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 Science,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 17, 2025
Abstract
Surface
defects
play
a
crucial
role
in
the
photophysical
properties
and
optoelectronic
applications
of
perovskite
materials.
Although
luminescent
efficiency
is
improved
through
post‐synthetic
defect
passivation,
comprehensive
optimization
photoluminescent
performance
via
chemistry
remains
significant
challenge.
Herein,
successful
engineering
strategy
demonstrated
toward
0D
[DADPA]PbBr
5
(DADPA
=
diaminodipropylamine)
single
crystal
to
achieve
multiple
adjustable
properties.
Through
fine‐tuning
crystallization
environment
diminish
Br
vacancy
(
V
),
displays
gradually
evolutionary
luminescence
range
from
broadband
blue‐white
narrow
green
light
emissions,
with
continuously
dominant
wavelengths
(445–535
nm)
linewidths
(134–27
nm).
Meanwhile,
quantum
yields
increase
significantly
3.7%
80.8%,
lifetime
extends
5.4
57.7
ns.
This
pioneering
discovery
for
simultaneous
modification
multi‐dimensional
performances.
Combined
spectroscopic
investigations
first‐principles
calculations
indicate
that
reducing
narrows
bandgap
inhibits
nonradiative
recombination,
which
attenuates
interband
trap‐state‐associated
emission
facilitates
formation
bound
exciton
enhanced
efficiency.
More
remarkably,
this
universal
can
be
extended
other
systems
similar
adjustability,
paving
way
diverse
perovskites
performance.
Abstract
A
poly‐phosphamide
(POP)
with
a
band
gap
of
2.8
eV
is
used
for
the
photochemical
conversion
CO
2
into
CH
4
and
chemical
organo‐epoxides
cyclic
carbonates.
The
Tauc
plot
Mott
Schottky
analyses
indicate
conduction
potential
at
−1.49
V
(vs
NHE),
much
more
negative
than
multi‐electron
reduction
lifetime
photo‐excited
electron
found
ns.
On
photoirradiation
420
nm
light,
POP
in
presence
triethanolamine
or
ascorbic
acid
can
selectively
convert
(≈99%)
yield
4.6
mmol
g
−1
.
visible‐light
irradiation,
drop
charge‐transfer
resistance
(R
ct
)
an
enhancement
cathodic
current
further
confirm
photon‐harvesting
efficiency
POP.
In
situ,
FTIR
study
identifies
adsorption
to
possible
reaction
intermediate,
like
*‐CO,
*‐CH
OH.
also
behaves
as
catalyst
carbonates
under
solvent‐free
conditions
98%
yield.
After
light‐phase
dark‐phase
reactions,
be
successfully
recycled
least
five
times
without
structural
degradation.
Herein,
acts
bi‐functional,
recyclable
polymeric
organic
material
essential
feedstocks
mild
conditions.
Enhancing
the
selectivity
of
photocatalytic
CO2
reduction
to
valuable
multicarbon
(C2+)
products
remains
a
significant
challenge
in
green
synthetic
chemistry.
Here,
we
present
dual-center
strategy
for
metal
oxides
that
boosts
photochemical
conversion
ethanol
by
regulating
coordination
number
and
oxygen
sites.
Notably,
CuO
catalysts
rich
low-coordinated
Cu–O
domains
have
achieved
nearly
perfect
(96.9%),
extraordinary
durability
(60
h),
superior
yield
rate
30.5
μmol·g–1·h–1,
surpassing
performance
many
existing
photocatalysts
water
vapor
CO2.
Density
functional
theory
calculations
operando
spectroscopic
results
provide
conclusive
evidence
tricoordinated
copper
(Cu3c)
increases
coverage
key
*CO
species,
while
bicoordinated
(O2c)
controls
migration
thereby
effectively
reducing
energy
requirement
dimerization
into
*OC–CO
intermediates
(ΔG*OC–CO
=
−0.56
eV)
pathway.
This
work
offers
insights
designing
exhibit
improved
C2+
fuels.
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
