Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Окт. 11, 2024
Rational
design
of
robust
photocatalytic
systems
to
direct
capture
and
in-situ
convert
diluted
CO2
from
flue
gas
is
a
promising
but
challenging
way
achieve
carbon
neutrality.
Here,
we
report
new
type
host-guest
photocatalysts
by
integrating
CO2-enriching
ionic
liquids
photoactive
metal-organic
frameworks
PCN-250-Fe2M
(M
=
Fe,
Co,
Ni,
Zn,
Mn)
for
artificial
photosynthetic
reduction
in
gas-solid
phase.
As
result,
[Emim]BF4(39.3
wt%)@PCN-250-Fe2Co
exhibits
record
high
CO2-to-CO
rate
313.34
μmol
g−1
h−1
under
pure
atmosphere
153.42
(15%)
with
about
100%
selectivity.
In
scaled-up
experiments
1.0
g
catalyst
natural
sunlight
irradiation,
the
concentration
could
be
significantly
decreased
below
85%
10%,
respectively,
indicating
its
industrial
application
potential.
Further
theoretical
calculations
reveal
that
not
only
benefit
enrichment,
also
form
synergistic
effect
Co2+
sites
PCN-250-Fe2Co,
resulting
significant
Gibbs
energy
barrier
during
rate-determining
step
conversion.
Artificial
fuel
authors
system
frameworks,
greatly
enhancing
conversion
efficiency.
Nature Communications,
Год журнала:
2024,
Номер
15(1)
Опубликована: Июнь 7, 2024
Developing
highly
active
materials
that
efficiently
utilize
solar
spectra
is
crucial
for
photocatalysis,
but
still
remains
a
challenge.
Here,
we
report
new
donor-acceptor
(D-A)
covalent
organic
framework
(COF)
with
wide
absorption
range
from
200
nm
to
900
(ultraviolet-visible-near
infrared
light).
We
find
the
thiophene
functional
group
accurately
introduced
into
electron
acceptor
units
of
TpDPP-Py
(TpDPP:
5,5'-(2,5-bis(2-ethylhexyl)-3,6-dioxo-2,3,5,6-tetrahydropyrrolo
[3,4-c]pyrrole-1,4-diyl)bis(thiophene-2-carbaldehyde),
Py:
1,3,6,8-tetrakis(4-aminophenyl)pyrene)
COFs
not
only
significantly
extends
its
spectral
capacity
also
endows
them
two-photon
and
three-photon
effects,
greatly
enhancing
utilization
rate
sunlight.
The
selective
coupling
benzylamine
as
target
reactant
used
assess
photocatalytic
activity
COFs,
showing
high
conversion
99%
selectivity
98%
in
20
min.
Additionally,
exhibit
universality
other
imine
derivatives
~100%
efficiency.
Overall,
this
work
brings
significant
strategy
developing
enhance
activity.
