Advanced Optical Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 16, 2024
Abstract
Lead
halide
perovskite
nanocrystals
(NCs)
rapidly
emerge
as
promising
materials
for
photovoltaics.
However,
to
fully
harness
their
potential,
efficient
charge
extraction
is
crucial.
Despite
rapid
advancements,
the
specific
active
sites
where
acceptor
molecules
interact
remain
inadequately
understood.
Surface
chemistry
and
interfacial
properties
are
pivotal,
they
directly
impact
transfer
efficiency
overall
device
performance.
This
study
identifies
maps
binding
hole
transporters,
examining
influence
on
dynamics
through
ligand
engineering
with
2,3‐dimercaptopropanol
(DMP),
a
compound
strong
affinity
lead
(Pb).
DMP
effectively
passivates
Pb
in
CsPbBr
3
(CPB)
NCs,
enhancing
photoluminescence
(PL)
by
forming
stable
chelating
bonds.
DMP‐modified
CPB
nearly
completely
suppresses
─COOH‐functionalized
ferrocene
(FcA)
partially
─NMe
2
‐functionalized
(FcAm),
suggesting
an
alternative
pathway
FcAm.
further
supported
enhanced
bromine‐excess
(CPB‐Br(XS))
synthesized
via
SOBr
treatment.
The
distinct
interactions
validated
steady‐state
time‐resolved
PL,
along
transient
absorption
spectroscopy.
These
findings
underscore
role
of
strategic
NC‐charge
interactions,
enabling
better
extraction,
higher
solar
cell
efficiency,
reduced
toxicity
binding.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
unknown
Опубликована: Окт. 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,
Год журнала:
2024,
Номер
unknown
Опубликована: Май 29, 2024
Abstract
Selective
photocatalytic
reduction
of
CO
2
to
value‐added
fuels,
such
as
CH
4
,
is
highly
desirable
due
its
high
mass‐energy
density.
Nevertheless,
achieving
selective
with
higher
production
yield
on
p
‐block
materials
hindered
by
non‐ideal
adsorption
*CHO
key
intermediate
and
an
unclear
structure‐function
relationship.
Herein,
we
unlock
the
reaction
steps
found
a
volcano‐type
relationship
for
‐to‐CH
conversion
gradual
p‐
band
center
Bi
element
leading
formation
Bi‐oxygen
vacancy
heterosites.
The
selectivity
also
positive
correlation
energy
*CHO.
heterosites
appropriate
filled
Bi‐6
orbital
electrons
(−0.64)
enhance
coupling
between
C‐2
orbitals,
thereby
resulting
in
(95.2
%)
productivity
(17.4
μmol
g
−1
h
)
towards
.
Further
studies
indicate
that
synergistic
effect
reduces
Gibbs
free
*CO‐*CHO
process,
activates
C−H
C=O
bonds
*CHO,
facilitates
enrichment
photoexcited
at
active
sites
multielectron
conversion.
This
work
provides
new
perspective
developing
elements
Abstract
The
photocatalytic
reduction
of
CO
2
into
valuable
chemicals
and
fuels
has
become
a
significant
research
focus
in
recent
years
due
to
its
environmental
sustainability
energy
efficiency.
Metal
halide
perovskites
(MHPs),
renowned
for
their
remarkable
optoelectronic
properties
tunable
structures,
are
regarded
as
promising
photocatalysts.
Yet,
practical
uses
constrained
by
inherent
instability,
severe
electron–hole
recombination,
scarcity
active
sites,
prompting
substantial
efforts
optimize
MHP‐based
This
review
summarizes
the
latest
advancements
photocatalysis.
First
fundamental
principles
photocatalysis
outlined
structural
optical
characteristics
MHPs
evaluated.
Then
key
strategies
enhancing
MHP
photocatalysts,
including
morphology
surface
modification,
encapsulation,
metal
cation
doping,
heterojunction
engineering,
molecular
immobilization
highlighted.
Finally,
considering
progress
needs
industrial
application,
challenges
future
prospects
explored.
aims
support
researchers
development
more
efficient
stable
Advanced Optical Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Дек. 16, 2024
Abstract
Lead
halide
perovskite
nanocrystals
(NCs)
rapidly
emerge
as
promising
materials
for
photovoltaics.
However,
to
fully
harness
their
potential,
efficient
charge
extraction
is
crucial.
Despite
rapid
advancements,
the
specific
active
sites
where
acceptor
molecules
interact
remain
inadequately
understood.
Surface
chemistry
and
interfacial
properties
are
pivotal,
they
directly
impact
transfer
efficiency
overall
device
performance.
This
study
identifies
maps
binding
hole
transporters,
examining
influence
on
dynamics
through
ligand
engineering
with
2,3‐dimercaptopropanol
(DMP),
a
compound
strong
affinity
lead
(Pb).
DMP
effectively
passivates
Pb
in
CsPbBr
3
(CPB)
NCs,
enhancing
photoluminescence
(PL)
by
forming
stable
chelating
bonds.
DMP‐modified
CPB
nearly
completely
suppresses
─COOH‐functionalized
ferrocene
(FcA)
partially
─NMe
2
‐functionalized
(FcAm),
suggesting
an
alternative
pathway
FcAm.
further
supported
enhanced
bromine‐excess
(CPB‐Br(XS))
synthesized
via
SOBr
treatment.
The
distinct
interactions
validated
steady‐state
time‐resolved
PL,
along
transient
absorption
spectroscopy.
These
findings
underscore
role
of
strategic
NC‐charge
interactions,
enabling
better
extraction,
higher
solar
cell
efficiency,
reduced
toxicity
binding.
