Precision Chemistry,
Год журнала:
2024,
Номер
2(11), С. 563 - 569
Опубликована: Авг. 24, 2024
Given
its
high
gravimetric
energy
density
and
status
as
a
clean
fuel
when
derived
from
renewables,
hydrogen
(H2)
is
considered
premier
candidate
for
storage;
however,
low
volumetric
limits
broader
application.
Chemical
storage
through
the
reversible
incorporation
of
H2
into
chemical
bonds
offers
promising
solution
to
density,
circumventing
subpar
densities
substantial
infrastructure
investments
associated
with
physical
methods.
Metal
hydrides
are
candidates
because
their
capacity
tunability
nanostructuring
alloying.
Moreover,
metal
hydride/H2
interconversion
may
be
interfaced
electrochemistry,
which
potential
solutions
some
challenges
traditional
thermochemical
platforms.
In
this
Perspective,
we
describe
anticipated
electrochemically
mediated
interconversion,
including
thermodynamic
efficiencies
hydride
formation,
sluggish
kinetics,
electrode
passivation.
Additionally,
propose
these
problems
design
molecular
mediators
that
control
factors
such
solubility,
particle
morphology,
affinity.
Realization
an
platform
introduces
new
tools
address
platforms
contributes
toward
development
room-temperature
Green Chemistry,
Год журнала:
2024,
Номер
26(4), С. 1846 - 1875
Опубликована: Янв. 1, 2024
Organocatalytic
enantioselective
cross-dehydrogenative
coupling
reaction
provides
a
great
opportunity
for
the
synthesis
of
highly
enantioenriched
molecules.
In
this
review,
recent
progress
in
field
is
summarized.
The Journal of Organic Chemistry,
Год журнала:
2024,
Номер
89(2), С. 1160 - 1174
Опубликована: Янв. 2, 2024
A
hypervalent
iodine(III)-mediated
cross-dehydrogenative
coupling
reaction
for
the
direct
formation
of
C–C,
C–N,
and
C–O
bonds
in
dihydroquinazolines
has
been
developed.
This
one-pot
method
allows
synthesis
C4-disubstituted
as
well
C4-spirolactam,
spirolactone,
spiroindene
moderate
to
high
yields.
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(46), С. 31420 - 31432
Опубликована: Ноя. 11, 2024
Hydride
abstraction
represents
a
promising
yet
underexplored
approach
in
the
functionalization
of
C-H
bonds.
In
this
work,
we
report
oxidation
α-C-H
bonds
ethers
via
oxoammonium
catalysis
using
3-chloroperbenzoic
acid
(
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(34), С. 15480 - 15487
Опубликована: Авг. 17, 2022
An
iridium-catalyzed
stereoselective
coupling
of
allylic
ethers
and
alkynes
to
generate
3,4-substituted
1,5-enynes
is
reported.
Under
optimized
conditions,
the
products
are
formed
with
excellent
regio-,
diastereo-,
enantioselectivities,
protocol
functional
group
tolerant.
Moreover,
we
report
conditions
that
allow
reaction
proceed
complete
reversal
diastereoselectivity.
Mechanistic
studies
consistent
an
unprecedented
dual
role
for
iridium
catalyst,
enabling
propargylic
deprotonation
alkyne
through
π-coordination,
as
well
generation
a
π-allyl
species
from
ether
starting
material.
The Journal of Organic Chemistry,
Год журнала:
2023,
Номер
88(6), С. 3954 - 3964
Опубликована: Март 7, 2023
A
novel
tandem
oxidative
Ritter
reaction/hydration/aldol
condensation
of
α-arylketones
with
substituted
propiolonitriles
has
been
developed.
This
protocol
conveniently
affords
a
wide
range
functionalized
3-acyl-3-pyrrolin-2-ones
through
the
efficient
construction
four
chemical
bonds,
C-N
bond,
C═C
and
two
C═O
formation
one
ring
bearing
an
aza-quaternary
center,
which
is
ascribed
to
strategical
introduction
nitriles
this
transformation.
reaction
mechanism
was
proposed
based
on
some
control
experiments.
Organic Letters,
Год журнала:
2022,
Номер
24(35), С. 6364 - 6368
Опубликована: Авг. 29, 2022
Secondary
alicyclic
amines
are
converted
to
α-aminonitriles
via
addition
of
TMSCN
their
corresponding
imines,
intermediates
that
produced
in
situ
the
oxidation
amine-derived
lithium
amides
with
simple
ketone
oxidants.
Amines
an
existing
α-substituent
undergo
regioselective
α'-cyanation
even
if
C-H
bonds
at
site
less
activated.
Amine
α-arylation
can
be
combined
generate
difunctionalized
products
a
single
operation.
Accounts of Chemical Research,
Год журнала:
2022,
Номер
55(23), С. 3537 - 3550
Опубликована: Ноя. 17, 2022
ConspectusThe
stereoselective
intermolecular
bond-forming
reactions
through
the
direct
manipulation
of
ubiquitous
yet
inert
C(sp3)–H
bonds
represent
an
important
and
long-standing
goal
in
chemistry.
In
particular,
developing
such
a
bimolecular
transformation
involving
carbocation
intermediates
generated
via
site-selective
hydride
abstraction
or
formal
by
organic
oxidants
would
avoid
preinstallation
directing
groups
is
therefore
attractive.
Hydride-abstraction-initiated
transformations
have
received
considerable
attention,
but
existing
examples
lack
studies.
Prevalent
studies
typically
suffer
from
narrow
substrate
scope
specific
highly
reactive
N-aryl
amines
diarylmethanes
together
with
limited
synthetic
utility.
This
Account
describes
our
recent
advances
development
application
hydride-abstraction-initiated
C–C
C–H
processes
significantly
expanded
scopes
structurally
diverse
N-acyl
ethers
nitriles,
esters,
perfluoroalkyl
moieties.We
first
explored
processes.
Utilizing
triarylmethyl
cations
oxoammonium
ions
as
abstractors,
we
accomplished
diastereoselective
oxidative
functionalization
range
organoboranes
components,
efficiently
installing
series
alkyl,
alkenyl,
aryl,
alkynyl
species
into
α-position
heteroatoms
good
levels
diastereocontrol.
Subsequently,
developed
"acetal
pool"
strategy
toolbox
to
regulate
stability
cationic
compatibility
delicate
asymmetric
catalysis
system.
this
strategy,
achieved
catalytic
enantioselective
alkenylation,
arylation,
alkynylation,
alkylation
heterocycles
boronates
components.
Simultaneously,
extended
ethers.
Notably,
method
allows
solvents
that
are
used
daily,
tetrahydrofuran,
tetrahydropyran,
diethyl
ether,
be
facilely
transformed
high-value-added
optically
pure
bioactive
molecules.
We
further
challenging
area
bond
adjacent
electron-donating
valuable
electron-withdrawing
functional
including
moieties
for
construction
single
vicinal
quaternary
carbon
stereocenters,
respectively.We
studied
processes,
known
redox
deracemization.
acetal
pool
reported
deracemization
cyclic
benzylic
Later,
disclosed
aerobic
one-pot
α-amino
acid
derivatives
excellent
group
compatibility.
tertiary
stereogenic
center
perfluoroalkyl,
cyano,
ester
moieties,
which
otherwise
difficult
construct.
