Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(37)
Опубликована: Июль 6, 2022
Currently,
nitrogen
fertilizers
feed
half
of
the
global
population,
but
their
use
is
limited
by
energy
consumption
and
transportation.
Therefore,
it
important
to
study
photocatalysts
for
in
solar
fertilizers.
Herein,
a
new
type
graphene-embedded
Ce-based
UiO-66
(Ce-UiO-66)
photocatalyst
(GSCe)
investigated.
Ce-UiO-66
activated
breakage
benzene-C
bonds
formation
active
sites
ultraviolet
light
water.
Moreover,
embedding
graphene
effectively
controls
activation
improves
fixation.
GSCe
exhibited
remarkable
apparent
quantum
efficiency
(AQE)
9.25
%
stability
under
365
nm
with
solar-level
intensity.
also
performed
well
as
ammonia
fertilizer
crop
cultivation.
This
investigation
opens
up
opportunities
fixation
be
used
environmentally
friendly
RSC Sustainability,
Год журнала:
2023,
Номер
2(2), С. 265 - 287
Опубликована: Дек. 4, 2023
g-C
3
N
4
:
a
sustainable
game-changer
in
photocatalysis.
This
work
explores
synthesis,
properties,
mechanisms,
and
applications,
addresses
challenges,
charts
future
trends.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(9), С. 5074 - 5082
Опубликована: Фев. 24, 2023
Heterogeneous
photocatalysis
is
considered
as
an
ecofriendly
and
sustainable
approach
for
addressing
energy
environmental
persisting
issues.
Recently,
heterogeneous
photocatalysts
based
on
covalent
organic
frameworks
(COFs)
have
gained
considerable
attention
due
to
their
remarkable
performance
recyclability
in
photocatalytic
transformations,
offering
a
prospective
alternative
homogeneous
precious
metal/organic
dyes.
Herein,
we
report
Hex-Aza-COF-3
metal-free,
visible-light-activated,
reusable
photocatalyst
the
synthesis
of
2,3-dihydrobenzofurans,
pharmaceutically
relevant
structural
motif,
via
selective
oxidative
[3+2]
cycloaddition
phenols
with
olefins.
Moreover,
demonstrate
natural
products
(±)-conocarpan
(±)-pterocarpin
reaction
important
step
using
photocatalyst.
Interestingly,
presence
phenazine
hexaazatriphenylene
rigid
heterocyclic
units
strengthens
linkages,
enhances
absorption
visible
region,
narrows
band,
leading
excellent
activity,
charge
transport,
stability,
reactions,
evident
from
theoretical
calculations
real-time
information
ultrafast
spectroscopic
measurements.
Advanced Functional Materials,
Год журнала:
2024,
Номер
unknown
Опубликована: Март 10, 2024
Abstract
Covalent
organic
frameworks
(COFs)
attract
significant
attention
due
to
their
ordered,
crystalline,
porous,
metal‐free,
and
predictable
structures.
These
unique
characteristics
offer
great
opportunities
for
the
diffusion
transmission
of
photogenerated
charges
during
photocatalysis.
Currently,
a
considerable
number
COFs
are
used
as
metal‐free
semiconductor
photocatalysts.
This
review
aims
understand
relationships
between
structure
photocatalysis
performance
provides
in‐depth
insight
into
synthetic
strategy
improve
performance.
Subsequently,
focuses
on
structural
motif
in
sustainable
photocatalytic
hydrogen
evolution,
carbon
dioxide
reduction,
peroxide
generation,
compound
transformations.
Last,
conjunction
with
progress
achieved
challenges
yet
be
overcome,
candid
discussion
is
undertaken
regarding
field
COF
photocatalysis,
accompanied
by
presentation
potential
research
avenues
future
directions.
seeks
provide
readers
comprehensive
understanding
pivotal
role
robust
guidance
innovative
utilization
Journal of the American Chemical Society,
Год журнала:
2024,
Номер
146(5), С. 3396 - 3404
Опубликована: Янв. 24, 2024
Covalent
organic
frameworks
(COFs),
with
the
features
of
flexible
structure
regulation
and
easy
introduction
functional
groups,
have
aroused
broad
interest
in
field
photocatalysis.
However,
due
to
low
light
absorption
intensity,
photoelectron
conversion
efficiency,
lack
suitable
active
sites,
it
remains
a
great
challenge
achieve
efficient
photocatalytic
aerobic
oxidation
reactions.
Herein,
based
on
reticular
chemistry,
we
rationally
designed
series
three-motif
molecular
junction
type
COFs,
which
formed
dual
photosensitizer
coupled
redox
junctions
containing
multifunctional
COF
photocatalysts.
Significantly,
strong
adsorption
ability
units
integrated
reduction
features,
PY-BT
exhibited
highest
activity
for
oxidation.
Especially,
achieved
benzylamine
efficiency
99.9%
2.5
h,
is
much
higher
than
that
two-motif
only
one
or
unit
lacking
COFs.
The
mechanism
selective
was
studied
through
comprehensive
experiments
density
theory
calculations.
results
showed
photoinduced
electron
transfer
occurred
from
PY
then
triphenylamine
BT.
Furthermore,
thermodynamics
energy
lower
others,
confirmed
synergistic
effect
This
work
provided
new
strategy
design
COFs
also
represented
insight
into
catalytic
ACS Catalysis,
Год журнала:
2024,
Номер
14(7), С. 4581 - 4592
Опубликована: Март 12, 2024
The
integration
of
solar-driven
H2
evolution
with
the
selective
conversion
biomass-derived
alcohols
into
value-added
chemicals
has
gained
significant
attention
for
full
use
electrons
and
holes.
We
develop
a
dual-functional
photocatalyst
highly
oxidation
Cα–H
bond
benzyl
alcohol
to
C–C
coupled
products
(hydrobenzoin
deoxybenzoin),
in
cooperation
evolution,
using
point-to-face
interface
engineering
by
decorating
CdS
quantum
dots
on
Zn2In2S5
nanosheets
(CdS
QDs/Zn2In2S5
NS).
NS
exhibit
high
rate
13
mmol
g–1
h–1
formation
10.8
96.3%
selectivity.
Benzyl
achieves
91%
an
89%
yield
gram-scale.
introduction
enhances
interfacial
contact,
facilitating
efficient
spatial
separation
photogenerated
electron–hole
pairs
providing
active
sites
evolution.
In
situ
characterization
DFT
calculation
reveal
that
carbon-centered
radical
•CH(OH)C6H5,
generated
abstracting
alcohol,
is
reactive
intermediate
photocatalytic
process.
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(28)
Опубликована: Апрель 29, 2024
Abstract
The
synthesis
of
covalent
organic
frameworks
(COFs)
at
bulk
scale
require
robust,
straightforward,
and
cost‐effective
techniques.
However,
the
traditional
solvothermal
synthetic
methods
COFs
suffer
low
scalability
as
well
requirement
sensitive
reaction
environment
multiday
time
(2–10
days)
which
greatly
restricts
their
practical
application.
Here,
we
report
microwave
assisted
rapid
optimized
a
donor‐acceptor
(D−A)
based
highly
crystalline
COF,
TzPm‐COF
in
second
(10
sec)
to
minute
min)
scale.
With
increasing
from
seconds
minutes
crystallinity,
porosity
morphological
changes
are
observed
for
.
Owing
visible
range
light
absorption,
suitable
band
alignment,
exciton
binding
energy
(E
b
=64.6
meV),
can
efficaciously
produce
superoxide
radical
anion
(O
2
.−
)
after
activating
molecular
oxygen
eventually
drives
aerobic
photooxidative
amidation
with
high
recyclability.
This
photocatalytic
approach
works
variety
substituted
aromatic
aldehydes
having
electron‐withdrawing
or
donating
groups
cyclic,
acyclic,
primary
secondary
amines
moderate
yield.
Furthermore,
catalytic
mechanism
was
established
by
monitoring
real‐time
progress
through
situ
diffuse
reflectance
infrared
Fourier
transform
spectroscopic
(DRIFTS)
study.
