Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Oct. 25, 2024
Abstract
Hybrid
lead
halides
show
significant
potential
in
photocatalysis
due
to
their
excellent
photophysical
properties,
but
the
atomically
precise
modification
of
organic
component
achieve
synergistic
interactions
with
halide
units
remains
a
great
challenge.
Herein,
for
first
time,
we
have
employed
crystal
engineering
strategy
construct
class
single‐atom‐substituted
hybrid
electron
donor‐acceptor
(D‐A)
effect.
The
frameworks
consist
1D
linear
[PbCl]
+
chains
as
inorganic
building
and
benzoxadiazole/benzothiadiazole/
benzoselenadiazole‐funtionalized
dicarboxylates
linkers.
covalent
bonding
between
ligands
electron−withdrawing
groups
electron‐rich
not
only
facilitate
charge
separation,
also
enhance
structural
robustness
that
is
critical
photocatalysis.
D‐A
structured
serve
highly
efficient
heterogeneous
photooxidation
catalysts,
including
aerobic
oxidation
C(sp
3
)−H
bonds,
oxidative
coupling
primary
amines,
phenylboronic
acids
selective
sulfides
are
demonstrated
30
examples.
Importantly,
these
reactions
able
be
driven
by
natural
sunlight
ambient
air
afford
quantitative
yields.
Moreover,
our
photocatalysts
successful
fix
into
photocatalytic
flow
system,
which
enables
flow‐type
synthesis
high
value‐added
products
on
gram
scale.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(29)
Published: May 15, 2024
Abstract
Lead
halide
molecular
ferroelectrics
represent
an
important
class
of
luminescent
ferroelectrics,
distinguished
by
their
high
chemical
and
structural
tunability,
excellent
processability
distinctive
characteristics.
However,
inherent
instability,
prone
to
decomposition
upon
exposure
moisture
light,
hinders
broader
ferroelectric
applications.
Herein,
for
the
first
time,
we
present
a
series
isoreticular
metal–organic
framework
(MOF)‐type
lead
demonstrating
exceptional
robustness
under
ambient
conditions
at
least
15
months
even
when
subjected
aqueous
boiling
conditions.
Unlike
conventional
metal‐oxo
secondary
building
units
(SBUs)
in
MOFs
adopting
highly
centrosymmetric
structure
with
limited
distortion,
our
halide‐based
occupy
structurally
deformable
[Pb
2
X]
+
(X=Cl
−
/Br
/I
)
SBUs
that
facilitate
c
‐axis‐biased
displacement
Pb
2+
centers
substantially
contribute
thermoinducible
transformation.
Importantly,
this
MOF‐type
undergo
ferroelectric‐to‐paraelectric
phase
transitions
remarkably
Curie
temperature
up
505
K,
superior
most
ferroelectrics.
Moreover,
covalent
bonding
between
phosphorescent
organic
component
light‐harvesting
inorganic
achieves
efficient
spin‐orbit
coupling
intersystem
crossing,
resulting
long‐lived
afterglow
emission.
The
compelling
combination
stability,
ferroelectricity
emission
exhibited
opens
many
potential
opportunities
energy‐conversion
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Jan. 1, 2024
Metal
oxides,
metal
sulfides,
MXenes,
and
metal–organic
frameworks
act
as
catalysts,
while
covalent
organic
frameworks,
carbon
nitrides,
phosphides,
graphene
oxides
serve
cocatalysts
for
CO
2
photoreduction
to
multicarbon
products.
Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(29)
Published: May 15, 2024
Abstract
Lead
halide
molecular
ferroelectrics
represent
an
important
class
of
luminescent
ferroelectrics,
distinguished
by
their
high
chemical
and
structural
tunability,
excellent
processability
distinctive
characteristics.
However,
inherent
instability,
prone
to
decomposition
upon
exposure
moisture
light,
hinders
broader
ferroelectric
applications.
Herein,
for
the
first
time,
we
present
a
series
isoreticular
metal–organic
framework
(MOF)‐type
lead
demonstrating
exceptional
robustness
under
ambient
conditions
at
least
15
months
even
when
subjected
aqueous
boiling
conditions.
Unlike
conventional
metal‐oxo
secondary
building
units
(SBUs)
in
MOFs
adopting
highly
centrosymmetric
structure
with
limited
distortion,
our
halide‐based
occupy
structurally
deformable
[Pb
2
X]
+
(X=Cl
−
/Br
/I
)
SBUs
that
facilitate
c
‐axis‐biased
displacement
Pb
2+
centers
substantially
contribute
thermoinducible
transformation.
Importantly,
this
MOF‐type
undergo
ferroelectric‐to‐paraelectric
phase
transitions
remarkably
Curie
temperature
up
505
K,
superior
most
ferroelectrics.
Moreover,
covalent
bonding
between
phosphorescent
organic
component
light‐harvesting
inorganic
achieves
efficient
spin‐orbit
coupling
intersystem
crossing,
resulting
long‐lived
afterglow
emission.
The
compelling
combination
stability,
ferroelectricity
emission
exhibited
opens
many
potential
opportunities
energy‐conversion
Nanoscale,
Journal Year:
2024,
Volume and Issue:
16(34), P. 16015 - 16025
Published: Jan. 1, 2024
We
computationally
screened
metal-single-atom
catalysts
(M-SAC)
on
carbon
nitride
for
selective
CO
2
reduction.
NiCN
significantly
lowered
the
rate-determining
potential
conversion
to
formic
acid
via
*OCHO
key
intermediate.
Angewandte Chemie International Edition,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 6, 2025
2D
covalent
organic
frameworks
(2D-COFs)
have
attracted
extensive
interest
in
solar
energy
to
hydrogen
conversion.
However,
insufficient
light
harvesting
and
difficult
exciton
dissociation
severely
limit
the
improvement
of
photocatalytic
activity
for
COFs,
thereby
impeding
progression
this
advanced
field.
In
work,
two
benzobisoxazole-bridged
fully
conjugated
2D-COFs
with
triazine
(COF-JLU44)
pyrene
(COF-JLU45)
units
were
constructed
first
time
via
Knoevenagel
polycondensation,
they
hold
long-range
ordered
structures,
largely
acceptable
surface
area,
fascinating
photoelectric
properties.
Significantly,
COF-JLU45
exhibits
an
impressive
evolution
rate
272.5
mmol
g-1
h-1
superior
reusability
presence
1.0
wt%
Pt
under
irradiation,
coupled
a
remarkable
apparent
quantum
yield
12.9%
at
long
wavelength
600
nm.
Multiple
spectroscopy
theoretical
simulation
demonstrate
ingenious
design
widen
its
absorption
effectively
promote
dissociation.
This
finding
contributes
valuable
insights
constructing
metal-free
photocatalysts
conversion
utilization.
