Abstract
The
use
of
sunlight
to
convert
CO
2
into
multi‐carbon
fuels,
particularly
propylene,
is
considered
a
sustainable
carbon
cycle
pathway,
but
propylene
requires
multi‐electron‐coupled
proton
reaction
process
that
has
not
been
reported.
Herein,
two
covalent
organic
frameworks
(DA‐COF
and
DP‐COF)
are
prepared
by
varying
the
bridging
positions
anthraquinone
conjugated
units.
experimental
results
show
neighbouring
bridge
in
DA‐COF
forms
unique
cleavage
structure
like
an
enzyme
catalyst,
which
can
provide
efficient
microenvironment
for
reduction
trap
protons.
At
same
time,
neighbor
form
electron
donor‐electron
acceptor
accelerate
photogenerated
carrier
migration.
As
result,
exhibits
excellent
visible
light
production
with
yield
270.54
µmol
g
−1
no
C₃H₆
product
detected
DP‐COF
during
process.
This
study
presents
novel
avenue
high
value‐added
products
using
photocatalysis.
Inorganic Chemistry,
Год журнала:
2025,
Номер
unknown
Опубликована: Фев. 6, 2025
The
essential
nature
of
the
photocatalytic
process
is
charge
transfer.
To
optimize
spatial
separation
photogenerated
electron–hole
(e–-h+)
pairs
for
high-performance
catalytic
efficiency,
in
this
work,
we
have
successfully
prepared
hierarchical
core–shell
two-dimensional
(2D)/2D
ZnIn2S4@TpBpy
(ZIS@TpBpy)
with
well-matched
Z-scheme
interfacial
transfer
channels
uranium
(U(VI))
photoreduction.
electron
configuration
was
confirmed
by
internal
electric
field
(IEF)
formation
analysis,
XPS
characterization,
and
DMPO
spin-trapping
EPR
spectroscopy.
With
large
specific
surface
area
abundant
active
sites,
ZIS@TpBpy
composite
achieved
a
U(VI)
extraction
rate
94.08%.
In
addition,
removal
constant
(0.0137
min–1)
2.05
4.28
times
higher
than
those
TpBpy
(0.0067
ZnIn2S4
(0.0032
min–1),
respectively.
First,
combination
organic
inorganic
components
expanded
range
visible
light
absorption
utilization.
Afterward,
under
visible-light
irradiation,
more
e–-h+
dissociated
migrated
to
driven
IEF
heterostructure.
Simultaneously,
synergistic
effect
between
polarization
potential
generated
sites
(N
O
atoms)
framework
further
accelerated
depletion
translocation
pairs,
which
significantly
improved
efficiency
reduction
U(VI).