ACS Catalysis,
Год журнала:
2023,
Номер
13(16), С. 11104 - 11116
Опубликована: Авг. 7, 2023
Hydroxyl
radicals
(OH•),
as
one
of
the
most
highly
oxidizing
oxidants,
are
difficult
to
utilize
in
chemical
synthesis
since
they
usually
cause
unavoidable
oxidative
damage
with
CO2
released.
Here,
a
Co–N–C
nanomaterial
composed
CoN4
sites
on
graphitic
carbon
nitride
was
constructed,
which
fulfills
self-cascade
activation
O2
water,
wherein
OH•
is
guided
generate
controlled
level
and
exerts
selective
oxidation
role
for
efficient
variety
organic
acids
by
furan
alcohols,
aromatic
fatty
alcohols
under
mild
conditions.
5-Hydroxymethylfurfural
(HMF)
reached
>99.9%
conversion
94.2%
yield
2,5-furandicarboxylic
acid
(FDCA)
at
25
°C
atmospheric
pressure.
This
study
allows
promising
utility
low
energy-consuming
way
independent
light
or
electricity.
Inorganic Chemistry Frontiers,
Год журнала:
2022,
Номер
9(11), С. 2479 - 2497
Опубликована: Янв. 1, 2022
A
novel
2D/0D
C
3
N
5
/Bi
2
WO
6
S-scheme
heterojunction
with
enhanced
structural
defects
has
been
designed
for
the
efficient
elimination
of
pharmaceutical
antibiotics
and
Cr(
vi
).
Angewandte Chemie International Edition,
Год журнала:
2024,
Номер
63(29)
Опубликована: Май 6, 2024
Abstract
Despite
the
pivotal
role
of
molecular
oxygen
(O
2
)
activation
in
artificial
photosynthesis,
efficiency
is
often
restricted
by
sluggish
exciton
dissociation
and
charge
transfer
kinetics
within
polymer
photocatalysts.
Herein,
we
propose
two
tetrathiafulvalene
(TTF)‐based
imine‐linked
covalent
organic
frameworks
(COFs)
with
tailored
donor‐acceptor
(D–A)
structures,
TTF‐PDI‐COF
TTF‐TFPP‐COF,
to
promote
O
activation.
Because
enhanced
electron
push‐pull
interactions
that
facilitated
separation
behavior,
exhibited
superior
photocatalytic
activity
electron‐induced
reactions
over
TTF‐TFPP‐COF
under
visible
light
irradiation,
including
photosynthesis
(
E
)‐3‐amino‐2‐thiocyano‐
α
,
β
‐unsaturated
compounds
H
.
These
findings
highlight
significant
potential
rational
design
COFs
D–A
configurations
as
suitable
candidates
for
advanced
applications.
ACS Catalysis,
Год журнала:
2022,
Номер
12(13), С. 7821 - 7832
Опубликована: Июнь 17, 2022
Artificial
enzymatic
systems
have
emerged
in
the
field
of
biomimetic
catalysis
by
constructing
specific
catalytic
centers
enzymes.
Inspired
high
activity
natural
monooxygenase
for
oxidation
transformation,
several
binuclear
Cu/Fe-based
metal–organic
frameworks
(MOFs)
been
frequently
used
as
catalysts,
yet
rarely
reports
MOFs
with
other
metals
nodes
reported
to
date.
In
this
work,
ingenious
decoration
Ce–O–Ce
moieties
and
anthraquinone
groups
good
oxygen
activation
ability
one
framework,
an
MOF-supported
artificial
cerium
was
obtained
highly
selective
inert
C(sp3)–H
bonds.
The
single-crystal
structural
study
reveals
that
molecule-level
modularity
a
moiety
design
MOF
creates
confined
microenvironment
offer
ordered
distribution
dense
substrate-accessible
active
sites
throughout
architecture.
After
photoexcitation,
trigger
ligand-to-metal
charge-transfer
(LMCT)
event
form
bridge
radical,
which
abstracts
hydrogen
atom
from
bond
generate
carbon-centered
radical
through
typical
transfer
(HAT)
process.
These
radicals
rapidly
combine
reactive
species
(ROS)
produced
via
energy
(EnT)
process
alkyl
peroxy
intermediates,
are
easily
trapped
another
unsaturated
coordinated
ions
further
facilitate
their
hydrolysis
formation
carbonyl
products.
This
anthraquinone-functionalized
framework
containing
resembling
exhibits
unique
selectivity
(>97%)
activity,
represent
first
example
constructed
different
applying
alkanes,
expanding
selection
range
metal
monooxygenase.
Taking
advantage
heterogeneity
MOF,
Ce–MOF
recycled
five
times
without
decrease
its
possessed
broader
applicability
substrate
C–H
bonds,
providing
blueprint
designing
new
alkane
oxidation.
