Angewandte Chemie,
Год журнала:
2024,
Номер
136(39)
Опубликована: Июль 2, 2024
Abstract
Photocatalytic
synthesis
of
H
2
O
is
an
advantageous
and
ecologically
sustainable
alternative
to
the
conventional
anthraquinone
process.
However,
achieving
high
conversion
efficiency
without
sacrificial
agents
remains
a
challenge.
In
this
study,
two
covalent
organic
frameworks
(COF−O
COF−C)
were
prepared
with
identical
skeletal
structures
but
their
pore
walls
anchored
different
alkyl
chains.
They
used
investigate
effect
chemical
microenvironment
pores
on
photocatalytic
production.
Experimental
results
reveal
change
hydrophilicity
in
COF−O,
leading
suppressed
charge
recombination,
diminished
transfer
resistance,
accelerated
interfacial
electron
transfer.
An
apparent
quantum
yield
as
10.3
%
(λ=420
nm)
can
be
achieved
through
oxygen
reduction
reaction.
This
among
highest
ever
reported
for
polymer
photocatalysts.
study
may
provide
novel
avenue
optimizing
activity
selectivity
generation.
Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Март 4, 2025
Abstract
Covalent
organic
frameworks
(COFs)
are
promising
for
photocatalytic
H₂O₂
generation.
However,
imine‐linked
COFs
often
suffer
from
poor
charge
separation
and
low
performance.
Therefore,
constructing
sp
2
carbon‐linked
with
extended
π‐conjugation
is
very
significant
in
boosting
the
properties,
but
their
synthesis
challenging
due
to
reversibility
of
C═C
bond.
Here,
two
vinylene‐linked
COFs:
BBT‐ACN
COF‐1
COF‐2
designed.
To
investigate
effects
different
structures
on
exciton
binding
energy
(
E
b
),
designed
possesses
a
Donor–Acceptor
(D–A)
structure
electron‐deficient
benzobisthiazole
(BBT)
as
acceptor
benzotrithiophene
donor,
while
latter
holds
π‐A
pyrene
π‐unit
BBT
acceptor.
Both
show
production
activity
two‐step
2e
−
oxygen
reduction
reaction
(ORR).
As
anticipated,
D–A
structured
exhibits
lower
value,
its
H
O
rate
pure
water
air
reaches
up
2.50
mmol
g⁻¹
h⁻¹,
≈3
times
higher
than
that
(0.91
h⁻¹).
This
study
reveals
fully
‐carbon‐linked
beneficial
production,
which
provides
an
effective
approach
designing
high‐performance
photocatalysts.
Nanoscale,
Год журнала:
2024,
Номер
16(34), С. 16015 - 16025
Опубликована: Янв. 1, 2024
We
computationally
screened
metal-single-atom
catalysts
(M-SAC)
on
carbon
nitride
for
selective
CO
2
reduction.
NiCN
significantly
lowered
the
rate-determining
potential
conversion
to
formic
acid
via
*OCHO
key
intermediate.
Catalysis Science & Technology,
Год журнала:
2024,
Номер
14(11), С. 3211 - 3218
Опубликована: Янв. 1, 2024
A
novel
anthracene-based
covalent
organic
framework
was
synthesized,
with
potential
application
for
white
light-induced
oxidative
coupling
of
amines
and
selective
oxidation
sulfides,
both
which
yielded
remarkable
conversion
selectivity.
Covalent
organic
frameworks
(COFs),
with
well-designed
structure
and
molecular
functionality
materials,
showed
great
promising
as
metal-free
catalysts
for
heterogeneous
photocatalysis.
Nevertheless,
the
influence
of
pore
COFs
on
photocatalytic
performances
is
always
neglected
in
ever
reports.
Herein,
by
rational
designation
topology
diagrams,
two-dimensional
porphyrin-based
(ETBA-por
COF
ETBC-por
COF)
different
sizes
were
synthesized
first
time.
Both
as-synthesized
exhibited
outstanding
crystallinity,
rich
micropores
high
surface
area.
Moreover,
also
have
similar
photoelectrochemical
efficaciously
production
superoxide
radical
anions
under
visible
irradiation.
To
test
effect
performances,
two
typical
characteristic
reactions
organics
transformation,
including
selective
aerobic
oxidation
sulfides
oxidative
amine
coupling
evaluated.
Interestingly,
although
both
good
recyclability
stability,
ETBA-por
smaller
size
has
higher
conversion
(94
%)
sulfoxides
selectivity
(>99
%),
while
things
reversed
imines
(99
%
substrate
96
yield
that
larger
size).
Mechanisms
activity
revealed
combing
experiments
simulation,
which
infers
suitable
molecules
accesses
critical
to
ensure
photocatalysis
performances.
This
study
confirmed
importance
efficient
transformation
organics.
