Angewandte Chemie,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 11, 2025
Abstract
The
arrangement
of
donor–acceptor
(D–A)
components
in
order
at
a
molecular
level
provides
means
to
achieve
efficient
electron‐hole
separation
for
promoting
the
activity
photocatalysts.
Herein,
we
report
coordination
assembly
D–A
molecules
with
desired
staggered
energy
levels
two
isostructural
metal‐organic
frameworks
(MOFs)
1
and
2
,
which
exhibit
high
photocatalytic
hydrogen
evolution
without
using
any
cocatalysts
photosensitizers.
modulation
active
metal
sites
MOFs
leads
an
increase
rates
from
1260
3218
µmol
h
−1
g
.
A
detailed
mechanism
study
revealed
that
bond
defined
by
assisted
centers
is
key
efficiently
generating
photogenerated
charge
carriers,
has
appropriate
affinity
proton
reduce
barrier
evolution.
Besides,
enhanced
transport
kinetics
based
on
arrayed
free
carboxyl
groups
hydrogen‐bonded
network
endows
higher
conductivity
than
thus
usage
rate
reaction
kinetics.
Metal-organic
frameworks
(MOFs)
are
crystalline
extended
structures
featuring
permanent
porosity,
assembled
from
metal
ions
and
organic
ligands,
often
synthesized
by
the
solvothermal
method
(50-260
°C,
12-72
h).
Here,
an
alternative
synthetic
approach-solvent-induced
structural
rearrangement
in
ultrasound-assisted
synthesis
is
presented.
Six
representative
Zn-based
MOFs,
each
composed
of
distinct
secondary
building
units,
within
2-180
min
consuming
less
solvent
(>0.03
m)
at
room
temperature.
It
observed
that
ultrasonication
induces
construction
a
coordination
network,
subsequent
exchange
triggers
to
yield
MOFs
high
crystallinity
porosity.
Furthermore,
scalability
this
demonstrated
through
bulk
MOF-5,
MOF-74,
ZIF-8,
MFU-4l
90
min.
The
initiation
nucleation
ultrasound
transformation
induced
offer
for
efficiently
synthesizing
bulk,
potentially
broadening
their
range
applications.
Angewandte Chemie International Edition,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 11, 2025
Abstract
The
arrangement
of
donor–acceptor
(D–A)
components
in
order
at
a
molecular
level
provides
means
to
achieve
efficient
electron‐hole
separation
for
promoting
the
activity
photocatalysts.
Herein,
we
report
coordination
assembly
D–A
molecules
with
desired
staggered
energy
levels
two
isostructural
metal‐organic
frameworks
(MOFs)
1
and
2
,
which
exhibit
high
photocatalytic
hydrogen
evolution
without
using
any
cocatalysts
photosensitizers.
modulation
active
metal
sites
MOFs
leads
an
increase
rates
from
1260
3218
µmol
h
−1
g
.
A
detailed
mechanism
study
revealed
that
bond
defined
by
assisted
centers
is
key
efficiently
generating
photogenerated
charge
carriers,
has
appropriate
affinity
proton
reduce
barrier
evolution.
Besides,
enhanced
transport
kinetics
based
on
arrayed
free
carboxyl
groups
hydrogen‐bonded
network
endows
higher
conductivity
than
thus
usage
rate
reaction
kinetics.
Efficient
and
selective
Li+
transport
within
the
nanochannel
is
essential
for
high-performance
solid-state
electrolytes
(SSEs)
in
lithium
metal
batteries.
Introducing
hopping
sites
into
SSEs
shows
great
potential
promoting
transport;
however,
it
typically
reduces
size,
consequently
increasing
energy
barrier
transport.
Herein,
we
present
a
molecular
defect
strategy
MOFs
to
introduce
increase
size
simultaneously
as
quasi-solid-state
(QSSEs).
Compared
with
defect-free
Li@UiO-66-based
QSSE,
optimized
Li@UiO-66-D2-based
QSSE
exhibits
remarkable
343%
enhancement
conductivity
improved
selectivity.
Furthermore,
9
cm
×
6
Li|Li@UiO-66-D2|LFP
pouch
cell
excellent
cycling
performance
high
capacity
retention.
An
in-depth
mechanism
study
has
unveiled
significant
impact
of
both
on
transport,
emphasizing
importance
enhancing
overall
MOF-based
QSSEs.
Angewandte Chemie,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 11, 2025
Abstract
The
arrangement
of
donor–acceptor
(D–A)
components
in
order
at
a
molecular
level
provides
means
to
achieve
efficient
electron‐hole
separation
for
promoting
the
activity
photocatalysts.
Herein,
we
report
coordination
assembly
D–A
molecules
with
desired
staggered
energy
levels
two
isostructural
metal‐organic
frameworks
(MOFs)
1
and
2
,
which
exhibit
high
photocatalytic
hydrogen
evolution
without
using
any
cocatalysts
photosensitizers.
modulation
active
metal
sites
MOFs
leads
an
increase
rates
from
1260
3218
µmol
h
−1
g
.
A
detailed
mechanism
study
revealed
that
bond
defined
by
assisted
centers
is
key
efficiently
generating
photogenerated
charge
carriers,
has
appropriate
affinity
proton
reduce
barrier
evolution.
Besides,
enhanced
transport
kinetics
based
on
arrayed
free
carboxyl
groups
hydrogen‐bonded
network
endows
higher
conductivity
than
thus
usage
rate
reaction
kinetics.
