Accounts of Chemical Research,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Jan. 25, 2024
ConspectusThe
pursuit
of
in-depth
studying
the
nature
and
law
life
activity
has
been
dominating
current
research
fields,
ranging
from
fundamental
biological
studies
to
applications
that
concern
synthetic
biology,
bioanalysis,
clinical
diagnosis.
Motivated
by
this
intention,
spatiotemporally
controlled
in
situ
analysis
living
cells
a
prospective
branch
virtue
high-sensitivity
imaging
key
biomolecules,
such
as
biomarkers.
The
past
decades
have
attested
deoxyribonucleic
acid
(DNA),
with
biocompatibility,
programmability,
customizable
features,
is
competitive
biomaterial
for
constructing
high-performance
molecular
sensing
tools.
To
conquer
complexity
wide
extracellular–intracellular
distribution
biomarkers,
it
meaningful
breakthrough
explore
high-efficiently
amplified
DNA
circuits,
which
excel
at
operating
complex
yet
captivating
dynamic
reaction
networks
various
bioapplications.
In
parallel,
multidimensional
performance
improvements
nucleic
including
availability,
detection
sensitivity,
reliability,
are
critical
parameters
realizing
accurate
cell
regulation
bioanalysis.In
Account,
we
summarize
our
recent
work
on
enzyme-free
bioanalysis
three
main
aspects:
circuitry
functional
extension
recognition
epigenetic
regulation,
amplification
ability
improvement
sensitive
biomarker
detection,
site-specific
activation
systems
reliable
imaging.
first
part,
designed
an
epigenetically
responsive
deoxyribozyme
(DNAzyme)
system
intracellular
gene
enriches
possible
analyzed
species
chemically
modifying
conventional
DNAzyme.
For
example,
exquisite
N6-methyladenine
(m6A)-caged
DNAzyme
was
built
achieving
precise
FTO
(fat
mass
obesity-associated
protein)-directed
regulation.
addition,
varieties
DNAzyme-based
nanoplatforms
self-sufficient
cofactor
suppliers
were
assembled,
subdued
speed-limiting
hardness
cofactors
live-cell
applications.
second
developed
series
hierarchically
assembled
improve
signal
transduction
traditional
circuits.
First,
circuit
significantly
enhanced
via
several
heterogeneously
or
homogeneously
concatenated
models.
Furthermore,
feedback
pathway
integrated
into
these
thus
dramatically
increasing
efficiency.
Second,
considering
cellular
environment,
simplified
redundancy
multicomponents
procedures
cascaded
relying
minimal
component
merely
one
modular
catalytic
reaction,
guaranteed
high
cell-delivering
uniformity
while
fostering
kinetics
reliability.
third
constructed
in-cell-selective
endogenous-stimulated
multiply
recognitions,
could
not
only
eliminate
leakage,
but
also
retain
its
on-site
multiplex
amplification.
Based
strategy,
more
availability
scenarios
acquired
These
demonstrate
purpose-to-concreteness
engineering
tailored
multimolecule
multiple
amplification,
high-gain
high-reliability
targeted
bioanalysis.
We
envision
network
can
contribute
bioanalytical
layouts,
will
facilitate
progression
diagnosis
prognosis.
ACS Nano,
Journal Year:
2021,
Volume and Issue:
15(9), P. 14253 - 14262
Published: Aug. 19, 2021
As
a
powerful
signal
amplification
tool,
the
DNA
walker
has
been
widely
applied
to
detect
rare
microRNA
(miRNA)
in
vivo.
Despite
significant
advances,
near-infrared
(NIR)
light
controllable
for
powered
by
an
endogenous
initiator
not
realized,
which
is
crucial
spatiotemporal
imaging
of
miRNA
living
cells
with
high
sensitivity.
Herein,
we
constructed
NIR-photoactivatable
system,
was
adenosine
triphosphate
(ATP)
situ
spatial
and
temporal
resolution.
The
system
very
stable
extremely
low
fluorescent
background
bioimaging
cells.
We
employed
upconversion
nanoparticles
(UCNPs)
as
carriers
probe
transducers
converting
NIR
UV
light.
Coupled
fueled
intracellular
ATP,
smart
based
on
initiated
successfully
developed
precise
control
Triggered
light,
could
autonomously
progressively
travel
along
track
assistance
ATP.
different
cell
lines
highly
This
strategy
can
expand
photocontrol
biological
system.
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(33), P. 17937 - 17941
Published: June 12, 2021
Abstract
MicroRNA
(miRNA)
functions
are
tightly
regulated
by
their
sub‐compartmental
location
in
living
cells,
and
the
ability
to
imaging
of
mitochondrial
miRNAs
(mitomiRs)
is
essential
for
understanding
related
pathological
processes.
However,
most
existing
DNA‐based
methods
could
not
be
used
this
purpose.
Here,
we
report
development
a
DNA
nanoreporter
technology
mitomiRs
cells
through
near‐infrared
(NIR)
light‐controlled
strand
displacement
reactions.
The
sensing
function
nanoreporters
silent
(OFF)
during
delivery
process,
but
can
photoactivated
(ON)
with
NIR
light
after
targeted
localization,
enabling
spatially‐restricted
two
types
cancer‐related
improved
detection
accuracy.
Furthermore,
demonstrate
vivo
spatiotemporally‐controlled
activation.
Therefore,
study
illustrates
simple
methodology
that
may
broadly
applicable
investigating
mitomiRs‐associated
physiological
events.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(45)
Published: July 1, 2022
Abstract
The
wide
extracellular‐intracellular
distribution
of
microRNA
requires
the
on‐site,
robust
and
efficient
activation
catalytic
DNA
circuits
inside
live
cells.
Herein,
we
develop
an
non‐enzymatic
circuitry
strategy
to
realize
orthogonally
controlled
(CCD)
circuit
for
achieving
high‐fidelity
in
vivo
imaging
through
multiply
guaranteed
molecular
recognition
progressively
accelerated
signal
amplification.
For
predictable
on‐site
useful
efficiency,
dominating
fuel
strand
was
initially
split
into
inactive
subunits
that
were
grafted
auxiliary
circuit.
There,
in‐cell‐specific
mRNA
triggered
orthogonal
amplification
active
strands
sensitive
target
detection
chief
entropy‐driven
We
believe
method
can
contribute
clinical
diagnosis
prognosis.
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
36(23)
Published: Feb. 15, 2024
Abstract
Photoactivatable
molecules,
with
high‐precision
spatialtemporal
control,
have
largely
promoted
bioimaging
and
phototherapy
applications
of
fluorescent
dyes.
Here,
the
first
photoactivatable
sensor
(
BI
)
is
described
that
can
be
triggered
by
broad
excitation
light
(405–660
nm),
which
further
undergoes
intersystem
crossing
H‐atom
transfer
processes
to
forming
superoxide
anion
radicals
(O
2
−•
carbon
radicals.
Particularly,
photoinduced
gain
carbon‐centered
BI•
allows
for
radical‐radical
coupling
afford
combined
crosslink
product
BI─BI
),
would
oxidized
in
presence
O
produce
an
extended
conjugate
system
near
infrared
emission
(820
nm).
Besides,
photochemically
generated
Cy─BI
possesses
ultra‐high
photothermal
conversion
efficiency
up
90.9%,
optimized
potential.
What′s
more,
Western
Blot
assay
reveals
both
photoproduct
efficiently
inhibit
expression
CHK1,
irradiation
induces
apoptosis
ultimately
enhances
phototherapeutic
effects.
Thus,
combination
cell
cycle
block
inducing
apoptosis,
photodynamic
therapy
treatments
significantly
suppress
solid
tumor
vivo
antitumor
efficacy
explorations.
This
a
novel
finding
developing
as
well
applicability
photoimaging
tumor‐related
areas.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(10)
Published: Jan. 23, 2024
DNAzyme-based
fluorescent
probes
for
imaging
metal
ions
in
living
cells
have
received
much
attention
recently.
However,
employing
situ
within
subcellular
organelles,
such
as
nucleus,
remains
a
significant
challenge.
We
developed
three-stranded
DNAzyme
probe
(TSDP)
that
contained
20-base-pair
(20-bp)
recognition
site
of
CRISPR/Cas9,
which
blocks
the
activity.
When
Cas9,
with
its
specialized
nuclear
localization
function,
forms
an
active
complex
sgRNA
cell
it
cleaves
TSDP
at
site,
resulting
formation
catalytic
structure.
With
this
design,
CRISPR/Cas9-inducible
Zn
Angewandte Chemie International Edition,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 9, 2025
Abstract
Adenosine
triphosphate
(ATP),
the
primary
energy
currency
in
cells,
is
dynamically
regulated
across
different
subcellular
compartments.
The
ATP
interplay
between
mitochondria
and
endoplasmic
reticulum
(ER)
underscores
their
coordinated
roles
various
biochemical
processes,
highlighting
necessity
for
precise
profiling
of
dynamics.
Here
we
present
an
exogenously
endogenously
dual‐regulated
DNA
nanodevice
spatiotemporally
selective,
subcellular‐compartment
specific
signal
amplification
sensing.
system
allows
exogenous
NIR
light‐controlled
spatiotemporal
localization
activation
aptamer
sensor
or
ER,
while
a
endogenous
enzyme
organelles
further
drives
via
consumption
molecular
beacon
fuels,
resulting
significantly
enhanced
sensitivity
spatial
precision
organelle
interest.
Furthermore,
demonstrate
application
this
robust
monitoring
fluctuations
ER
following
drug
interventions.
This
advancement
provides
powerful
tool
improving
our
understanding
cellular
energetics
at
level
holds
potential
development
targeted
therapeutics.
ACS Nano,
Journal Year:
2021,
Volume and Issue:
15(9), P. 14465 - 14474
Published: Sept. 9, 2021
Employing
one-step
hydrothermal
treatment
of
o-phenylenediamine
and
lysine
to
exploit
their
self-
copolymerization,
four
kinds
CDs
(ECDs,
NCDs,
GCDs,
LCDs)
are
synthesized,
possessing
different
surface
groups
(CH3,
C–O–C,
NH2,
COOH)
lipophilicity
which
endow
them
with
various
uptake
pathways
achieve
tunable
organelle
imaging.
Specifically,
highly
lipophilic
ECDs
CH3
group
NCDs
C–O–C
select
passive
manner
target
endoplasmic
reticulum
nucleus,
respectively.
Amphiphilic
GCDs
CH3,
NH2
prefer
caveolin-mediated
endocytosis
locate
at
Golgi
apparatus.
Highly
hydrophilic
LCDs
COOH
involved
in
clathrin-mediated
localize
lysosomes.
Besides,
imaging
results
cell
division,
three-dimensional
reconstruction
living
zebrafish
demonstrate
that
the
obtained
promising
potential
candidates
for
specific
organelle-targeting
Angewandte Chemie International Edition,
Journal Year:
2021,
Volume and Issue:
60(27), P. 14887 - 14891
Published: April 19, 2021
The
dynamic
variation
of
the
expression
profile
and
spatial
landscape
multiple
enzymes
are
crucial
factors
influencing
tumor
progression
drug
treatment.
However,
comprehensive
analysis
these
events
has
been
hampered
by
limitations
existing
imaging
technologies.
Here
we
report
a
cooperatively
activatable,
DNA-based
fluorescent
reporter
programmed
to
detect
correlated
activity
dual
enzymes,
telomerase
(TE)
apurinic/apyrimidinic
endonuclease
1
(APE1),
both
in
vitro
vivo.
conformational
change
DNA
probe
can
be
orthogonally
triggered
through
TE-induced
elongation
APE1-mediated
specific
cleavage,
producing
signal
for
two
an
AND-gated
manner.
Furthermore,
demonstrate
capability
system
"dual
lock-and-key"
strategy,
visualizing
enzymatic
activities
during
treatment
cancer.
Advanced Science,
Journal Year:
2021,
Volume and Issue:
9(3)
Published: Nov. 17, 2021
Abstract
Heterostructure
nanoparticles
(NPs),
constructed
by
two
single‐component
NPs
with
distinct
nature
and
multifunctional
properties,
have
attracted
intensive
interest
in
the
past
few
years.
Among
them,
heterostructures
made
of
upconversion
(UCNPs)
metal–organic
frameworks
(MOFs)
can
not
only
integrate
advantageous
characteristics
(e.g.,
porosity,
structural
regularity)
MOFs
unique
upconverted
optical
features
UCNPs,
but
also
induce
cooperative
properties
observed
either
for
single
component
due
to
their
special
or
electronic
communications.
Recently,
diverse
UCNP‐MOF
are
designed
synthesized
via
different
strategies
demonstrated
appealing
potential
applications
biosensing
imaging,
drug
delivery,
photodynamic
therapy
(PDT).
In
this
review,
synthesis
first
summarized,
then
authors
focus
mainly
on
discussion
biomedical
applications,
particularly
as
PDT
agents
cancer
treatment.
Finally,
briefly
outlook
current
challenges
future
perspectives
hybrid
nanocomposites.
The
believe
that
review
will
provide
comprehensive
understanding
inspirations
toward
recent
advances
heterostructures.
ACS Applied Materials & Interfaces,
Journal Year:
2021,
Volume and Issue:
13(33), P. 38931 - 38946
Published: Aug. 10, 2021
With
the
continuous
development
of
DNA
nanotechnology,
various
spatial
structures
and
assembly
techniques
emerge.
Hybridization
chain
reaction
(HCR)
is
a
typical
example
with
exciting
features
bright
prospects
in
biosensing,
which
has
been
intensively
investigated
past
decade.
In
this
Spotlight
on
Applications,
we
summarize
principles
conventional
HCR
some
novel
forms
linear/nonlinear
HCR.
advantages
like
great
kinetics,
facile
operation,
an
enzyme-free
isothermal
reaction,
these
strategies
can
be
integrated
most
mainstream
reporters
(e.g.,
fluorescence,
electrochemistry,
colorimetry)
for
ultrasensitive
detection
abundant
targets.
Particularly,
select
several
representative
studies
to
better
illustrate
ideas
performances
strategies.
Theoretical
practical
utilities
are
confirmed
range
biosensing
applications.
end,
deep
discussion
provided
about
challenges
future
tasks
field.