Chemical Communications,
Год журнала:
2022,
Номер
58(50), С. 7034 - 7037
Опубликована: Янв. 1, 2022
The
origins
of
the
reactivity
strain-increase
allylborations
were
computationally
investigated.
low
vinylcyclopropyl
boronates
is
due
to
weak
electronic
interactions
between
benzaldehyde
and
allylboronates.
By
increasing
acidity
boron
center,
significantly
improved
because
stronger
stabilizing
O→B
interaction
effectively
compensates
for
destabilizing
steric
effects.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(19)
Опубликована: Март 11, 2024
Abstract
The
advanced
aqueous
zinc–ion
batteries
(AZIBs)
are
still
challenging
due
to
the
harmful
reactions
including
hydrogen
evolution
and
corrosion.
Here,
a
natural
small
molecule
acid
vitamin
C
(Vc)
as
an
electrolyte
additive
has
been
selectively
identified.
Vc
can
adjust
d
band
center
of
Zn
substrate
which
fixes
active
H
+
so
that
reaction
(HER)
is
restrained.
Simultaneously,
it
could
also
fine–tune
solvation
structure
ions
enhanced
electrostatics
reduced
Pauli
repulsion
verified
by
energy
decomposition
analysis
(EDA).
Hence,
cell
retains
ultra–long
cycle
performance
over
1300
cycles
superior
Coulombic
efficiency
(CE)
99.5
%.
prepared
full
cells
display
increased
rate
capability,
lifetime,
self–discharge
suppression.
Our
results
shed
light
on
mechanistic
principle
additives
improvement
ZIBs,
anticipated
render
new
round
studies.
ACS Catalysis,
Год журнала:
2022,
Номер
12(19), С. 11573 - 11585
Опубликована: Сен. 8, 2022
The
conversion
of
renewable
bioethanol
into
high-energy-density
higher
alcohols
has
become
essential
for
meeting
the
increasing
global
demand
to
achieve
carbon
neutrality.
In
this
study,
Zn-
and
nitrogen-codoped
Ni-based
lignin-derived
catalysts
(NiZn@NC)
were
prepared
by
solvent
volatile
self-assembly
in
situ
reductive
carbonization
using
pulp
paper
waste
stream
alkali
lignin
as
source.
Lignin
amphipathic
derivatives
with
−COOH
−NH2
groups
would
coordinate
metal
ions
form
a
stable
lignin–metal
framework;
thus,
layer
disperses
NiZn
bimetallic
catalyst
prevents
from
corroding.
At
an
amination
reagent/lignin
mass
ratio
1:2,
ethanol
75.2%
high
alcohol
yield
41.7%
achieved
over
Ni20Zn1@NC
catalyst.
Experimental
results
density
functional
theory
calculations
showed
that
Zn
doping
improved
electronic
environment
defect
structures
metallic
Ni
carrier,
which
effectively
inhibited
C–C
cleavage
suppressed
byproduct
formation,
such
methane.
Thereby,
synergetic
effect
between
facilitated
efficient
aqueous
Guerbet
reaction.
This
work
provides
strategy
pyrolytic
stabilizing
biomass
macromolecules
frameworks
construction
highly
active
cost-efficient
upgrading.
Catalysis Science & Technology,
Год журнала:
2022,
Номер
12(13), С. 4380 - 4387
Опубликована: Янв. 1, 2022
In
the
present
study,
mechanism
of
a
cobalt-catalyzed
hydroarylation
reaction
between
N
-pyridylindole
and
1,6-enynes
origin
its
stereoselectivity
have
been
systematically
investigated
using
DFT
calculation
method.
Physical Chemistry Chemical Physics,
Год журнала:
2021,
Номер
23(36), С. 20095 - 20106
Опубликована: Янв. 1, 2021
Quantum
chemical
activation
strain
analyses
reveal
that
asynchronicity
in
Diels–Alder
reactions
reduces
both
destabilizing
Pauli
repulsion
as
well
stabilizing
orbital
interactions,
and
occurs
if
the
former
dominates.
Inorganic Chemistry,
Год журнала:
2022,
Номер
61(18), С. 7130 - 7142
Опубликована: Апрель 25, 2022
A
mononuclear
uranyl
complex,
[UO2L]
(1),
has
been
synthesized
with
the
ligand
N,N'-bis(3-methoxy-2-hydroxybenzylidene)-1,6-diamino-3-azahexane
(H2L).
The
complex
showed
a
reversible
U(VI)/U(V)
redox
couple
in
cyclic
voltammetric
measurements.
reduction
potential
of
this
positive
shift
upon
addition
redox-inactive
alkali-
and
alkaline-earth
Lewis
acidic
metal
ions
(Li+,
Na+,
K+,
Ca2+,
Sr2+,
Ba2+)
to
an
acetonitrile
solution
1.
explained
on
basis
acidity
internal
electric-field
effect
respective
ions.
bimetallic
complexes
[UO2LLi(NO3)]
(2),
[UO2LNa(BF4)]2
(3),
[UO2LK(PF6)]2
(4),
[(UO2L)2Ca]·(ClO4)2·CH3CN
(5),
[(UO2L)2Sr(H2O)2]·(ClO4)2·CH3CN
(6),
[(UO2L)2Ba(ClO4)]·(ClO4)
(7)
have
also
isolated
solid
state
by
reacting
1
corresponding
characterized
single-crystal
X-ray
diffraction.
Density
functional
theory
calculations
optimized
[UO2LM]n+
used
rationalize
experimental
potentials
imposed
non-redox-active
cations.
The Journal of Organic Chemistry,
Год журнала:
2023,
Номер
88(15), С. 11102 - 11110
Опубликована: Июль 24, 2023
The
physical
factors
governing
the
catalysis
in
Lewis
acid-promoted
carbonyl-ene
reactions
have
been
explored
detail
quantum
chemically.
It
is
found
that
binding
of
a
acid
to
carbonyl
group
directly
involved
transformation
greatly
accelerates
reaction
by
decreasing
corresponding
activation
barrier
up
25
kcal/mol.
makes
process
much
more
asynchronous
and
transition
state
less
in-plane
aromatic.
remarkable
acceleration
induced
catalyst
ascribed,
means
strain
model
energy
decomposition
analysis
methods,
mainly
significant
reduction
Pauli
repulsion
between
key
occupied
π-molecular
orbitals
reactants
not
widely
accepted
stabilization
LUMO
enophile.
Angewandte Chemie,
Год журнала:
2024,
Номер
136(19)
Опубликована: Март 11, 2024
Abstract
The
advanced
aqueous
zinc–ion
batteries
(AZIBs)
are
still
challenging
due
to
the
harmful
reactions
including
hydrogen
evolution
and
corrosion.
Here,
a
natural
small
molecule
acid
vitamin
C
(Vc)
as
an
electrolyte
additive
has
been
selectively
identified.
Vc
can
adjust
d
band
center
of
Zn
substrate
which
fixes
active
H
+
so
that
reaction
(HER)
is
restrained.
Simultaneously,
it
could
also
fine–tune
solvation
structure
ions
enhanced
electrostatics
reduced
Pauli
repulsion
verified
by
energy
decomposition
analysis
(EDA).
Hence,
cell
retains
ultra–long
cycle
performance
over
1300
cycles
superior
Coulombic
efficiency
(CE)
99.5
%.
prepared
full
cells
display
increased
rate
capability,
lifetime,
self–discharge
suppression.
Our
results
shed
light
on
mechanistic
principle
additives
improvement
ZIBs,
anticipated
render
new
round
studies.
Green Chemistry,
Год журнала:
2023,
Номер
26(1), С. 353 - 361
Опубликована: Ноя. 21, 2023
This
work
reports
on
a
new
carbon-centered
radical
based
γ-valerolactone
(GVL)
that
can
activate
C(sp
3
)–H
bonds
and
has
application
potential
in
various
radical-mediated
reactions.