Molecules,
Journal Year:
2024,
Volume and Issue:
29(21), P. 5071 - 5071
Published: Oct. 26, 2024
Catalytic
technologies
are
pivotal
in
enhancing
energy
efficiency,
promoting
clean
production,
and
reducing
consumption
the
chemical
industry.
The
pursuit
of
novel
catalysts
for
renewable
is
a
long-term
goal
researchers.
In
this
work,
we
synthesized
three
two-dimensional
covalent
organic
frameworks
(COFs)
featuring
electron-rich
carbazole-based
architectures
evaluated
their
catalytic
performance
photocatalytic
reactions
electrocatalytic
oxygen
reduction
(ORRs).
Pyrene-functionalized
COF,
termed
as
FCTD-TAPy,
demonstrated
excellent
amino
oxidation
coupling
showed
remarkable
preference
substrates
with
electron-withdrawing
groups
(up
to
>99%
Conv.
Sel).
Furthermore,
FCTD-TAPy
favored
four-electron
transfer
pathway
during
ORR
exhibited
favorable
reaction
kinetics
(51.07
mV/dec)
high
turnover
frequency
(0.011
s−1).
contrast,
benzothiadiazole-based
FCTD-TABT
two-electron
pathway,
which
maximum
double-layer
capacitance
14.26
mF
cm−2,
Tafel
slope
53.01
mV/dec,
hydrogen
peroxide
generation
rate
70.3
mmol
g−1
h−1.
This
work
underscores
potential
COFs
advanced
materials
offers
new
insights
into
design
metal-free
enhanced
performance.
ACS Sustainable Chemistry & Engineering,
Journal Year:
2024,
Volume and Issue:
12(4), P. 1655 - 1665
Published: Jan. 17, 2024
For
environmentally
friendly
and
sustainable
development
demands,
visible-light-driven
oxidation
of
sulfides
has
become
one
the
most
popular
strategies
to
synthesize
functionalized
sulfoxides
degrade
mustard
gas
simulants.
Herein,
three
novel
polyoxometalate-based
covalent
triazine
frameworks,
SiW12-CTF
(1),
PW12-CTF
(2)
PMo12-CTF
(3)
(CTF
=
framework),
were
synthesized
via
hydrothermal
reaction
characterized
by
infrared
spectroscopy,
powder
X-ray
diffraction,
XPS
spectroscopy
UV–vis
DRS,
etc.
These
compounds
are
excellent
photocatalysts
for
selective
synthesis
various
as
well
degradation
2-chloroethyl
ethyl
sulfide
(CEES)
illuminated
a
10
W
425
nm
LED
in
an
O2
atmosphere.
Oxygen-rich
POMs
with
strong
electronegativity
modulate
electronic
structure
create
built-in
electric
field
POM-CTFs,
which
promotes
separation
migration
photogenerated
carriers.
Meanwhile,
encapsulation
POM
guests
into
CTF
induces
different
electron
transfer
behaviors,
resulting
photocatalytic
activities.
Specifically,
PW12-CTF,
visible-light-induced
methyl
phenyl
sulfide,
obtain
sulfoxide
yields
96%
88%
within
2
h,
respectively,
is
higher
than
(68%)
SiW12
(5%).
However,
exhibits
inferior
properties,
yield
35%
under
same
conditions.
The
in-depth
mechanism
reveals
that
process
dominated
O2•–
energy
induced
1O2
exist
system.
In
addition,
can
be
used
catalyze
sulfur-containing
maintains
boosted
structural
stability
catalytic
activity
after
reaction.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
unknown
Published: May 31, 2024
Abstract
Reactive
oxygen
species
(ROS)
play
a
crucial
role
in
determining
photocatalytic
reaction
pathways,
intermediate
species,
and
product
selectivity.
However,
research
on
ROS
regulation
polymer
photocatalysts
is
still
its
early
stages.
Herein,
we
successfully
achieved
series
of
modulations
to
the
skeleton
Pyrene‐alkyne‐based
(Tetraethynylpyrene
(TEPY))
conjugated
porous
polymers
(CPPs)
by
altering
linkers
(1,4‐dibromobenzene
(BE),
4,4′‐dibromobiphenyl
(IP),
3,3′‐dibromobiphenyl
(BP)).
Experiments
combined
with
theoretical
calculations
indicate
that
BE‐TEPY
exhibits
planar
structure
minimal
exciton
binding
energy,
which
favors
dissociation
followed
charge
transfer
adsorbed
O
2
produce
⋅O
−
.
Thus
shows
optimal
activity
for
phenylboronic
acid
oxidation
[3+2]
cycloaddition.
Conversely,
BP‐TEPY
significantly
distorted.
Its
conjugation
decreases,
intersystem
crossing
(ISC)
efficiency
increases,
makes
it
more
prone
resonance
energy
generate
1
Therefore,
displays
best
[4+2]
cycloaddition
thioanisole
oxidation.
Both
above
reactant
conversion
selectivity
exceed
99
%.
This
work
systematically
reveals
intrinsic
structure–activity
relationship
among
CPPs,
excitonic
behavior,
selective
generation
ROS,
providing
new
insights
rational
design
highly
efficient
CPPs
photocatalysts.
Journal of Materials Chemistry A,
Journal Year:
2024,
Volume and Issue:
12(32), P. 21156 - 21164
Published: Jan. 1, 2024
The
formation
of
heterojunctions
between
CeO
2
and
WO
2.72
reduces
the
band
gap.
Sample
–
x
wt%
shows
hydrophobicity
due
to
effective
shielding
4f
1
Ce
by
octet
electrons
in
outer
5s
5p
6
layer.
