ACS Applied Materials & Interfaces,
Год журнала:
2023,
Номер
15(29), С. 35052 - 35061
Опубликована: Июль 12, 2023
Lanthanide-organic
frameworks
(LnOFs)
are
a
class
of
promising
catalysts
on
large
number
organic
reactions
because
the
higher
coordination
Ln3+
ions,
inspired
by
which
exploratory
preparation
cluster-based
LnOFs
was
carried
out
us.
Herein,
exquisite
combination
spindly
[Ln5(μ3-OH)6(CO2)6(H2O)6]
clusters
(abbreviated
as
{Ln5})
and
fluorine-functionalized
tetratopic
ligand
2',3'-difluoro-[p-terphenyl]-3,3″,5,5″-tetracarboxylic
acid
(F-H4PTTA)
engendered
two
highly
robust
isomorphic
nanoporous
{[Ln5(FPTTA)2(μ3-OH)6(H2O)6](NO3)}n
(NUC-61,
Ln
=
Ho
Dy).
NUC-61
compounds
rarely
reported
{Ln5}-based
3D
with
nano-caged
voids
(19
Å
×
17
Å),
shaped
twelve
[Ln5(μ3-OH)6(COO)8]
eight
completely
deprotonated
F-PTTA4-
ligands.
Activated
NUC-61a
characterized
plentiful
coexisted
Lewis
acid-base
sites
open
LnIII
sites,
capped
μ3-OH,
-F.
Judged
ideal
adsorbed
solution
theory
(IAST),
activated
NUC-61Ho-a
had
high
CO2/CH4
adsorptive
selectivity
value
12.7
(CO2/CH4
50/50)
9.1
5/95)
at
298
K,
could
lead
to
high-purity
CH4
(≥99.9996%).
Furthermore,
catalytic
experiments
exhibited
that
NUC-61Ho-a,
representative,
efficiently
catalyze
cycloaddition
CO2
epoxides
well
Knoevenagel
condensation
aldehydes
malononitrile.
This
work
proves
skeletons
chemical
stability,
heterogeneity,
recyclability
an
excellent
bifunctional
catalyst
for
some
reactions.
Chemical Society Reviews,
Год журнала:
2023,
Номер
52(22), С. 8005 - 8058
Опубликована: Янв. 1, 2023
Afterglow
materials
have
attracted
widespread
attention
owing
to
their
distinctive
and
long-lived
optical
emission
properties
which
create
exciting
opportunities
in
various
fields.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(19)
Опубликована: Март 18, 2023
Abstract
The
excited‐state
tuning
of
luminescent
metal–organic
compounds
has
made
great
progress
in
the
fields
optical
imaging,
photocatalysis,
photodynamic
therapy,
light‐emitting
devices,
sensors,
and
so
on.
Although
with
high
luminescence
efficiency
can
be
realized
via
enhanced
molecular
rigidity
heavy‐atom
effect,
their
corresponding
lifetimes
are
still
limited
on
order
a
nanosecond
to
millisecond,
owing
inherent
competition
between
luminous
lifetime.
Therefore,
advanced
applications
(i.e.,
persistent
afterglow
information
security,
anti‐counterfeiting,
smart
materials,
among
others)
related
long
(LPL,
typically
lifetime
larger
than
millisecond)
seriously
hindered.
This
review
gives
timely
systematic
summary
for
realizing
room‐temperature
phosphorescence
(RTP)‐type
thermally
activated
delayed
fluorescence
(TADF)‐type
LPL
during
last
few
years.
Particularly,
based
perspectives
time,
space,
energy
dimensions,
fundamental
materials
design
coordination
assembly
systematically
described
first
time.
Moreover,
internal
external
factors
influencing
properties
terms
efficiency,
lifetime,
color
illustrated.
Last
but
not
least,
challenges
also
discussed
developing
from
compounds.
Abstract
Circularly
polarized
luminescence
(CPL)
originates
from
the
chiral
emissive
excited
states.
CPL
materials
have
promising
applications
in
3D
optical
displays,
encryptions,
biological
probes,
photoelectric
devices,
and
switches,
most
of
which
require
excellent
performances
including
bright
high
dissymmetry
factor
(
g
lum
)
agglomerate
state.
This
review
systematically
summarizes
progress
about
aggregate
solid
materials,
such
as
organic
metal‐organic
(such
coordination
polymers,
organic‐inorganic
metal
halides,
clusters,
cluster‐assembled
materials),
assembled
by
supramolecular
interactions,
liquid
crystals.
We
also
present
current
challenges
a
future
perspective
emitting
materials.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(39)
Опубликована: Июль 12, 2022
Realizing
efficient
and
ultralong
room-temperature
phosphorescence
(RTP)
is
highly
desirable
but
remains
a
challenge
due
to
the
inherent
competition
between
excited
state
lifetime
photoluminescence
quantum
yield
(PLQY).
Herein,
we
report
bottom-up
self-assembly
of
transparent
metal-organic
framework
(MOF)
bulk
glasses
exhibiting
direct
all-phosphorescence
(lifetime:
630.15
ms)
with
PLQY
up
75
%
at
ambient
conditions.
These
macroscopic
MOF
have
high
Young's
modulus
hardness,
which
provide
rigid
environment
reduce
non-radiative
transitions
boost
triplet
excitons.
Spectral
technologies
theoretical
calculations
demonstrate
directly
derived
from
different
states,
indicating
great
capability
for
color-tunable
afterglow
emission.
We
further
developed
information
storage
light-emitting
devices
based
on
pure
RTP
fabricated
photonic
glasses.
Advanced Functional Materials,
Год журнала:
2023,
Номер
33(20)
Опубликована: Фев. 20, 2023
Abstract
Circularly
polarized
luminescence
(CPL)
materials
have
received
increasing
attention
in
recent
years.
Amongst
various
CPL
materials,
circularly
phosphorescence
(CPP)
featuring
long
life‐time
represent
a
novel
research
frontier
and
exhibit
promising
applications
fields.
Herein,
the
state‐of‐the‐art
advances
of
CPP
are
systematically
summarized,
as
classified
into
transition
metal
complexes,
organic
small
molecules,
polymers,
organic/inorganic
hybrid
materials.
Besides,
light‐emitting
diodes
encryption
display
also
summarized.
Furthermore,
current
challenges
future
perspectives
put
forward.
It
is
expected
that
this
review
will
offer
more
inspirations
for
rational
design
advanced
thus
further
promoting
their
practical
applications.
ACS Applied Materials & Interfaces,
Год журнала:
2022,
Номер
14(16), С. 18589 - 18599
Опубликована: Апрель 13, 2022
Stable
metal-organic
frameworks
containing
periodically
arranged
nanosized
pores
and
active
Lewis
acid-base
sites
are
considered
as
ideal
candidates
for
efficient
heterogeneous
catalysis.
Herein,
the
exquisite
combination
of
[Y2(CO2)7(H2O)2]
cluster
(abbreviated
{Y2})
multifunctional
linker
2,4,6-tri(2,4-dicarboxyphenyl)pyridine
(H6TDP)
led
to
a
nanoporous
framework
{[Y2(TDP)(H2O)2]·5H2O·4DMF}n
(NUC-53,
NUC
=
North
University
China),
which
is
rarely
reported
binuclear
three-dimensional
(3D)
with
hierarchical
tetragonal-microporous
(0.78
nm)
octagonal-nanoporous
(1.75
channels.
The
inner
walls
these
channels
aligned
by
{Y2}
clusters
plentifully
coexisted
YIII
ions
Npyridine
atoms.
Furthermore,
NUC-53
has
quite
large
void
volume
∼65.2%,
significantly
higher
than
most
documented
3D
rare-earth-based
MOFs.
performed
catalytic
experiments
exhibited
that
activated
showed
high
activity
on
cycloaddition
reactions
CO2
styrene
oxide
under
mild
conditions
excellent
turnover
number
(TON:
1980)
frequency
(TOF:
495
h-1).
Moreover,
deacetalization-Knoevenagel
condensation
benzaldehyde
dimethyl
acetal
malononitrile
could
be
efficiently
prompted
catalyst
NUC-53.
These
findings
not
only
pave
way
construction
MOF
based
rare-earth
variety
activities
but
also
provide
some
new
insights
into
mechanism.
Inorganic Chemistry,
Год журнала:
2022,
Номер
61(51), С. 21107 - 21114
Опубликована: Дек. 16, 2022
The
design
of
white-light
phosphor
is
highly
desirable
for
practical
applications
in
SSL
(solid-state
lighting)
and
its
related
fields.
Dye-loaded
metal-organic
frameworks
(MOFs)
have
been
widely
demonstrated
as
one
type
promising
down
conversion
materials
WLEDs
(white-light-emitting
diodes),
but
two
issues
(dye
leakage
inadequate
quantum
efficiency)
require
to
be
addressed
before
possible
applications.
Here,
a
series
single-phase
dyes@In-MOF
phosphors
prepared
different
ways:
the
in-situ
process
soaking
method.
study
these
confirms
importance
this
that
could
effectively
increase
dye
loading
efficiency
greatly
decrease
leakage.
As
result,
perfect
WLED,
fabricated
using
in-situ-synthesized
(AF/RhB@In-MOF)-3
(AF:
Acriflavine;
RhB:
Rhodamine
B)
450
nm
blue
LED
chip,
exhibited
very
high
yield
(QY,
up
42.27%),
luminous
efficacy
(LE)
50.75
lm/W,
color
rendering
index
(CRI)
91.2,
nearly
identical
Commission
International
ed'Eclairage
(CIE)
coordinates
(0.33,0.31),
indicating
potential
application
dye-loaded
MOFs
with
good
quality
smart
white
LEDs.
Abstract
The
development
and
applications
of
materials
with
efficient
circularly
polarized
luminescence
(CPL)
have
become
an
interdisciplinary
frontier
research
topic.
We
summarize
herein
the
recent
advance
in
CPL‐active
aggregates
based
on
metal‐ligand
coordination
(termed
as
“coordination
aggregates”).
surveyed
are
classified
small‐molecular
metal
complexes,
which
include
monocomponent
assemblies
Pt(II)
complexes
other
binary
helicates,
polymers,
frameworks.
efforts
improving
dissymmetry
factors
quantum
yields
these
use
aggregation
strategy
enhancing
performance
isolated
molecules
discussed.
chiral
organic
light‐emitting
diodes
(OLEDs)
solution‐
or
evaporation‐processed
procedures
surveyed.
In
addition,
uses
lanthanide
CPL‐contrast
imaging
CPL
probes
highlighted.
common
discussion
mechanism
aggregation‐enhanced
CPLs
a
perspective
future
works
finally
given.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(21), С. 9380 - 9389
Опубликована: Май 20, 2022
Three
achiral
polycyclic
aromatic
fluorophores─namely,
1-pyrenecarboxylic
acid,
9-anthracenecarboxylic
and
perylene-3,9-dicarboxylic
acid─were
chosen
based
on
their
desired
properties
before
being
incorporated
into
the
construction
of
a
K+-carrying
gamma-cyclodextrin
(γ-CD)-based
metal–organic
framework
(CD-MOF-1)
γ-CD-containing
hybrid
frameworks
(CD-HFs).
Among
these
fluorophores,
only
pyrene-carrying
one
shows
significant
noncovalent
bonding
interactions
with
γ-CD
in
solution.
This
fluorophore
is
encapsulated
CD-HF
trigonal
superstructure
instead
common
cubic
CD-MOF-1
found
case
other
two
fluorophores.
Single-crystal
X-ray
diffraction
analysis
reveals
π-stacked
chiral
positioning
inside
(γ-CD)2
tunnels
held
uniformly
around
an
enantiomorphous
32
screw
axis
along
c
direction
solid-state
structure.
helix-like
structure
demonstrates
additional
level
chirality
over
above
point-chiral
stereogenic
centers
axial
associated
self-assembled
These
arrangements
result
specifically
generated
photophysical
chiroptical
properties,
such
as
controlled
emergence
circularly
polarized
luminescence
(CPL)
emission.
In
this
manner,
complete
understanding
mechanism
transfer
from
host
(CD-HF)
to
has
been
achieved,
attribute
which
often
missing
development
materials
CPL.