Dalton Transactions,
Год журнала:
2024,
Номер
53(37), С. 15688 - 15695
Опубликована: Янв. 1, 2024
The
efficiency
of
photocatalysts
depends
largely
on
the
accessibility
reaction
species
to
active
centre,
electron
transfer
and
geometric
matching
between
surface
catalyst
species.
In
this
work,
we
successfully
synthesized
designed
one
two-dimensional
Mn(II)
MOF
with
[Mn
Monolayer
2D
metal‐organic
framework
(MOF)
nanosheets,
characterized
by
abundant
exposed
active
sites
and
tunable
structure
function
(such
as
altering
the
metal
nodes
or
organic
ligands),
have
emerged
a
pivotal
class
of
materials,
demonstrating
irreplaceable
applications
across
diverse
research
domains
in
materials
chemistry.
This
review
provides
comprehensive
survey
latest
progress
synthesis
monolayer
MOF
nanosheets.
Specifically,
recent
synthetic
strategies,
including
top‐down
bottom‐up
methods,
are
delved
their
gas
separation,
catalysis,
sensing
platforms,
energy
storage
explored.
Additionally,
challenges
faced
investigation
nanosheets
elucidated
future
opportunities
for
these
novel
generation
outlined.
Inorganic Chemistry Frontiers,
Год журнала:
2024,
Номер
11(15), С. 4731 - 4739
Опубликована: Янв. 1, 2024
Novel
visible-light-responsive
BODIPY-based
MOFs
exhibited
excellent
photocatalytic
activity
toward
oxidation
of
sulfides
and
arylboronic
acids
under
ambient
conditions,
which
was
attributed
to
the
active
oxygen
species
produced
in
reaction.
Angewandte Chemie,
Год журнала:
2024,
Номер
136(11)
Опубликована: Янв. 13, 2024
Abstract
Modifying
redox
potential
of
substrates
and
intermediates
to
balance
pairs
steps
are
important
stages
for
multistep
photosynthesis
but
faced
marked
challenges.
Through
co‐clathration
iridium
photosensitizer
imine
substrate
within
one
packet
a
metal‐organic
capsule
shift
the
potentials
substrate,
herein,
we
reported
multiphoton
enzymatic
strategy
generation
heterocycles
by
intramolecular
C−X
hydrogen
evolution
cross‐couplings.
The
cage
facilitated
pre‐equilibrium
substrate‐involving
clathrate
that
cathodic
shifts
oxidation
substrate‐dye‐host
ternary
complex
configuration
inversion
via
spatial
constraints
in
confined
space.
new
two
photon
excitation
enabled
precise
control
electron
transfer
between
each
pair
(photosensitizer,
capsule),
endowing
catalytic
system
proceeding
smoothly
with
an
fashion.
Three
kinds
2‐subsituted
(−OH,
−NH
2
,
−SH)
imines
N‐aryl
enamines
all
give
corresponding
cyclization
products
efficiently
under
visible
light
irradiation,
demonstrating
promising
microenvironment
driven
thermodynamic
activation
host‐dye‐substrate
synergistic
combination
photocatalytic
transformations.
ACS Applied Materials & Interfaces,
Год журнала:
2024,
Номер
16(11), С. 13938 - 13947
Опубликована: Март 7, 2024
Natural
copper
oxygenases
provide
fundamental
principles
for
catalytic
oxidation
with
kinetically
inert
molecular
oxygen,
but
it
remains
a
marked
challenge
to
mimic
both
their
structure
and
function
in
an
entity.
Inspired
by
the
CuA
enzymatic
sites,
herein
we
report
two
new
photoactive
binuclear
copper–iodine-
bisbenzimidazole-comodified
coordination
polymers
reproduce
natural
oxo-functionalization
repertoire
unique
photocatalytic
pathway.
Under
light
irradiation,
Cu–halide
effectively
reduce
NHP
esters
complete
oxygen
reduction
activation
via
photoinduced
electron
transfer
aerobic
oxidative
coupling
of
hydroquinone
terminal
alkynes,
affording
hydroxyl-functionalized
ketones
high
efficiency
selectivity.
This
supramolecular
approach
developing
bioinspired
artificial
that
merge
transition
metal-
photocatalysis
supplies
way
fabricate
distinctive
photocatalysts
desirable
performances
controllable
precise
active
sites.
ACS Materials Letters,
Год журнала:
2023,
Номер
5(8), С. 2263 - 2269
Опубликована: Июль 24, 2023
Enzymes
facilitate
chemical
conversions
through
the
integrated
activity
of
multicomponents,
but
aggregation
multiactive
sites
with
molecular
containers
to
emulate
enzymatic
conversion
remains
challenging.
Herein,
we
report
a
new
CeIII-based
octahedral
cage
chloride
ligands
that
boosts
C(sp3)−H
photoactivation
by
marrying
CeIV–Cl
photocatalyst
and
photoredox
catalyst
integrate
photoinduced
electron
transfer
(PET),
ligand-to-metal
charge
(LMCT),
hydrogen-atom
(HAT)
events
multiphoton
excitation.
This
binds
2-chloro-9H-thioxanthen-9-one
(TXO)
for
boosting
PET
via
pseudointramolecular
pathway
oxidize
CeIII–Cl
form
TXO•–.
The
LMCT
excitation
is
triggered
Cl•
activates
HAT,
resulting
in
regeneration
formation
an
alkyl
radical.
TXO•–
reduces
reaction
intermediate,
which
transforms
facilitates
recovery
TXO
subsequent
recycling.
approach
offers
feasible
strategy
creating
highly
electrophilic
radicals
resembling
enzymes
demonstrates
their
potential
functionalization.
Dalton Transactions,
Год журнала:
2024,
Номер
53(37), С. 15688 - 15695
Опубликована: Янв. 1, 2024
The
efficiency
of
photocatalysts
depends
largely
on
the
accessibility
reaction
species
to
active
centre,
electron
transfer
and
geometric
matching
between
surface
catalyst
species.
In
this
work,
we
successfully
synthesized
designed
one
two-dimensional
Mn(II)
MOF
with
[Mn