Chemistry - A European Journal,
Год журнала:
2022,
Номер
28(66)
Опубликована: Сен. 6, 2022
Abstract
The
electrochemical
synthesis
of
fluorinated
allyl
silanes
and
boronates
was
disclosed.
addition
electrogenerated
boryl
or
silyl
radicals
onto
many
α‐trifluoromethyl
α‐difluoromethylstyrenes
in
an
undivided
cell
allowed
the
formation
a
large
panel
synthetically
useful
gem
‐difluoro
γ‐fluoroallyl
(64
examples,
from
31
%
to
95
yield).
In
addition,
scale
up
reactions
under
continuous
flow
showcased
using
reactor
with
promising
volumetric
productivity
(688
g.L
−1
.h
496
).
Moreover,
synthetic
utility
these
building
blocks
highlighted
through
versatile
transformations.
Finally,
plausible
reaction
mechanisms
were
suggested
explain
products.
ACS Catalysis,
Год журнала:
2023,
Номер
14(1), С. 45 - 55
Опубликована: Дек. 9, 2023
The
attention
toward
single-atom
catalysts
(SACs)
for
electrochemical
processes
is
growing
at
an
impressive
pace.
Electronic
structure
calculations
play
important
role
in
this
race
by
providing
proposals
of
potentially
relevant
based
on
screening
studies
or
the
identification
descriptors
chemical
activity.
So
far,
almost
all
these
predictions
ignore
a
crucial
aspect
design
catalyst:
its
stability.
We
propose
simple
yet
general
first-principles
approach
to
predict
stability
SACs
under
working
conditions
pH
and
applied
voltage.
This
construction
thermodynamic
cycle,
where
part
information
taken
from
experiment
rest
density
functional
theory
(DFT)
calculations.
In
particular,
we
make
use
formalism
Pourbaix
diagrams
investigate
reductive
oxidative
identify
those
that
show
pronounced
tendency
dissolve
form
other
species.
Applying
procedure
four
transition
metal
atoms,
Cr,
Mn,
Fe,
Co,
three
supports,
N-doped
graphene,
carbon
nitride,
covalent
organic
frameworks,
key
factor
determining
final
binding
energy
free
atom
support.
results
several
very
good
reactions
are,
fact,
dramatically
prone
dissolution
transformation
species,
suggesting
every
prediction
SAC's
catalytic
activity
should
be
accompanied
parallel
investigation
Chemical Society Reviews,
Год журнала:
2023,
Номер
52(21), С. 7305 - 7332
Опубликована: Янв. 1, 2023
Electrochemical
hydrogenation
reactions
hold
the
promise
of
more
sustainable
production
routes
for
towards
bulk
and
fine
chemicals.
Their
broad
applicability,
reactor
concepts,
achieved
milestones
future
perspectives
are
described
herein.
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.
Abstract
Single
atom
catalysts
(SACs)
consist
of
isolated
metal
atoms
stabilized
on
a
solid
support.
The
name
suggests
that
the
catalytic
activity
is
due
to
nature
atom,
but
course
interaction
with
substrate
plays
role
as
well.
But
what
more
important?
or
its
surrounding?
To
answer
this
question,
we
have
performed
numerical
experiments
based
density
functional
theory
(DFT).
24
transition
been
incorporated
in
Nitrogen‐doped
graphene,
and
hydrogen
evolution
reaction
(HER)
has
studied
changing
keeping
N‐doped
graphene
matrix
fixed.
Then,
one
specific
Pt,
embedded
same
nitrogen
neighbors
Pt
systematically
replaced
by
carbon
oxygen
generating
than
20
structures.
HER
thus
center
fixed
surrounding.
It
turns
out
great
variability
chemical
behavior
can
be
achieved
active
site
surrounding
environment.
This
shows
importance
local
coordination
determining
activity.
consequences
conclusion
for
modeling
studies
SACs
are
discussed.
Abstract
Oxygen
electrocatalysis
has
aroused
considerable
interest
over
the
past
years
because
of
new
energy
technologies
boom
in
hydrogen
and
metal–air
battery.
However,
due
to
sluggish
kinetic
four‐electron
transfer
process
oxygen
reduction
reaction
evolution
reaction,
electro‐catalysts
are
urgently
needed
accelerate
electrocatalysis.
Benefit
from
high
atom
utilization
efficiency,
unprecedentedly
catalytic
activity,
selectivity,
single‐atom
catalysts
(SACs)
considered
most
promising
candidate
replace
traditional
Pt‐group‐metal
catalysts.
Compared
with
SACs,
dual‐atom
(DACs)
attracting
more
attraction
including
higher
metal
loading,
versatile
active
sites,
excellent
activity.
Therefore,
it
is
essential
explore
universal
methods
approaching
preparation,
characterization,
elucidate
mechanisms
DACs.
In
this
review,
several
general
synthetic
strategies
structural
characterization
DACs
introduced
involved
discussed.
Moreover,
state‐of‐the‐art
electrocatalytic
applications
fuel
cells,
batteries,
water
splitting
have
been
sorted
out
at
present.
The
authors
hope
review
given
some
insights
inspiration
researches
about
electro‐catalysis.
Chemical Communications,
Год журнала:
2024,
Номер
60(24), С. 3226 - 3239
Опубликована: Янв. 1, 2024
This
feature
article
presents
an
overview
of
continuous
flow
chemistry,
including
photoflow
and
electroflow
technologies
in
the
preparation
active
pharmaceutical
ingredients
(APIs)
fine
chemical
intermediates.
