments.
This
study
aims
to
present
combination
therapy.
Journal of the American Chemical Society,
Год журнала:
2020,
Номер
142(48), С. 20313 - 20317
Опубликована: Ноя. 13, 2020
Functionalizing
the
redox-active
tetrathiafulvalene
(TTF)
core
with
groups
capable
of
coordination
to
metals
provides
new
perspectives
on
modulation
architectures
and
electronic
properties
organic–inorganic
hybrid
materials.
With
a
view
extending
this
concept,
we
have
now
synthesized
nickel
bis(dithiolene-dibenzoic
acid),
[Ni(C2S2(C6H4COOH)2)2],
which
can
be
considered
as
inorganic
analogue
organic
tetrathiafulvalene-tetrabenzoic
acid
(H4TTFTB).
Likewise,
[Ni(C2S2(C6H4COOH)2)2]
is
linker
for
functional
metal–organic
frameworks,
demonstrated
here
synthesis
[Mn2{Ni(C2S2(C6H4COO)2)2}(H2O)2]·2DMF,
(1,
DMF
=
N,N-dimethylformamide).
1
isomorphic
reported
[Mn2(TTFTB)(H2O)2]
(2)
but
better
electrochemical
glucose
sensor
due
multiple
oxidation–reduction
states
[NiS4]
core,
allow
oxidized
glucolactone
by
high
oxidation
state
center.
As
non-enzymatic
sensor,
Cu
foam
(CF),
1-CF,
was
one-step
hydrothermal
method
exhibited
an
excellent
performance.
The
fabricated
1-CF
electrode
offers
sensitivity
27.9
A
M–1
cm–2,
wide
linear
detection
range
from
2.0
×
10–6
10–3
M,
low
limit
1.0
10–7
M
(signal/noise
3),
satisfactory
stability
reproducibility.
Journal of the American Chemical Society,
Год журнала:
2020,
Номер
142(38), С. 16409 - 16419
Опубликована: Сен. 3, 2020
Lanthanide-containing
functional
complexes
have
found
a
variety
of
applications
in
materials
science
and
biomedicine
because
their
unique
electroptical
magnetic
properties.
However,
the
poor
stability
solubility
water
multicomponent
lanthanide
organic
assemblies
significantly
limit
practical
applications.
We
report
here
series
water-stable
anionic
Ln2nL3n-type
(n
=
2,
3,
4,
5)
polyhedra
(LOPs)
constructed
by
deprotonation
self-assembly
three
fully
conjugated
ligands
(H4L1
H4L2a/b)
featuring
2,6-pyridine
bitetrazolate
chelating
moiety.
The
outcomes
LOPs
formation
reactions
were
to
be
very
sensitive
toward
reaction
conditions
including
base,
metal
source,
solvents,
concentrations
as
characterized
combination
NMR,
high-resolution
ESI-MS
X-ray
crystallography.
Ligands
H4L2a/b
manifested
an
excellent
sensitization
ions
(Ln
EuIII
TbIII),
with
high
luminescent
quantum
yields
for
Tb8L2a12
(Φ
11.2%
water)
Eu8L2b12
76.8%
DMSO)
measured
polar
solvents.
Furthermore,
due
giant
molecular
weight
rigidity
polyhedral
skeleton,
Gd8L2b12
showed
longitudinal
relaxivity
(r1)
400.53
mM-1S-1.
performance
potential
resonance
imaging
contrast
agents
(CAs)
vivo
was
evaluated
much
longer
retention
time
tumor
sites
compared
commercial
GdIII-based
CAs.
Dual-modal
has
also
been
demonstrated
mixed
Eu/Gd
LOPs.
Our
results
not
only
provide
new
design
route
multinuclear
but
offer
candidates
supramolecular-edifices
bioimaging
drug
delivery.
Chemical Science,
Год журнала:
2020,
Номер
11(26), С. 6701 - 6708
Опубликована: Янв. 1, 2020
Photodynamic
therapy
has
become
an
emerging
strategy
for
the
treatment
of
cancer.
This
technology
relies
on
development
photosensitizers
(PSs)
that
convert
molecular
oxygen
to
cytotoxic
reactive
species
upon
exposure
light.
In
this
study,
we
have
developed
a
facile
and
general
obtaining
visible
light/near-infrared-absorbing
PSs
by
performing
simple
sulfur-for-oxygen
replacement
within
existing
fluorophores.
Thionation
carbonyl
groups
fluorophore
cores
leads
improvement
singlet
quantum
yield
molar
absorption
coefficient
at
longer
wavelengths
(deep
600-800
nm).
Additionally,
these
thio-based
lack
dark
cytotoxicity
but
exhibit
significant
phototoxicity
against
monolayer
cancer
cells
3D
multicellular
tumor
spheroids
with
IC50
in
micromolar
range.
To
achieve
tumor-specific
delivery,
conjugated
antibody
demonstrated
their
therapeutic
activity.
Journal of the American Chemical Society,
Год журнала:
2021,
Номер
143(19), С. 7541 - 7552
Опубликована: Май 11, 2021
Phototheranostics
constitute
an
emerging
cancer
treatment
wherein
the
core
diagnostic
and
therapeutic
functions
are
integrated
into
a
single
photosensitizer
(PS).
Achieving
full
potential
of
this
modality
requires
being
able
to
tune
photosensitizing
properties
PS
in
question.
Structural
modification
organic
framework
represents
time-honored
strategy
for
tuning
photophysical
features
given
system.
Here
we
report
easy-to-implement
metal
selection
approach
that
allows
fine-tuning
excited-state
energy
dissipation
phototheranostics
as
exemplified
by
set
lanthanide
(Ln
=
Gd,
Yb,
Er)
carbazole-containing
porphyrinoid
complexes.
Femto-
nanosecond
time-resolved
spectroscopic
studies,
conjunction
with
density
functional
theory
calculations,
revealed
pathways
PSs
highly
dependent
on
gap
between
lowest
triplet
excited
state
ligand
states
coordinated
Ln
ions.
The
Yb
complex
displayed
balance
deactivation
mechanisms
made
it
attractive
combined
photoacoustic
imaging
photothermal/photodynamic
therapy
agent.
It
was
encapsulated
mesoporous
silica
nanoparticles
(MSN)
provide
biocompatible
construct,
YbL@MSN,
which
displays
high
photothermal
conversion
efficiency
(η
45%)
decent
singlet
oxygen
quantum
yield
(ΦΔ
31%).
Mouse
model
studies
YbL@MSN
both
synergistic
photothermal-
photodynamic-therapy-based
tumor
reduction
vivo.
Our
results
lead
us
suggest
promising
phototheranostics.
Chemical Society Reviews,
Год журнала:
2022,
Номер
51(14), С. 6177 - 6209
Опубликована: Янв. 1, 2022
This
Review
summarises
the
history
and
‘state-of-the-art’
development
of
lanthanide
(Ln)
porphyrinoids
as
theranostic
agents.
Applications
such
near-infrared
(NIR)
fluorescence
imaging
(FL),
magnetic
resonance
(MRI),
radiotherapy,
chemotherapy
phototheranostics
will
be
discussed.
Chemistry of Materials,
Год журнала:
2022,
Номер
34(4), С. 1956 - 1964
Опубликована: Фев. 12, 2022
Incorporation
of
molecular
switches
with
light,
heat,
and
electricity
responsibility
into
artificial
solids
has
been
developed
as
a
successful
strategy
to
construct
stimuli-responsive
functional
materials.
However,
precise
manipulation
their
geometries
electronic
structures
control
the
properties
macroscopic
materials
still
remains
fundamental
challenge.
Herein,
photoresponsive
covalent
organic
framework
(o-COF)
square
lattice
was
fabricated
from
dynamic
chemistry
reaction
ring-open
dithienylethene–dialdehyde
5,10,15,20-tetrakis(4-aminophenyl)porphyrin
(H2TAPP).
UV
irradiation
dithienylethene-based
units
in
o-COF
afforded
its
reversible
photoisomer
(c-COF)
ring-closed
form.
In
addition
range
diffraction,
microscopic,
gas
physical
sorption
characterizations,
spectroscopic
investigations
help
theoretical
simulations
revealed
different
photocatalytic
activities
toward
evolution
singlet
oxygen
corresponding
oxidation
amines
due
energy
transfer
pathways
porphyrin
unit
BBTP
photoisomers
these
two
COFs.
Most
interestingly,
such
behaviors
for
COFs
could
be
easily
tuned
manner
by
adjusting
ring-closed/open
form
dithienylethene
means
visible
light.