MOF-Based Frustrated Lewis Pairs: Expanding Horizons in Catalysis
Industrial & Engineering Chemistry Research,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 17, 2025
Language: Английский
Zeotype-Confined Frustrated Lewis Pair and Its Role in Catalyzing Hydrogenation
Journal of the American Chemical Society,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 22, 2025
Recent
theoretical
studies
predicted
that
the
frustrated
Lewis
pair
(FLP)
formed
by
carbonaceous
species
confined
in
zeolites/zeotypes
can
activate
H-H
and
C-H
bonds.
However,
there
still
lacks
experimental
evidence
understanding
on
role
of
FLP
hydrogenation
reaction.
Herein,
we
combined
experiments
density
functional
theory
(DFT)
calculations
to
demonstrate
Brønsted
acid
sites
with
weak
strength
transfer
H+
form
Si-O--Al
as
a
base
carbocation
acid.
They
are
electrostatically
attracted
sterically
repelled,
thus,
forming
sites.
We
present
for
first
time
general
principle
about
formation
inside
zeotypes
investigated
effect
topology
formation.
active
ethylene
hydrogenation,
their
activity
is
inversely
correlated
parent
strength.
derived
from
weaker
promotes
C2H4
adsorption
H2
activation,
thus
enhancing
hydrogenation.
This
work
not
only
provides
mechanistic
insights
into
origin
olefin
over
metal-free
but
also
offers
guidance
further
development
high-performance
zeolite/zeotype-based
catalysts
heterogeneous
catalysts.
Language: Английский
Constructing Robust Cu and P Lewis Acid-Base Pair Sites on Tubular G-C3n4 for Promoting Photocatalytic Reduction of Co2 to Ch4
Xianglin Li,
No information about this author
Shuangshuang Huai,
No information about this author
Shi-Jian Zhang
No information about this author
et al.
Published: Jan. 1, 2025
Language: Английский
Electrostatic Atlas of Noncovalent Interactions Built in Metal-Organic Frameworks
Published: Aug. 28, 2024
Noncovalent
interactions
form
the
basis
of
matter
and
life
yet
are
difficult
to
characterize.
Here
we
devised
a
platform
strategy
systematically
build
noncovalent
with
selective
chemical
groups
into
precisely
designed
configurations
by
using
metal-organic
frameworks
(MOF)
as
molecular
scaffold.
Using
vibrational
Stark
effect
benchmarked
against
computer
models,
found
electric
field
provides
unifying
metric
for
quantifying
diverse
in
MOFs
solutions.
By
synthetically
making
spectroscopically
testing
collection
nitrile
probe,
identified
stabilizing
fields
strong
-123
MV/cm
produced
additively
multiple
hydrogen
bonds,
an
unusual
destabilizing
+6
between
antiparallel
dipoles
,
anomalous
hydrogen-bond
blueshifts
large
34
cm-1,
unique
solvation
under
nanoconfinement.
This
method
opens
new
avenues
exploring
universe
interactions.
Language: Английский
Highly Efficient Organic Light‐emitting Diodes Based on Spatially Compacted π‐Stacked MR‐TADF Emitters
Guowei Chen,
No information about this author
Siwei Chen,
No information about this author
Yaozu Su
No information about this author
et al.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: April 18, 2025
Abstract
Organic
fluorophores
with
through‐space
donor/acceptor
interaction
have
garnered
significant
attention
for
their
unique
charge
transfer
properties
and
advanced
applications.
However,
use
in
luminescent
applications
is
hindered
by
challenges
such
as
low
luminescence
efficiency,
broad
emission
spectra.
Herein,
a
series
of
highly
emissive
thermally
activated
delayed
combining
boron‐based
multi‐resonance
acceptor
an
arylamine
donor
within
spatially
compacted
structure
designed
synthesized.
By
strategically
varying
spatial
compactness,
interactions
are
fine‐tuned,
enabling
precise
control
over
high‐lying
excited
states
characteristics
while
preserving
narrow‐spectrum
fluorescence.
Key
structural
optimizations,
including
planar
space‐compacting
methyl
group,
resulted
compact
configuration,
boosting
reverse
intersystem
crossing
rates
20‐fold
compared
to
the
parent
fluorophore.
This
design
minimizes
concentration‐induced
quenching
spectral
broadening,
yielding
superior
solid‐state
luminescence.
The
resulting
organic
light‐emitting
diodes
achieved
ultranarrow
electroluminescence
(full
width
at
half‐maximum
22
nm)
remarkable
external
quantum
efficiency
31.1%,
along
reduced
roll‐offs.
Language: Английский
Space Exploration of Metal–Organic Frameworks in the Mesopore Regime
Accounts of Chemical Research,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Dec. 13, 2024
ConspectusThe
past
decades
have
witnessed
the
proliferation
of
porous
materials
offering
high
surface
areas
and
revolution
in
gas
storage
separation,
where
metal–organic
frameworks
(MOFs)
stand
out
as
an
important
family.
Alongside
pursuit
higher
area,
increase
size
guests,
such
nanoparticles
biomolecules,
has
also
led
to
demand
for
larger
space
defined
by
pores
cages
within
MOF
structure,
from
conventional
micropore
regime
(<2
nm)
toward
mesopore
(2–50
nm).
Among
essential
elements
design
MOFs,
molecular
building
blocks,
their
coordination
spatial
arrangement,
chemistry
design,
bonds
become
relatively
mature,
precise
control
shape
environment
molecularly
3D
cages;
however,
correlation
between
geometrical
parameters
polyhedrons
describing
cages,
concerning
arrangement
is
much
less
explored.In
this
Account,
we
made
efforts
associate
actual
cage
with
critical
components,
vertices,
edges,
connectivity,
rings,
underlying
polyhedrons,
well
combination
components
various
types
MOFs.
Several
trends
were
found,
influence
connectivity
expansion
efficiency,
insights
into
construction
This
enables
creation
extremely
large
mesoporous
MOFs
internal
diameter
up
11.4
nm
small
blocks.
Furthermore,
discuss
a
strategy
partial
removal
or
replacement
organic
linkers
construct
readily
known
topologies.All
above
urged
us
ask
following
questions:
Is
there
any
limit
sculpting
molecules?
How
area
can
one
chemical
bond
support?
The
answer
these
questions
will
deepen
knowledge
efficient
utilization
spaces
guide
mesopores.
general
principals
emerged:
(1)
Expansion
efficiency
radius
are
positively
correlated
number
vertices.
(2)
Increase
vertices
decrease
favor
cages.
(3)
boundary
constructed
related
polyhedron
type
determined
energy
involved
crystallinity.
Such
likely
be
applicable
isolated
supramolecular
chemistry.
In
addition
structural
synthesis,
applications
summarized.
Language: Английский
Tri‐site Synergistic Cu(I)/Cu(II)─N Single‐Atom Catalysts for Additive‐Free CO2 Conversion
Qiuyan Cao,
No information about this author
Wenqiang Sun,
No information about this author
Zhihe Xiao
No information about this author
et al.
Small,
Journal Year:
2024,
Volume and Issue:
20(45)
Published: July 22, 2024
As
the
highly
stable
and
abundant
carbon
source
in
nature,
activation
conversion
of
CO
Language: Английский
Synthesis of Cyclic Carbonates by CO2 Cycloaddition with Epoxides: Recent Advances, Challenges and Perspectives
Decun Luo,
No information about this author
Zhun Hu,
No information about this author
Chun‐Ran Chang
No information about this author
et al.
Authorea (Authorea),
Journal Year:
2024,
Volume and Issue:
unknown
Published: Aug. 27, 2024
The
fixation
of
CO2
into
high-value
chemicals
has
emerged
as
a
critical
research
priority,
attracting
considerable
interest
from
both
academia
and
industry.
synthesis
cyclic
carbonates
via
the
cycloaddition
with
epoxides,
process
exhibiting
100%
atom
economy,
exemplifies
highly
desirable
reaction
aligned
principles
"green
chemistry"
"atomic
economy".
Cyclic
find
widespread
applications
in
lithium-ion
batteries,
pharmaceutical
manufacturing,
various
fine
chemical
industries.
This
review
provides
comprehensive
overview
recent
advances,
challenges,
perspectives
field
reactions.
Initially,
pathways
(CO2
activation,
epoxides
activation
dual
activation)
are
elucidated,
followed
by
an
in-depth
analysis
homogeneous
heterogeneous
catalysts.
Then,
paper
evaluates
suitability
batch
reactors,
continuous
flow
micro-pass
reactors
for
this
reaction.
Finally,
highlights
importance
developing
green
catalyst
capable
selectively
capturing
low-concentration
industrial
exhaust
gas
or
air
at
room
temperature
pressure,
converting
it
site.
insights
presented
offer
valuable
framework
roadmap
future
endeavors
field.
Language: Английский