Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(34)
Published: July 3, 2023
Abstract
Herein,
we
report
a
one‐pot
method
for
enantioselective
C−H
allylation
of
pyridines
at
C3
via
tandem
borane
and
palladium
catalysis.
This
involves
borane‐catalyzed
pyridine
hydroboration
to
generate
dihydropyridines,
then
palladium‐catalyzed
the
dihydropyridines
with
allylic
esters,
finally
air
oxidation
allylated
afford
products.
enables
introduction
an
group
excellent
regio‐
enantioselectivities.
Chemical Reviews,
Journal Year:
2023,
Volume and Issue:
123(19), P. 11269 - 11335
Published: Sept. 26, 2023
Late-stage
functionalization
(LSF)
constitutes
a
powerful
strategy
for
the
assembly
or
diversification
of
novel
molecular
entities
with
improved
physicochemical
biological
activities.
LSF
can
thus
greatly
accelerate
development
medicinally
relevant
compounds,
crop
protecting
agents,
and
functional
materials.
Electrochemical
synthesis
has
emerged
as
an
environmentally
friendly
platform
transformation
organic
compounds.
Over
past
decade,
electrochemical
late-stage
(eLSF)
gained
major
momentum,
which
is
summarized
herein
up
to
February
2023.
Advanced Materials,
Journal Year:
2023,
Volume and Issue:
35(46)
Published: July 25, 2023
The
electrocatalytic
reduction
of
nitrate
(NO3-
)
to
nitrogen
(N2
is
an
environmentally
friendly
approach
for
efficient
N-cycle
management
(toward
a
nitrogen-neutral
cycle).
However,
poor
catalyst
durability
and
the
competitive
hydrogen
evolution
reaction
significantly
impede
its
practical
application.
Interface-chemistry
engineering,
utilizing
close
relationship
between
surface/interface
microenvironment
electron/proton
transfer
process,
has
facilitated
development
catalysts
with
high
intrinsic
activity
physicochemical
durability.
This
study
reports
synthesis
nitrogen-doped
carbon-coated
rice-like
iron
nitride
(RL-Fe2
N@NC)
electrocatalyst
excellent
nitrate-reduction
(high
N2
selectivity
(≈96%)
NO3-
conversion
(≈86%)).
According
detailed
mechanistic
investigations
by
in
situ
tests
theoretical
calculations,
strong
hydrogenation
ability
enhanced
enrichment
system
synergistically
contribute
rapid
nitrogen-containing
species,
increasing
reducing
occurrence
competing
hydrogen-evolution
side
reaction.
Moreover,
RL-Fe2
N@NC
shows
stability,
retaining
good
-to-N2
electrocatalysis
more
than
40
cycles
(one
cycle
per
day).
paper
could
guide
interfacial
design
Fe-based
composite
nanostructures
reduction,
facilitating
shift
toward
neutrality.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(45)
Published: June 16, 2023
Abstract
Electrochemistry
utilizes
electrons
as
a
potent,
controllable,
and
traceless
alternative
to
chemical
oxidants
or
reductants,
typically
offers
more
sustainable
option
for
achieving
selective
organic
synthesis.
Recently,
the
merger
of
electrochemistry
with
readily
available
electrophiles
has
been
recognized
viable
increasingly
popular
methodology
efficiently
constructing
challenging
C−C
C‐heteroatom
bonds
in
manner
complex
molecules.
In
this
mini‐review,
we
have
systematically
summarized
most
recent
advances
electroreductive
cross‐electrophile
coupling
(eXEC)
reactions
during
last
decade.
Our
focus
on
electrophiles,
including
aryl
alkyl
(pseudo)halides,
well
small
molecules
such
CO
2
,
SO
D
O.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(23), P. 8106 - 8125
Published: Jan. 1, 2023
This
tutorial
review
delves
into
the
unique
advantages
of
electrochemistry
in
context
asymmetric
catalysis,
first
providing
a
brief
introduction
to
electrosynthesis,
then
exploring
representative
case
studies
with
mechanistic
focus.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(23)
Published: April 3, 2023
Carboxylation
of
easily
available
alkenes
with
CO2
is
highly
important
to
afford
value-added
carboxylic
acids.
Although
dicarboxylation
activated
alkenes,
especially
1,3-dienes,
has
been
widely
investigated,
the
challenging
unactivated
1,n-dienes
(n>3)
remains
unexplored.
Herein,
we
report
first
skipped
dienes
via
electrochemistry,
affording
valuable
dicarboxylic
Control
experiments
and
DFT
calculations
support
single
electron
transfer
(SET)
reduction
its
radical
anion,
which
followed
by
sluggish
addition
SET
unstabilized
alkyl
radicals
carbanions
nucleophilic
attack
on
give
desired
products.
This
reaction
features
mild
conditions,
broad
substrate
scope,
facile
derivations
products
promising
application
in
polymer
chemistry.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(42)
Published: April 4, 2023
The
pyridine
moiety
is
an
important
core
structure
for
a
variety
of
drugs,
agrochemicals,
catalysts,
and
functional
materials.
Direct
functionalization
C-H
bonds
in
pyridines
straightforward
approach
to
access
valuable
substituted
pyridines.
Compared
the
direct
ortho-
para-functionalization,
meta-selective
far
more
challenging
due
inherent
electronic
properties
entity.
This
review
summarizes
currently
available
methods
meta-C-H
using
directing
group,
non-directed
metalation,
temporary
dearomatization
strategies.
Recent
advances
ligand
control
are
highlighted.
We
analyze
advantages
as
well
limitations
current
techniques
hope
inspire
further
developments
this
area.
