Accounts of Chemical Research,
Год журнала:
2025,
Номер
unknown
Опубликована: Июнь 3, 2025
ConspectusOver
the
past
decade,
experiments
involving
microdroplets
have
challenged
framework
of
chemistry.
These
droplets
constitute
a
multiphase
system,
where
dynamic
interplay
between
solid,
liquid,
and
gas
influences
reactions.
Multiphase
systems
are
prevalent
in
nature
possess
unique
physicochemical
properties.
However,
chemistry,
phase
boundary
reactivity
is
often
overlooked
because
molecules
experience
"bulk"
reactivity.
biological
processes,
such
as
cell
mitosis,
sensor
technology,
organic
synthesis,
pollution
remediation.Recently,
our
group
has
developed
different
strategies
electrochemiluminescence
(also
called
electrogenerated
chemiluminescence,
both
shortened
to
ECL)
microscopy
imaging
understand
properties
dynamics
at
electrified
interfaces.
ECL
takes
advantage
luminophore
that
radically
annihilates
with
strong
oxidizing
or
reducing
reagent.
If
enthalpy
annihilation
high
enough,
will
be
left
an
excited
state
radiatively
decay,
producing
light.
Thus,
requires
no
incident
light,
analytical
figures
merit
due
light
being
emitted
close
interface
(1-10
μm),
providing
insight
into
within
electrode's
proximity.This
Account
detail
group's
efforts
discovering
reactions
environments
exhibiting
native
triphasic
(liquid|liquid|electrode)
interfaces
new
phases
formed
(e.g.,
bubble
nucleation
electroprecipitation).
We
first
began
developing
tools
necessary
image
liquid|liquid
discovered
that,
when
neighboring
fuse
together,
small
pockets
(inclusions)
continuous
existed
inside
merged
droplets.
Studies
inclusion
chemical
led
interesting
observation
on
can
act
micropumps,
protecting
electrode
from
buildup
during
electrocatalytic
reactions.Even
though
strength
emission
confined
directly
surface,
this
also
significant
weakness,
considering
phenomena
occur
far
away
surface.
One
recent
thrust
community
ways
using
phenomenon
termed
"Through-Space
ECL".
Our
used
technique
measure
forces
boundaries
surface.By
playing
relative
solubilities
reactants
products,
we
showed
if
radical
ion
generated
precipitates
more
quickly
than
its
lifetime,
salts
formed.
way
fossilize
highly
energetic
molecules.
seemingly
tenet
effectively
bottle
up
ECL,
fossilizing
elsewhere
space
time.
Given
passion
teach
world
beauties
electrochemistry,
concepts
surrounding
pedagogically
innovate
performed
by
children
visualize
competing
reactions.In
depict
current
spectroscopy
focus
contributions
burgeoning
field.
field
been
discuss
probability
impact
across
sciences
moving
forward.
Chemical & Biomedical Imaging,
Год журнала:
2025,
Номер
3(5), С. 310 - 321
Опубликована: Март 10, 2025
Two-dimensional
cell
culture
may
be
insufficient
when
it
comes
to
understanding
human
disease.
The
redox
behavior
of
complex,
three-dimensional
tissue
is
critical
disease
genesis
and
propagation.
Unfortunately,
few
measurement
tools
are
available
for
such
models
yield
quantitative
insight
into
how
reactive
oxygen
species
(ROS)
form
over
time.
Here,
we
demonstrate
an
imaging
platform
the
real-time
visualization
H2O2
formation
mammalian
spheroids
made
noncancerous
embryonic
kidney
cells
(HEK-293)
metastatic
breast
cancer
(MCF-7
MDA-MB-231).
We
take
advantage
luminol
electrochemiluminescence
reaction
on
a
transparent
tin-doped
indium
oxide
electrode.
luminescence
this
as
function
[H2O2]
linear
(R2
=
0.98)
with
dynamic
range
between
0.5
μM
0.1
mM,
limit
detection
2.26
±
0.58
μM.
Our
method
allows
observation
ROS
activity
in
growing
days
advance
current
techniques
without
need
sacrifice
sample
postanalysis.
Finally,
use
our
procedure
key
pathways
cancerous
can
up-regulated
downregulated
through
addition
common
metabolic
drugs,
rotenone
carbonyl
cyanide-p-trifluoromethoxyphenylhydrazone.
results
suggest
that
Warburg
Effect
studied
single
spheroids,
drugs
one
implicate
specific
formation.
expect
diagnostic
tool
have
wide
applications
propagation
system
more
closely
related
tissue.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(46), С. 31945 - 31949
Опубликована: Ноя. 5, 2024
Microbubbles,
inside-out
microdroplets,
act
as
extraordinary
microreactors
to
facilitate
thermodynamically
unfavorable
reactions
in
bulk
solutions
of
water.
We
explored
the
formation
hydrogen
peroxide
(H
Chemical Communications,
Год журнала:
2025,
Номер
unknown
Опубликована: Янв. 1, 2025
Using
an
Ir(
iii
)-based
redox
mediator
([Ir(sppy)
3
]
3-
)
overcomes
the
traditional
kinetic
barrier
of
tri-
n
-propylamine
oxidation
on
BDD,
enhancing
ECL
from
Ru(
ii
)-labeled
beads
by
up
to
46-fold.
Analytical Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 6, 2025
Traditional
electrochemiluminescence
(ECL)
detection
makes
it
difficult
to
realize
the
spatial
separation
of
sensing
and
reporting
sides,
which
inevitably
causes
mutual
interference
between
target
luminescent
substance.
By
studying
relationship
luminol
luminescence
position
electrode
potential
in
a
three-electrode
system,
this
work
realized
sides
for
first
time.
Experimental
investigations
showed
that
only
emitted
ECL
signals
at
electrodes
with
positive
polarity,
regardless
whether
or
negative
voltage
was
applied.
Inspired
by
this,
we
introduced
carbon
vacancy-modified
iron
single-atom
catalyst
(VC-Fe-N-C
SAC)
excellent
oxygen
reduction
reaction
(ORR)
activity
into
working
electrode,
can
catalyze
dissolved
O2
produce
abundant
reactive
species
(ROS).
ROS
diffused
surface
counter
oxidize
high-intensity
signal
an
ultralow
trigger
potential.
As
proof-of-concept
application,
sensitive
biosensor
constructed
microcystin-LR
(MC-LR)
detection.
This
solved
substance
traditional
system
improved
accuracy
sensitivity.
Furthermore,
introduction
catalysts
(SAC)
avoided
use
coreactant
H2O2
tedious
electrochemical
oxidation
process
luminol,
broadened
application
biosensors.
Analytical Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 12, 2025
A
low
collision
frequency
and
an
insufficient
number
of
free
radicals
are
the
main
problems
leading
to
electroluminescence
(ECL)
efficiency
luminol
its
derivatives.
In
order
solve
above
issues,
this
work
used
nanoconfinement
combined
with
nanozyme
catalysis
significantly
enhance
ECL
efficiency.
We
assembled
isoluminol
(ILu)
into
hydrogen-bonded
organic
framework
HOF-14
prepared
a
novel
emitter
ILu/HOF-14
for
first
time.
Surprisingly,
compared
ILu/H2O2
system,
signal
ILu/HOF-14/H2O2
was
increased
by
33
times.
This
because
porous
structure
effectively
limited
movement
their
frequency.
Therefore,
reaction
rate
between
improved
achieve
amplification.
To
further
increase
radicals,
we
introduced
hybrid
Zn
SAC@CuO2
NPs
superior
peroxidase
(POD)-like
activity.
It
could
catalyze
coreactant
H2O2
produce
large
amount
ROS
(OH•
O2•-),
accelerating
ILu
improving
signal.
Based
on
research,
dual-mode
biosensing
imaging
platform
constructed
detect
microcystin-LR
(MC-LR).
nonspecific
trans-cleavage
activity
CRISPR-Cas12a
system
dynamic
continuity
amplification
capability
platform,
detection
sensitivity
broadening
avenues
molecular
diagnostic
strategies.
Analytical Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 15, 2025
Herein,
an
efficient
luminol-H2O2
electrochemiluminescence
(ECL)
system
with
bimetallic
organic
gels
as
ECL
signal
booster
and
innovative
heterosequence
aptamer
recognition
a
target
conversion
strategy
is
used
to
construct
sensitive
specific
aptasensor
for
the
detection
of
β2-microglobulin
(B2M),
key
biomarker
end-stage
renal
disease
(ESRD).
Impressively,
porous
Fe@Cu
(Fe@Cu
MOGs)
act
coreaction
accelerators
confinement-enhanced
reactors
system,
amplifying
by
21-fold
compared
traditional
which
greatly
enhanced
sensitivity
biosensor.
Compared
homosequence
approach
competitive
binding
aptamers
single
site,
synergistic
multiple
sites
could
improve
specificity
aptasensor,
validated
experiments
molecular
docking
simulations.
Therefore,
developed
exhibits
remarkable
dynamic
range
10
fg/mL-1
μg/mL
ultralow
limit
0.9
fg/mL,
superior
previously
reported
works.
Additionally,
demonstrated
consistent
performance
conventional
clinical
immunoturbidimetric
assays
high
B2M
concentration
in
14
samples,
well
exhibiting
trace
levels
that
are
undetectable
immunoturbidimetry.
This
offers
accurate
platform
recognition,
promising
applications
detection,
diagnosis,
therapeutic
monitoring,
advancing
scientific
research
on
early
pathological
changes
discovery.
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 16, 2025
Recently,
liquid|liquid
and
liquid|gas
interfaces
have
been
implicated
in
driving
unexpected
chemistries,
including
dramatic
rate
enhancement
spontaneous
redox
reactions.
Given
such
studies,
new
methods
are
necessary
to
observe
implicate
reactive
species.
Tris(2,2'-bipyridyl)ruthenium(II)
([Ru(bpy)3]2+)
is
a
common
luminophore
for
photoluminescence
electrochemiluminescence
(ECL)
studies.
In
this
work,
we
demonstrate
that
the
electro-oxidation
of
[Ru(bpy)3]2+
water
produces
light
without
addition
sacrificial
coreactants.
We
studied
by
confining
an
aqueous
droplet
adhered
both
tin-doped
indium
oxide
electrode
and,
separately,
glassy
carbon
inlaid
disc
macroelectrode
(d
=
3
mm).
also
generalized
method
observation
at
larger
electrodes.
The
intensity
higher
absence
O2,
diminishes
when
adding
H2O2,
disappears
presence
well-behaved,
one-electron
oxidant
(hexaammineruthenium(III)).
Our
results
indicate
powerful
reducing
agent
present
during
[Ru(bpy)3]2+.
This
least
energetic
enough
create
excited
state,
[Ru(bpy)3]2+*,
giving
minimum
energy
∼2
eV.
Chemiluminescence
persists
as
[Ru(bpy)3]3+
diffuses
into
solution,
indicating
strong
may
exist
natively
low
abundance.
These
observations
significant
fundamental
ramifications
because
they
elucidate
pathway
ECL
allow
real-time
visualization
highly
