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,
Journal Year:
2024,
Volume and Issue:
136(42)
Published: July 20, 2024
Abstract
Selective
CO
2
photoreduction
to
value‐added
multi‐carbon
(C
2+
)
feedstocks,
such
as
C
H
4
,
holds
great
promise
in
direct
solar‐to‐chemical
conversion
for
a
carbon‐neutral
future.
Nevertheless,
the
performance
is
largely
inhibited
by
high
energy
barrier
of
C−C
coupling
process,
thereby
leading
products
with
low
selectivity.
Here
we
report
that
through
facile
surface
immobilization
1‐ethyl‐3‐methylimidazolium
tetrafluoroborate
(EMIM‐BF
ionic
liquid,
plasmonic
Cu
nanowires
could
enable
highly
selective
product.
At
an
optimal
condition,
resultant
photocatalyst
exhibits
production
selectivity
up
96.7
%
under
450
nm
monochromatic
light
irradiation,
greatly
surpassing
its
pristine
counterpart.
Combined
situ
spectroscopies
and
computational
calculations
unravel
addition
EMIM‐BF
liquid
modulates
local
electronic
structure
Cu,
resulting
enhanced
adsorption
strength
*CO
intermediate
significantly
reduced
process.
This
work
paves
new
path
plasmons
artificial
photosynthesis
targeted
products.
Angewandte Chemie International Edition,
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:
unknown
Published: July 20, 2024
Abstract
Selective
CO
2
photoreduction
to
value‐added
multi‐carbon
(C
2+
)
feedstocks,
such
as
C
H
4
,
holds
great
promise
in
direct
solar‐to‐chemical
conversion
for
a
carbon‐neutral
future.
Nevertheless,
the
performance
is
largely
inhibited
by
high
energy
barrier
of
C−C
coupling
process,
thereby
leading
products
with
low
selectivity.
Here
we
report
that
through
facile
surface
immobilization
1‐ethyl‐3‐methylimidazolium
tetrafluoroborate
(EMIM‐BF
ionic
liquid,
plasmonic
Cu
nanowires
could
enable
highly
selective
product.
At
an
optimal
condition,
resultant
photocatalyst
exhibits
production
selectivity
up
96.7
%
under
450
nm
monochromatic
light
irradiation,
greatly
surpassing
its
pristine
counterpart.
Combined
situ
spectroscopies
and
computational
calculations
unravel
addition
EMIM‐BF
liquid
modulates
local
electronic
structure
Cu,
resulting
enhanced
adsorption
strength
*CO
intermediate
significantly
reduced
process.
This
work
paves
new
path
plasmons
artificial
photosynthesis
targeted
products.
Small,
Journal Year:
2024,
Volume and Issue:
20(45)
Published: Aug. 15, 2024
Abstract
As
of
the
present
time,
in‐depth
study
structure‐activity
relationship
between
electronic
configuration
and
CO
2
photoreduction
performance
is
often
overlooked.
Herein,
a
series
Cu
x
species
modified
CeO
nanodots
are
constructed
in
situ
by
flame
spray
pyrolysis
(FSP)
to
achieve
an
efficient
photocatalytic
‐to‐C
conversion
with
electron
utilization
up
142.5
µmol
g
−1
.
Through
behavior
catalytic
pathways,
it
found
that
0
/Cu
+
coexistence
state
2+
can
optimize
energy
band
structure,
photocurrent
stability,
provide
kinetic
basis
for
active
surface
reaction
process
requires
multiple
electrons
into
C
products,
which
ultimately
enhances
H
6
3.8‐fold
4
5.2‐fold.
Besides,
able
regulate
choice
pathway,
enabling
transitions
This
work
indicates
optimization
effective
strategy
significantly
enhance
provides
new
ideas
design
synthesis
high‐performance
heterostructure
photocatalysts.
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.
