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.
Chemical Society Reviews,
Год журнала:
2022,
Номер
51(16), С. 6965 - 7045
Опубликована: Янв. 1, 2022
This
review
summarizes
the
recent
advances
in
light
driven
catalytic
H
2
evolution
and
CO
reduction
systems
towards
production
of
solar
fuels,
utilizing
porphyrin
or
phthalocyanine
derivatives.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Май 29, 2023
The
strong
excitonic
effects
widely
exist
in
polymer-semiconductors
and
the
large
exciton
binding
energy
(Eb)
seriously
limits
their
photocatalysis.
Herein,
density
functional
theory
(DFT)
calculations
are
conducted
to
assess
band
alignment
charge
transfer
feature
of
potential
donor-acceptor
(D-A)
covalent
organic
frameworks
(COFs),
using
1,3,5-tris(4-aminophenyl)triazine
(TAPT)
or
1,3,5-tris(4-aminophenyl)benzene
(TAPB)
as
acceptors
tereph-thaldehydes
functionalized
diverse
groups
donors.
Given
discernable
D-A
interaction
strengths
pairs,
Eb
can
be
systematically
regulated
with
minimum
TAPT-OMe.
Guided
by
these
results,
corresponding
COFs
synthesized,
where
TAPT-OMe-COF
possesses
best
activity
photocatalytic
H2
production
trend
other
is
associated
that
calculated
for
pairs.
In
addition,
further
alkyne
cycloaddition
imine
linkage
greatly
improves
stability
resulting
TAPT-OMe-alkyne-COF
a
substantially
smaller
exhibits
~20
times
higher
than
parent
COF.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(30)
Опубликована: Апрель 29, 2023
Optimizing
the
electronic
structure
of
covalent
organic
framework
(COF)
photocatalysts
is
essential
for
maximizing
photocatalytic
activity.
Herein,
we
report
an
isoreticular
family
multivariate
COFs
containing
chromenoquinoline
rings
in
COF
and
electron-donating
or
withdrawing
groups
pores.
Intramolecular
donor-acceptor
(D-A)
interactions
allowed
tuning
local
charge
distributions
carrier
separation
under
visible
light
irradiation,
resulting
enhanced
performance.
By
optimizing
optoelectronic
properties
COFs,
a
uranium
extraction
efficiency
8.02
mg/g/day
was
achieved
using
nitro-functionalized
multicomponent
natural
seawater,
exceeding
performance
all
reported
to
date.
Results
demonstrate
effective
design
strategy
towards
high-activity
with
intramolecular
D-A
structures
not
easily
accessible
traditional
synthetic
approaches.
Angewandte Chemie International Edition,
Год журнала:
2022,
Номер
61(15)
Опубликована: Янв. 21, 2022
As
hot
topics
in
the
chemical
conversion
of
CO2
,
photo-/electrocatalytic
reduction
and
use
as
a
supporter
for
energy
storage
have
shown
great
potential
utilization
.
However,
many
obstacles
still
exist
on
road
to
realizing
highly
efficient
conversion,
such
inefficient
uptake/activation
mass
transport
catalysts.
Covalent
organic
frameworks
(COFs),
kind
porous
material,
been
widely
explored
catalysts
owing
their
unique
features.
In
particular,
COF-based
functional
materials
containing
diverse
active
sites
(such
single
metal
sites,
nanoparticles,
oxides)
offer
storage.
This
Minireview
discusses
recent
breakthroughs
basic
knowledge,
mechanisms,
pathways
strategies
that
addition,
challenges
prospects
are
also
introduced.
Nature Communications,
Год журнала:
2022,
Номер
13(1)
Опубликована: Янв. 10, 2022
Abstract
Developing
a
facile
strategy
for
the
construction
of
vinylene-linked
fully
π
-conjugated
covalent
organic
frameworks
(COFs)
remains
huge
challenge.
Here,
versatile
condition
Knoevenagel
polycondensation
constructing
2D
COFs
was
explored.
Three
new
examples
(
BTH-1
,
2
3
)
containing
benzobisthiazoles
units
as
functional
groups
were
successfully
prepared
under
this
and
mild
condition.
The
electron-deficient
benzobisthiazole
cyano-vinylene
linkages
both
integrated
into
conjugated
skeleton
acted
acceptor
moieties.
Interestingly,
we
found
highly
ordered
D-A
system
is
favorable
photocatalytic
activity.
BTH-3
with
benzotrithiophene
donor
strong
effect
exhibited
an
attractive
HER
15.1
mmol
h
−1
g
visible
light
irradiation.
Chemistry of Materials,
Год журнала:
2022,
Номер
34(11), С. 5232 - 5240
Опубликована: Май 16, 2022
Covalent
organic
frameworks
(COFs)
are
an
ideal
template
for
photocatalytic
H2O2
synthesis
because
of
the
tunable
chemical
structures
and
semiconductor
properties.
However,
photoactivity
COFs
is
still
under-improved
due
to
inefficient
intrinsic
charge
generation,
fast
recombination
photogenerated
charges,
limited
electron
transport
along
frameworks.
Herein,
spatially
separated
synergistic
triazine
acetylene
units
first
integrated
into
(EBA-COF
BTEA-COF)
production.
The
spatial
separation
cores
leads
efficient
suppressed
recombination,
C═C
linkage
facilitates
electrons
over
skeletons.
Both
experimental
computational
results
suggested
that
synergistically
promote
in
a
two-electron
pathway.
EBA-COF
showed
attractive
activity
with
production
rate
1830
μmol
h–1
gcat–1,
superior
most
other
COF-based
catalysts.
This
study
provides
method
designing
photocatalysts
active
sites
based
on
vinylene-linked
COFs.
Nature Communications,
Год журнала:
2023,
Номер
14(1)
Опубликована: Фев. 3, 2023
Covalent
organic
frameworks
(COFs)
are
an
emerging
type
of
crystalline
and
porous
photocatalysts
for
hydrogen
evolution,
however,
the
overall
water
splitting
activity
COFs
is
rarely
known.
In
this
work,
we
firstly
realized
β-ketoamine
by
systematically
engineering
N-sites,
architecture,
morphology.
By
in
situ
incorporating
sub-nanometer
platinum
(Pt)
nanoparticles
co-catalyst
into
pores
nanosheets,
both
Pt@TpBpy-NS
Pt@TpBpy-2-NS
show
visible-light-driven
activity,
with
optimal
H
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(34)
Опубликована: Апрель 24, 2023
Abstract
Intensifying
energy
crises
and
severe
environmental
issues
have
led
to
the
discovery
of
renewable
sources,
sustainable
conversion,
storage
technologies.
Photocatalysis
is
a
green
technology
that
converts
eco‐friendly
solar
into
high‐energy
chemicals.
Covalent
organic
frameworks
(COFs)
are
porous
materials
constructed
by
covalent
bonds
show
promising
potential
for
converting
chemicals
owing
their
pre‐designable
structures,
high
crystallinity,
porosity.
Herein,
we
highlight
recent
progress
in
synthesis
COF‐based
photocatalysts
applications
water
splitting,
CO
2
reduction,
H
O
production.
The
challenges
future
opportunities
rational
design
COFs
advanced
discussed.
This
Review
expected
promote
further
development
toward
photocatalysis.
