Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(34), P. 18931 - 18938
Published: Aug. 17, 2023
Interfacial
charge
transfer
on
the
surface
of
heterogeneous
photocatalysts
dictates
efficiency
reactive
oxygen
species
(ROS)
generation
and
therefore
aerobic
oxidation
reactions.
Reticular
chemistry
in
metal-organic
frameworks
(MOFs)
allows
for
rational
design
donor-acceptor
pairs
to
optimize
interfacial
charge-transfer
kinetics.
Herein,
we
report
a
series
isostructural
fcu-topology
Ni8-MOFs
(termed
JNU-212,
JNU-213,
JNU-214,
JNU-215)
with
linearly
bridged
bipyrazoles
as
organic
linkers.
These
crystalline
can
maintain
their
structural
integrity
7
M
NaOH
at
100
°C
24
h.
Experimental
studies
reveal
that
linker
engineering
by
tuning
electron-accepting
capacity
pyrazole-bridging
units
renders
these
significantly
improved
separation
under
visible-light
irradiation.
Among
them,
one
containing
benzoselenadiazole
unit
(JNU-214)
exhibits
best
photocatalytic
performance
benzylamines
conversion
rate
99%
Recycling
experiments
were
carried
out
confirm
stability
reusability
JNU-214
robust
catalyst.
Significantly,
systematic
modulation
bridging
donor-acceptor-donor
MOFs
provides
new
pathway
develop
viable
noble-metal-free
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(5), P. 3396 - 3404
Published: Jan. 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
Chemical Society Reviews,
Journal Year:
2024,
Volume and Issue:
53(18), P. 9378 - 9418
Published: Jan. 1, 2024
Organic
transformation
by
light-driven
catalysis,
especially,
photocatalysis
and
photothermal
denoted
as
photo(thermal)
is
an
efficient,
green,
economical
route
to
produce
value-added
compounds.
In
recent
years,
owing
their
diverse
structure
types,
tunable
pore
sizes,
abundant
active
sites,
metal-organic
framework
(MOF)-based
catalysis
has
attracted
broad
interest
in
organic
transformations.
this
review,
we
provide
a
comprehensive
systematic
overview
of
MOF-based
for
First,
the
general
mechanisms,
unique
advantages,
strategies
improve
performance
MOFs
are
discussed.
Then,
outstanding
examples
transformations
over
introduced
according
reaction
type.
addition,
several
representative
advanced
characterization
techniques
used
revealing
charge
kinetics
intermediates
presented.
Finally,
prospects
challenges
field
proposed.
This
review
aims
inspire
rational
design
development
materials
with
improved
catalysis.
ACS Applied Polymer Materials,
Journal Year:
2024,
Volume and Issue:
6(7), P. 3909 - 3917
Published: March 27, 2024
Donor–acceptor
covalent
organic
framework
(COF)
materials
have
proven
to
be
an
optimal
choice
for
heterogeneous
photocatalysis
due
their
capacity
effective
charge
separation
and
harvesting
of
visible
light.
The
poor
chemical
photostability
imine-linked
D–A
COFs
restrict
potential
broader
applications.
So,
researchers
are
focused
on
developing
with
enhanced
photocatalytic
activity.
In
this
study,
we
also
emphasize
the
pivotal
role
molecular
engineering
overcome
these
challenges.
Herein,
a
carbazole-based
highly
crystalline
CzDA-TAPT
COF
was
developed.
Not
only
does
incorporation
alkyl
group-substituted
carbazole
provide
excellent
donor
ability,
but
butyl
groups
in
pore
skeleton
guide
attachment
successive
layers
different
AB
stackings,
significantly
amplifying
efficiency
by
providing
more
active
sites
reaction.
Compared
previously
reported
photoactive
benzothiadiazole-based
COFs,
innovative
material
exhibits
superior
heightened
photostability,
resulting
notable
advancement
aerobic
oxidation
aryl
boronic
acids
phenols.