Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
61(3)
Опубликована: Ноя. 15, 2021
Titanium
metal-organic
frameworks
(Ti-MOFs),
as
an
appealing
type
of
artificial
photocatalyst,
have
shown
great
potential
in
the
field
solar
energy
conversion
due
to
their
well-studied
photoredox
activity
(similar
TiO2
)
and
good
optical
responsiveness
linkers,
which
serve
antenna
absorb
visible-light.
Although
much
effort
has
been
dedicated
developing
Ti-MOFs
with
high
photocatalytic
activity,
performances
are
still
poor.
Herein,
we
implemented
a
covalent-integration
strategy
construct
series
multivariate
Ti-MOF/COF
hybrid
materials
PdTCPP⊂PCN-415(NH2
)/TpPa
(composites
1,
2,
3),
featuring
excellent
visible-light
utilization,
suitable
band
gap,
surface
area
for
H2
production.
Notably,
resulting
composites
demonstrated
remarkably
enhanced
visible-light-driven
evolution
performance,
especially
composite
2
maximum
rate
13.98
mmol
g-1
h-1
(turnover
frequency
(TOF)=227
),
is
higher
than
that
(0.21
TpPa
(6.51
).
Our
work
thereby
suggests
new
approach
highly
efficient
photocatalysts
beyond.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(42)
Опубликована: Авг. 27, 2022
Abstract
Two‐dimensional
covalent
organic
frameworks
(2D‐COFs)
have
emerged
as
attractive
platforms
for
solar‐to‐chemical
energy
conversion.
In
this
study,
we
implemented
a
gradient
heating
strategy
to
synthesize
sp
2
‐carbon‐linked
triazine‐based
COF,
COF‐JLU100,
exhibiting
high
crystallinity,
large
surface
area,
good
durability
and
carrier
mobility
solar‐driven
photocatalytic
hydrogen
evolution.
The
Pt‐doped
COF‐JLU100
demonstrated
evolution
rate
of
over
100
000
μmol
g
−1
h
water
splitting
under
visible‐light
illumination
(λ>420
nm).
Experimental
theoretical
studies
corroborate
that
the
cyano‐vinylene
segments
in
extend
π‐delocalization
enable
fast
charge
transfer
separation
rates
well
dispersion
water.
Moreover,
can
be
prepared
by
low‐cost
easily
available
monomers
has
excellent
stability,
which
is
desirable
practical
production.
Journal of the American Chemical Society,
Год журнала:
2022,
Номер
144(30), С. 13953 - 13960
Опубликована: Июль 25, 2022
Vinylene/olefin-linked
two-dimensional
covalent
organic
frameworks
(v-2D-COFs)
have
emerged
as
advanced
semiconducting
materials
with
excellent
in-plane
conjugation,
high
chemical
stabilities,
and
precisely
tunable
electronic
structures.
Exploring
new
linkage
chemistry
for
the
reticular
construction
of
v-2D-COFs
remains
in
infancy
challenging.
Herein,
we
present
a
solid-state
benzobisoxazole-mediated
aldol
polycondensation
reaction
two
novel
isomeric
benzobisoxazole-bridged
(v-2D-COF-NO1
v-2D-COF-NO2)
trans
cis
configurations
benzobisoxazole.
Interestingly,
benzobisoxazole
linkers
endow
distinct
optoelectronic
electrochemical
properties,
ranging
from
light
absorption
emission
to
charge-transfer
properties.
When
employed
photocathode,
v-2D-COF-NO1
exhibits
photocurrent
up
∼18
μA/cm2
under
AM
1.5G
irradiation
at
-0.3
V
vs
reversible
hydrogen
electrode
(RHE),
which
is
twice
value
v-2D-COF-NO2
(∼9.1
μA/cm2).
With
Pt
cocatalyst,
demonstrates
photocatalytic
evolution
rate
∼1.97
mmol
h-1
g-1,
also
clear
contrast
that
(∼0.86
g-1)
identical
conditions.
This
work
synthesis
via
structures
Nature Communications,
Год журнала:
2022,
Номер
13(1)
Опубликована: Авг. 6, 2022
High-performance
and
low-cost
photocatalysts
play
the
key
role
in
achieving
large-scale
solar
hydrogen
production.
In
this
work,
we
report
a
liquid-exfoliation
approach
to
prepare
NiPS
Angewandte Chemie International Edition,
Год журнала:
2021,
Номер
61(3)
Опубликована: Ноя. 15, 2021
Titanium
metal-organic
frameworks
(Ti-MOFs),
as
an
appealing
type
of
artificial
photocatalyst,
have
shown
great
potential
in
the
field
solar
energy
conversion
due
to
their
well-studied
photoredox
activity
(similar
TiO2
)
and
good
optical
responsiveness
linkers,
which
serve
antenna
absorb
visible-light.
Although
much
effort
has
been
dedicated
developing
Ti-MOFs
with
high
photocatalytic
activity,
performances
are
still
poor.
Herein,
we
implemented
a
covalent-integration
strategy
construct
series
multivariate
Ti-MOF/COF
hybrid
materials
PdTCPP⊂PCN-415(NH2
)/TpPa
(composites
1,
2,
3),
featuring
excellent
visible-light
utilization,
suitable
band
gap,
surface
area
for
H2
production.
Notably,
resulting
composites
demonstrated
remarkably
enhanced
visible-light-driven
evolution
performance,
especially
composite
2
maximum
rate
13.98
mmol
g-1
h-1
(turnover
frequency
(TOF)=227
),
is
higher
than
that
(0.21
TpPa
(6.51
).
Our
work
thereby
suggests
new
approach
highly
efficient
photocatalysts
beyond.
