Chemical Science,
Journal Year:
2022,
Volume and Issue:
13(9), P. 2528 - 2550
Published: Jan. 1, 2022
The
combination
of
electrochemiluminescence
and
semiconductor
gives
rise
to
a
rich
field
at
the
interface
photoelectrochemistry,
materials
analytical
chemistry.
It
offers
interesting
possibilities
for
ultrasensitive
(bio)detection,
imaging
light
conversion.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(12)
Published: Jan. 2, 2023
Facile
evaluation
of
oxygen
reduction
reaction
(ORR)
kinetics
for
electrocatalysts
is
critical
sustainable
fuel-cell
development
and
industrial
H2
O2
production.
Despite
great
success
in
ORR
studies
using
mainstream
strategies,
such
as
the
membrane
electrode
assembly,
rotation
electrodes,
advanced
surface-sensitive
spectroscopy,
time
spatial
distribution
reactive
species
(ROS)
intermediates
diffusion
layer
remain
unknown.
Using
time-dependent
electrochemiluminescence
(Td-ECL),
we
report
an
intermediate-oriented
method
analysis.
Owing
to
multiple
ultrasensitive
stoichiometric
reactions
between
ROS
ECL
emitter,
except
electron
transfer
numbers
rate
constants,
potential-dependent
were
successfully
obtained
first
time.
Such
exclusively
uncovered
information
would
guide
fuel
cells
production
with
maximized
activity
durability.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(16)
Published: Feb. 22, 2023
Here
we
report
on
a
label-free
electrochemiluminescence
(ECL)
microscopy
using
exceptionally
low
concentrations
of
the
[Ru(bpy)3
]2+
luminophore.
This
work
addresses
central
point
minimal
concentration
ECL
luminophore
required
to
image
single
entities.
We
demonstrate
possibility
record
images
cells
and
mitochondria
at
down
nM
pM.
is
7
orders
magnitude
lower
than
classically-used
corresponds
few
hundreds
luminophores
diffusing
around
biological
Yet,
it
produces
remarkably
sharp
negative
optical
contrast
images,
as
demonstrated
by
structural
similarity
index
metric
analyses
supported
predictions
covering
time.
Finally,
show
that
reported
approach
simple,
fast,
highly
sensitive
method,
which
opens
new
avenues
for
ultrasensitive
imaging
reactivity
molecule
level.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
61(14)
Published: Jan. 27, 2022
Abstract
Classical
electrochemical
characterization
tools
cannot
avoid
averaging
between
the
active
reaction
sites
and
their
support,
thus
obscuring
intrinsic
roles.
Single‐molecule
techniques
are
in
high
demand.
Here,
we
demonstrate
super‐resolution
imaging
of
Ru(bpy)
3
2+
based
reactions
on
Au
plates
using
single‐molecule
electrochemiluminescence
microscopy.
By
converting
signals
into
optical
signals,
manage
to
achieve
ultimate
sensitivity
single‐entity
chemistry,
that
is
directly
resolving
single
photons
from
individual
reactions.
High
spatial
resolution,
up
37
nm,
further
enables
mapping
chemical
activity
kinetics.
The
spatiotemporally
resolved
dynamic
structure–activity
relationship
shows
restructuring
catalysts
plays
an
important
role
determining
reactivity.
Our
approach
may
lead
gaining
new
insights
towards
evaluating
designing
electrocatalytic
systems.
Angewandte Chemie International Edition,
Journal Year:
2022,
Volume and Issue:
62(6)
Published: Dec. 7, 2022
Nanoconfinement
in
mesoporous
nanoarchitectures
could
dramatically
change
molecular
transport
and
reaction
kinetics
during
electrochemical
process.
A
molecular-level
understanding
of
nanoconfinement
mass
is
critical
for
the
applications,
but
a
proper
route
to
study
it
lacking.
Herein,
we
develop
single
nanoreactor
electrochemiluminescence
(SNECL)
microscopy
based
on
Ru(bpy)32+
-loaded
silica
nanoparticle
directly
visualize
situ
nanoconfinement-enhanced
reactions
at
molecule
level.
Meanwhile,
capability
nanoreactor,
reflected
as
long
decay
time
recovery
ability,
monitored
simulated
with
high
spatial
resolution.
The
effects
our
system
also
enable
imaging
proteins
cellular
membrane.
Our
SNECL
approach
may
pave
way
decipher
process,
build
bridges
between
potential
applications.
Analytical Chemistry,
Journal Year:
2022,
Volume and Issue:
94(13), P. 5441 - 5449
Published: March 21, 2022
Exploring
new
electrochemiluminescence
(ECL)
luminophores
with
high
ECL
efficiency
and
good
stability
in
aqueous
solution
is
great
demand
for
biological
sensing.
In
this
work,
highly
efficient
aggregation-induced
enhanced
of
cyanophenyl-functionalized
tetraphenylethene
(tetra[4-(4-cyanophenyl)phenyl]ethene,
TCPPE)
its
application
biothiols
analysis
were
reported.
TCPPE
contains
four
4-cyanophenyl
groups
covalently
attached
to
the
(TPE)
core,
generating
a
nonplanar
three-dimensional
twisted
conformation
structure.
nanoparticles
(NPs)
an
average
size
15.84
nm
prepared
by
precipitation
method.
High
(593%,
CdS
as
standard)
stable
emission
(over
one
month)
obtained
NPs
solution.
The
unique
properties
could
be
ascribed
suppression
nonradiative
transition,
decrease
energy
gap,
increase
anionic
radical
stability,
which
proved
theoretical
calculation
electrochemical
fluorescence
methods.
Contrasting
chromic
was
first
observed
NPs.
As
proof-of-methodology,
method
developed
three
biothiol
assays
detection
limits
6,
7,
300
nM
cysteine,
homocysteine,
glutathione,
respectively.
This
work
demonstrates
that
are
promising
luminophores,
incorporation
appropriate
substituents
into
can
improve
stability.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(31), P. 17420 - 17426
Published: July 27, 2023
Electrochemiluminescence
(ECL)
is
widely
employed
for
medical
diagnosis
and
imaging.
Despite
its
remarkable
analytical
performances,
the
technique
remains
intrinsically
limited
by
essential
need
an
external
power
supply
electrical
wires
electrode
connections.
Here,
we
report
electrically
autonomous
solution
leading
to
a
paradigm
change
designing
fully
integrated
all-optical
wireless
monolithic
photoelectrochemical
device
based
on
nanostructured
Si
photovoltaic
junction
modified
with
catalytic
coatings.
Under
illumination
light
ranging
from
visible
near-infrared,
photogenerated
holes
induce
oxidation
of
ECL
reagents
thus
emission
photons.
The
blue
easily
viewed
naked
eyes
recorded
smartphone.
A
new
scheme
introduced
where
energy
(2.82
eV)
higher
than
excitation
(1.18
via
intermediate
electrochemical
process.
In
addition,
mapping
activity
optical
microscopy
reveals
minority
carrier
interfacial
transfer
mechanism
at
nanoscale.
This
breakthrough
provides
strategy
generalizing
without
setups,
electrodes,
wiring
constraints,
specific
knowledge.
simplest
configuration
reported
so
far
opens
opportunities
develop
imaging
bioanalytical
systems
such
as
portable
point-of-care
sensing
devices.
