ACS Measurement Science Au,
Год журнала:
2022,
Номер
3(1), С. 62 - 72
Опубликована: Ноя. 1, 2022
Characterizing
the
decomposition
of
electrogenerated
species
in
solution
is
essential
for
applications
involving
electrosynthesis,
homogeneous
electrocatalysis,
and
energy
storage
with
redox
flow
batteries.
In
this
work,
we
present
an
automated,
multiplexed,
highly
robust
platform
determining
rate
constant
chemical
reaction
steps
following
electron
transfer,
known
as
EC
mechanism.
We
developed
a
generation-collection
methodology
based
on
microfabricated
interdigitated
electrode
arrays
(IDAs)
variable
gap
widths
single
device.
Using
combination
finite-element
simulations
statistical
analysis
experimental
data,
our
results
show
that
natural
logarithm
collection
efficiency
linear
respect
to
width,
quantitative
used
determine
(kc).
The
integrated
IDA
method
series
experiments
measure
kc
values
between
∼0.01
100
s-1
aqueous
nonaqueous
solvents
at
concentrations
high
0.5
M
redox-active
species,
conditions
are
challenging
address
using
standard
methods
conventional
macroelectrodes.
versatility
approach
allows
characterization
wide
range
reactions
including
intermolecular
cyclization,
hydrolysis,
candidate
molecules
batteries
concentration
water
content.
Overall,
new
presents
straightforward
automated
assess
degradation
sufficient
flexibility
enable
high-throughput
workflows.
Advanced Materials,
Год журнала:
2022,
Номер
34(42)
Опубликована: Авг. 29, 2022
Electrocatalytic
oxidation
of
5-hydroxymethylfurfural
(HMF)
provides
an
efficient
way
to
obtain
high-value-added
biomass-derived
chemicals.
Compared
with
other
transition
metal
oxides,
CuO
exhibits
poor
oxygen
evolution
reaction
performance,
leading
high
Faraday
efficiency
for
HMF
oxidation.
However,
the
weak
adsorption
and
activation
ability
OH-
species
restricts
its
further
development.
Herein,
CuO-PdO
heterogeneous
interface
is
successfully
constructed,
resulting
in
advanced
onset-potential
(HMFOR),
a
higher
current
density
than
CuO.
The
results
open-circuit
potential,
situ
infrared
spectroscopy,
theoretical
calculations
indicate
that
introduction
PdO
enhances
capacity
organic
molecule.
Meanwhile,
promotes
species,
as
demonstrated
by
zeta
potential
electrochemical
measurements.
This
work
elucidates
enhancement
mechanism
interfaces
constructive
guidance
designing
multicomponent
electrocatalysts
electrocatalytic
reactions.
eScience,
Год журнала:
2022,
Номер
2(3), С. 243 - 277
Опубликована: Апрель 23, 2022
Compared
with
general
redox
chemistry,
electrochemistry
using
the
electron
as
a
potent,
controllable,
yet
traceless
alternative
to
chemical
oxidants/reductants
usually
offers
more
sustainable
options
for
achieving
selective
organic
synthesis.
With
its
environmentally
benign
features
gradually
being
uncovered
and
studied,
electrosynthesis
is
currently
undergoing
revival
becoming
rapidly
growing
area
within
synthetic
community.
Among
electrochemical
transformations,
anodically
enabled
ones
have
been
far
extensively
exploited
than
those
driven
by
cathodic
reduction,
although
both
approaches
are
conceptually
attractive.
To
stimulate
development
of
cathodically
reactions,
this
review
summarizes
recently
developed
reductive
electrosynthetic
protocols,
discussing
highlighting
reaction
features,
substrate
scopes,
applications,
plausible
mechanisms
reveal
recent
trends
in
area.
Herein,
reduction-enabled
preparative
transformations
categorized
into
four
types:
reduction
(1)
unsaturated
hydrocarbons,
(2)
heteroatom-containing
carbon-based
systems,
(3)
saturated
C-hetero
or
C–C
polar/strained
bonds,
(4)
hetero-hetero
linkages.
Apart
from
net
electroreductive
few
examples
photo-electrosynthesis
well
paired
electrolysis
also
introduced,
which
offer
opportunities
overcome
certain
limitations
improve
versatility.
The
electrochemically
driven,
transition
metal-catalyzed
cross-couplings
that
comprehensively
discussed
several
other
reviews
not
included
here.
SusMat,
Год журнала:
2022,
Номер
2(2), С. 114 - 141
Опубликована: Март 28, 2022
Abstract
The
need
for
large‐scale
electrochemical
energy
storage
devices
in
the
future
has
spawned
several
new
breeds
of
batteries
which
aqueous
zinc
ion
(AZIBs)
have
attracted
great
attention
due
to
their
high
safety,
low
cost,
and
excellent
performance.
In
current
research,
dendrite
corrosion
caused
by
electrolytes
are
main
problems
being
studied.
However,
research
on
metal
anode
is
still
its
infancy.
We
think
it
really
needs
provide
clear
guidelines
about
how
reasonably
configure
system
AZIBs
realize
high‐energy
density
long
cycle
life.
Therefore,
worth
analyzing
works
anode,
strategies
proposed
improve
stability
life
battery
recent
years.
Based
crystal
chemistry
interface
chemistry,
this
review
reveals
key
factors
essential
causes
that
inhibit
growth
side
reactions
puts
forward
potential
prospects
work
direction.
It
foreseeable
guiding
construction
with
various
systems
would
be
quite
possible
following
overview
as
a
roadmap.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(15), С. 6964 - 6971
Опубликована: Апрель 6, 2022
Merging
electrochemistry
with
asymmetric
catalysis
promises
to
provide
an
environmentally
friendly
and
efficient
strategy
for
the
construction
of
nonracemic
chiral
molecules.
However,
in
practice,
significant
challenges
arise
from
instability
or
incompatibility
catalysts
under
electrochemical
conditions
at
interface
electrode
solution.
Herein,
we
report
a
catalytic
indirect
electrolysis
employing
combination
redox
mediator
chiral-at-rhodium
Lewis
acid,
which
achieves
previously
elusive
enantioselective
nucleophilic
α-C(sp3)−H
alkenylation
ketones.
Specifically,
2-acyl
imidazoles
react
potassium
alkenyl
trifluoroborates
high
yields
(up
94%)
exceptional
enantioselectivities
(27
examples
≥99%
ee)
without
need
any
additional
stoichiometric
oxidants
(overall
40
examples).
The
new
electrosynthesis
can
be
scaled
gram
quantities
was
applied
straightforward
synthesis
intermediates
natural
product
cryptophycin
A
cathepsin
K
inhibitor.
Chemical Society Reviews,
Год журнала:
2023,
Номер
53(2), С. 566 - 585
Опубликована: Дек. 5, 2023
This
tutorial
review
explains
the
use
of
cyclic
voltammetry
and
chronoamperometry
to
interrogate
reaction
mechanisms,
optimize
electrochemical
reactions,
or
design
new
reactions.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(27)
Опубликована: Апрель 23, 2024
Homogeneous
electrocatalysts
can
indirect
oxidate
the
high
overpotential
substrates
through
single-electron
transfer
on
electrode
surface,
enabling
efficient
operation
of
organic
electrosynthesis
catalytic
cycles.
However,
problems
this
chemistry
still
exist
such
as
dosage,
difficult
recovery,
and
low
efficiency.
Single-atom
catalysts
(SACs)
exhibit
atom
utilization
excellent
activity,
hold
great
promise
in
addressing
limitations
homogeneous
catalysts.
In
view
this,
we
have
employed
Fe-SA@NC
an
advanced
redox
mediator
to
try
change
situation.
was
synthesized
using
encapsulation-pyrolysis
method,
it
demonstrated
remarkable
performance
a
range
reported
reactions,
construction
various
C-C/C-X
bonds.
Moreover,
potential
exploring
new
synthetic
method
for
electrosynthesis.
We
develop
electro-oxidative
ring-opening
transformation
cyclopropyl
amides.
reaction
system,
showed
good
tolerance
drug
molecules
with
complex
structures,
well
flow
electrochemical
syntheses
gram-scale
transformations.
This
work
highlights
SACs
electrosynthesis,
thereby
opening
avenue
chemistry.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(29)
Опубликована: Апрель 3, 2023
Abstract
The
organic‐carbon
core‐shell
structure
is
constructed
for
the
cathode
material
of
[
N
,
N'
‐bis(2‐anthraquinone)]‐perylene‐3,4,9,10‐tetracarboxydiimide
(PTCDI‐DAQ,
200
mAh
g
−1
)
through
an
interesting
strategy
called
surface
self‐carbonization.
As
expected,
core–shell
(PTCDI‐DAQ@C)
can
endow
PTCDI‐DAQ
outstanding
performance
in
Na‐ion
batteries.
In
half
cells
using
1
m
NaPF
6
/DME,
PTCDI‐DAQ@C
maintain
173
nearly
one
year,
while
quickly
decreases
from
203
to
121
only
after
100
cycles.
Meanwhile,
full
with
Na‐intercalated
hard
carbon
anode
deliver
peak
discharge
capacity
195
and
high
median
voltage
1.7
V
0.9–3.2
V,
corresponding
energy
densities
332
Wh
kg
184
total
mass
respectively.
Notably,
electrode
materials
include
very
cheap
elements
C,
H,
O,
N,
Na.
Furthermore,
also
show
impressive
high‐temperature
(197
at
50
°C)
subzero
(185/90
−10/−40
performances,
To
best
authors’
knowledge,
comprehensive
properties
are
results
based
on
organic
cathodes.
Green Chemistry,
Год журнала:
2023,
Номер
25(8), С. 3095 - 3102
Опубликована: Янв. 1, 2023
A
regiodivergent
electrochemical
defluorocarboxylation
of
gem
-difluorocyclopropanes
is
realized,
providing
access
to
branched
and
linear
carboxylated
monofluorinated
alkenes.
