ACS Catalysis,
Год журнала:
2024,
Номер
14(21), С. 16374 - 16382
Опубликована: Окт. 22, 2024
Combining
abiotic
photocatalytic
modules
with
enzymatic
conversion
to
reform
biomass
represents
a
compelling
way
for
sustainable
energy
schemes
but
faces
marked
challenges
on
the
electron
and
proton
transport
corresponding
cofactor
regeneration
shuttling
between
biotic
partners.
Herein,
we
report
consecutive
photoinduced
electron-transfer
approach
into
fuels
active
H-source
nitroarene
reduction
by
grafting
cage-dye-NADH
(nicotinamide
adenine
dinucleotide)
clathrate
glucose
dehydrogenase
(GDH).
Under
light
irradiation,
acts
as
photoactive
relay
conduct
two
1e–
reactions
consecutively
2e–
oxidation
of
NADH
NAD+,
guaranteeing
an
orderly
path
related
regeneration.
When
is
positioned
inside
pocket
GDH
join
NAD+-mediated
synthesis,
metal–organic
artificial
enzyme
facilitates
fast
generation
native
within
one
working
module.
The
combines
photocatalysis
dehydrogenation
endow
efficient
feedstocks
green
H-source,
innovating
unique
paradigm
scheme
that
photons
in
turnover
cycle.
superiority
allows
direct
hydrogenation
fine
chemicals
enables
tandem
number
reaching
15,000,
providing
distinguished
avenue
utilization
solar
conversion.
Chemistry - A European Journal,
Год журнала:
2024,
Номер
30(43)
Опубликована: Май 28, 2024
Imines
are
essential
intermediates
in
organic
transformations,
and
is
generally
produced
by
dehydrogenative
condensation
of
alcohols
amines
with
the
assist
specialized
catalysts
additives.
Heterogeneous
photocatalysis
provides
a
sustainable
platform
for
such
process
without
using
toxic
oxidants,
yet
functionalized
photocatalyst
optimized
co-adsorption
reactants
needs
to
be
developed
promote
stoichiometric
oxidative
under
ambient
conditions.
Here,
we
show
that
benzyl
alcohol
aniline
adsorb
non-interferingly
on
Fe
node
linker
sites
MIL-53(Fe)
metal
frameworks
(MOFs),
respectively.
The
both
barely
influences
reduction
molecular
oxygen
generate
radicals,
resulting
efficient
formation
benzaldehyde
visible
light.
Additionally,
weak
adsorption
water
together
surface
acidity
rapid
depletion
generated
water,
achieving
an
C-N
bond
creation
wide
range
substrates.
Chemosensors,
Год журнала:
2024,
Номер
12(8), С. 145 - 145
Опубликована: Июль 30, 2024
Nitroreductase
(NTR)
is
an
enzyme
expressed
at
abnormally
high
level
in
solid
tumors,
which
associated
with
the
hypoxia
tumors.
The
establishment
of
a
high-performance
and
convenient
fluorescent
platform
for
fast
monitoring
NTR
pivotal
importance.
Herein,
novel
host–guest
complex
was
created
by
encapsulating
substrate
GP-NTR
within
metal–organic
capsule
Zn-MPB
that
included
NADH
mimic
detection
via
responding
to
nitroreductase
responsiveness
good
fluorescence
imaging.
Notably,
double-substrate
process
streamlined
single–substrate
supramolecular
method
catalytic
NTR,
enabled
reaction
be
independent
cofactor
supply
shortened
distance
between
active
site
NTR.
increasing
intensity
Zn-MPB⊃GP-NTR
exhibits
linear
relationship
concentration
shows
response
toward
solution
tens
seconds.
also
displays
sensitivity
low
limit
6.4
ng/mL.
Cells
vivo
studies
have
confirmed
could
successfully
applied
imaging
NTR-overexpressed
tumor
cells
tumor-bearing
animals.
not
only
provides
new
avenue
design
optimization
rapid
quantitative
activity,
but
offers
tool
early
diagnosis
hypoxia-related
Dalton Transactions,
Год журнала:
2023,
Номер
52(23), С. 8135 - 8141
Опубликована: Янв. 1, 2023
Brønsted-base
active
sites
on
a
Pd
4
L
2
cage
facilitates
enhanced
catalytic
efficiency,
wide
substrate
scope
and
high
turnover
number
(TON)
for
the
one-pot
photooxidation/Knoevenagel
condensation
reaction
under
mild
conditions.
ACS Catalysis,
Год журнала:
2024,
Номер
14(21), С. 16374 - 16382
Опубликована: Окт. 22, 2024
Combining
abiotic
photocatalytic
modules
with
enzymatic
conversion
to
reform
biomass
represents
a
compelling
way
for
sustainable
energy
schemes
but
faces
marked
challenges
on
the
electron
and
proton
transport
corresponding
cofactor
regeneration
shuttling
between
biotic
partners.
Herein,
we
report
consecutive
photoinduced
electron-transfer
approach
into
fuels
active
H-source
nitroarene
reduction
by
grafting
cage-dye-NADH
(nicotinamide
adenine
dinucleotide)
clathrate
glucose
dehydrogenase
(GDH).
Under
light
irradiation,
acts
as
photoactive
relay
conduct
two
1e–
reactions
consecutively
2e–
oxidation
of
NADH
NAD+,
guaranteeing
an
orderly
path
related
regeneration.
When
is
positioned
inside
pocket
GDH
join
NAD+-mediated
synthesis,
metal–organic
artificial
enzyme
facilitates
fast
generation
native
within
one
working
module.
The
combines
photocatalysis
dehydrogenation
endow
efficient
feedstocks
green
H-source,
innovating
unique
paradigm
scheme
that
photons
in
turnover
cycle.
superiority
allows
direct
hydrogenation
fine
chemicals
enables
tandem
number
reaching
15,000,
providing
distinguished
avenue
utilization
solar
conversion.