Advanced Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Апрель 3, 2025
The
efficient
conversion
of
solar
energy
into
clean
hydrogen
fuel
presents
a
promising
pathway
for
sustainable
production.
However,
utilizing
the
full
spectrum,
particularly
near-infrared
(NIR)
region,
remains
underexplored
in
photosynthetic
biohybrid
systems.
In
this
study,
biocompatible,
low-bandgap
conjugated
polymer
nanosheets
(PyTT-tBAL-HAB)
are
developed
to
integrate
with
non-photosynthetic,
non-genetically
engineered
Escherichia
coli
(E.
coli)
enhanced
solar-driven
biological
PyTT-tBAL-HAB
exhibit
unique
NIR
light
absorption
properties.
Integrating
these
E.
facilitates
electron
transfer,
resulting
1.96-fold
increase
production
rate
under
light.
Consequently,
system
achieves
quantum
efficiency
18.36%
at
940
nm.
This
study
demonstrates
potential
using
as
advanced
photosensitizers
semi-artificial
systems,
offering
robust
platform
effective
utilization
spectrum.
Environmental Science & Technology,
Год журнала:
2022,
Номер
56(8), С. 5161 - 5169
Опубликована: Март 21, 2022
Semiartificial
photosynthesis
shows
great
potential
in
solar
energy
conversion
and
environmental
application.
However,
the
rate-limiting
step
of
photoelectron
transfer
at
biomaterial
interface
results
an
unsatisfactory
quantum
yield
(QY,
typically
lower
than
3%).
Here,
anthraquinone
molecule,
which
has
dual
roles
microbial
photosensitizer
capacitor,
was
demonstrated
to
negotiate
via
decoupling
photochemical
reaction
with
a
dark
reaction.
In
model
system,
anthraquinone-2-sulfonate
(AQS)-photosensitized
Thiobacillus
denitrificans,
maximum
QY
solar-to-nitrous
oxide
(N2O)
96.2%
achieved,
is
highest
among
semiartificial
systems.
Moreover,
nitrate
into
N2O
almost
100%,
indicating
excellent
selectivity
reduction.
The
capacitive
property
AQS
resulted
82–89%
photoelectrons
released
enhanced
5.6–9.4
times
solar-to-N2O.
Kinetics
investigation
revealed
zero-order-
first-order-
kinetics
production
(reductive
AQS-mediated
electron
transfer)
under
light
(direct
transfer),
respectively.
This
work
first
study
demonstrate
role
photosensitizing
microorganism
provides
simple
highly
selective
approach
produce
from
nitrate-polluted
wastewater
strategy
for
efficient
solar-to-chemical
by
system.
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(12), С. 6719 - 6729
Опубликована: Март 14, 2023
Semi-artificial
approaches
to
solar-to-chemical
conversion
can
achieve
chemical
transformations
that
are
beyond
the
capability
of
natural
enzymes,
but
face
marked
challenges
facilitate
in
vivo
cascades,
due
their
inevitable
need
for
cofactor
shuttling
and
regeneration.
Here,
we
report
on
an
enzyme
grafting
strategy
build
a
metal-organic
capsule-docking
artificial
(metal-organic-enzyme,
MOE)
comprised
self-assembly
cofactor-decorated
capsule
supramolecular
enzyme-recognition
features
between
scaffold
bypass
The
incorporated
NADH
mimics
within
interacted
with
imine
intermediate
formed
from
condensation
amines
dehydrogenation
alcohol
substrates
microenvironment
form
complexes
subsequently
served
as
situ-generated
photoresponsive
cofactor.
Upon
illumination,
facilitates
efficient
proton/electron
transport
inner
space
(supramolecular
hydrogenation)
outer
(enzymatic
dehydrogenation)
dehydrogenize
alcohols
hydrogenize
intermediates,
respectively,
circumventing
conventionally
complex
multistep
semi-artificial
endows
diverse
types
amine
products
both
aqueous/organic
solutions
Escherichia
coli
high
efficiency,
offering
wide
range
opportunities
sustainable
environmentally
friendly
biomanufacturing
commodity
fine
chemicals.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Окт. 19, 2024
Natural
photosynthesis
utilizes
solar
energy
to
convert
water
and
atmospheric
CO2
into
carbohydrates
through
all-weather
light/dark
reactions
based
on
molecule-based
enzymes
coenzymes,
inspiring
extensive
development
of
artificial
photosynthesis.
However,
efficient
photosynthetic
systems
free
noble
metals,
as
well
rational
integration
functional
units
a
single
system
at
the
molecular
level,
remain
challenging.
Here
we
report
an
system,
assembly
Cu6
cluster
cobalt
terpyridine
complex,
that
mimics
natural
precise
nanozyme
complexes
ubiquinone
(coenzyme
Q)
clusters.
This
biomimetic
efficiently
reduces
CO
in
light
reaction,
achieving
production
rate
740.7
μmol·g−1·h−1
with
high
durability
for
least
188
hours.
Notably,
our
realizes
decoupling
dark
reactions,
utilizing
phenol-evolutive
coenzyme
Q
acting
electron
reservoir.
By
regulating
stabilizer
Q,
reaction
time
can
be
extended
up
8.5
hours,
which
fully
meets
day/night
cycle
requirements.
Our
findings
advance
design
replicate
comprehensive
functions
converts
H2O
coenzymes.
Here,
authors
under
intermittent
irradiation
by
integrating
copper
nanocluster.
ACS Sustainable Chemistry & Engineering,
Год журнала:
2025,
Номер
13(4), С. 1522 - 1531
Опубликована: Янв. 22, 2025
Current
efforts
to
decarbonize
the
chemical
sector
by
using
captured
CO2
and
electrolytic
H2
typically
lead
high
production
costs
environmental
collateral
damage.
Hence,
there
is
a
clear
need
look
for
alternative,
more
efficient
synthesis
routes
that
could
pave
way
fully
sustainable
industry.
Bearing
this
in
mind,
here,
we
evaluate
economic
implications
of
two
low
technology
readiness
level
(TRL)
novel
single-step
acetic
acid
as
raw
material:
gas-to-acid
methane
carboxylation
semiartificial
photosynthesis.
Using
process
simulation
life-cycle
assessment,
determine
these
pathways,
under
specific
set
assumptions,
outperform
business-as-usual
methanol
carbonylation
at
their
current
development
state
terms
global
warming,
human
health,
ecosystem
quality,
resource
scarcity
impacts,
showing
no
signs
burden
shifting.
Furthermore,
also
result
lower
derived
from
reduced
energy
requirement
associated
with
single
step.
Overall,
our
preliminary
results
TRL
technologies
based
on
experimental
data
highlight
potential
benefits
exploring
alternative
routes,
which
help
bridge
fossil-based
industrial
landscape
future.
