Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(3), P. 1475 - 1496
Published: Jan. 16, 2023
Multicomponent
reactions
(MCRs)
combine
at
least
three
reactants
to
afford
the
desired
product
in
a
highly
atom-economic
way
and
are
therefore
viewed
as
efficient
one-pot
combinatorial
synthesis
tools
allowing
one
significantly
boost
molecular
complexity
diversity.
Nowadays,
MCRs
no
longer
confined
organic
have
found
applications
materials
chemistry.
In
particular,
can
be
used
prepare
covalent
frameworks
(COFs),
which
crystalline
porous
assembled
from
monomers
exhibit
broad
range
of
properties
applications.
This
synthetic
approach
retains
advantages
small-molecule
MCRs,
not
only
strengthening
skeletal
robustness
COFs,
but
also
providing
additional
driving
forces
for
their
crystallization,
has
been
series
robust
COFs
with
diverse
The
present
perspective
article
provides
general
background
discusses
types
employed
COF
date,
addresses
related
critical
challenges
future
perspectives
inspire
MCR-based
design
new
promote
further
progress
this
emerging
field.
Journal of the American Chemical Society,
Journal Year:
2022,
Volume and Issue:
144(4), P. 1861 - 1871
Published: Jan. 20, 2022
Single
clusters
have
attracted
extensive
research
interest
in
the
field
of
catalysis.
However,
achieving
a
highly
uniform
dispersion
single-cluster
catalyst
is
challenging.
In
this
work,
for
first
time,
we
present
versatile
strategy
uniformly
dispersed
polyoxometalates
(POMs)
covalent
organic
frameworks
(COFs)
through
confining
POM
cluster
into
regular
nanopores
COF
by
linkage.
These
COF-POM
composites
combine
properties
light
absorption,
electron
transfer,
and
suitable
catalytic
active
sites;
as
result,
they
exhibit
outstanding
activity
artificial
photosynthesis:
that
is,
CO2
photoreduction
with
H2O
donor.
Among
them,
TCOF-MnMo6
achieved
highest
CO
yield
(37.25
μmol
g-1
h-1
ca.
100%
selectivity)
gas-solid
reaction
system.
Furthermore,
mechanism
study
based
on
density
functional
theory
(DFT)
calculations
demonstrated
photoinduced
transfer
(PET)
process
occurs
from
to
POM,
then
reduction
oxidation
occur
COF,
respectively.
This
work
developed
method
single
which
also
shows
potential
using
materials
photocatalysis.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: Feb. 27, 2023
Covalent
organic
frameworks
(COFs)
represent
an
emerging
class
of
photocatalysts.
However,
their
complicated
structures
lead
to
indeterminacy
about
photocatalytic
active
sites
and
reaction
mechanisms.
Herein,
we
use
reticular
chemistry
construct
a
family
isoreticular
crystalline
hydrazide-based
COF
photocatalysts,
with
the
optoelectronic
properties
local
pore
characteristics
COFs
modulated
using
different
linkers.
The
excited
state
electronic
distribution
transport
pathways
in
are
probed
host
experimental
methods
theoretical
calculations
at
molecular
level.
One
our
developed
(denoted
as
COF-4)
exhibits
remarkable
electron
utilization
efficiency
charge
transfer
properties,
achieving
record-high
uranium
extraction
performance
~6.84
mg/g/day
natural
seawater
among
all
techniques
reported
so
far.
This
study
brings
new
understanding
operation
COF-based
guiding
design
improved
photocatalysts
for
many
applications.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(15), P. 8364 - 8374
Published: March 14, 2023
Two-dimensional
covalent-organic
frameworks
(2D
COFs)
have
recently
emerged
as
great
prospects
for
their
applications
new
photocatalytic
platforms
in
solar-to-hydrogen
conversion;
nevertheless,
inefficient
solar
energy
capture
and
fast
charge
recombination
hinder
the
improvement
of
hydrogen
production
performance.
Herein,
two
photoactive
three-component
donor-π-acceptor
(TCDA)
materials
were
constructed
using
a
multicomponent
synthesis
strategy
by
introducing
electron-deficient
triazine
electron-rich
benzotrithiophene
moieties
into
through
sp2
carbon
imine
linkages,
respectively.
Compared
with
two-component
COFs,
novel
TCDA-COFs
are
more
convenient
regulating
inherent
photophysical
properties,
thereby
realizing
outstanding
activity
evolution
from
water.
Remarkably,
first
carbon-linked
TCDA-COF
displays
an
impressive
rate
70.8
±
1.9
mmol
g-1
h-1
excellent
reusability
presence
1
wt
%
Pt
under
visible-light
illumination
(420-780
nm).
Utilizing
combination
diversified
spectroscopy
theoretical
prediction,
we
show
that
full
π-conjugated
linkage
not
only
effectively
broadens
harvesting
COFs
but
also
enhances
transfer
separation
efficiency.
Chemical Society Reviews,
Journal Year:
2022,
Volume and Issue:
51(15), P. 6307 - 6416
Published: Jan. 1, 2022
This
review
highlights
the
recent
advances
of
metalated
covalent
organic
frameworks,
including
synthetic
strategies
and
applications,
discusses
current
challenges
future
directions.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(30)
Published: April 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,
Journal Year:
2022,
Volume and Issue:
61(15)
Published: Jan. 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.
Journal of the American Chemical Society,
Journal Year:
2021,
Volume and Issue:
143(46), P. 19446 - 19453
Published: Nov. 3, 2021
Development
of
new
porous
materials
as
hosts
to
suppress
the
dissolution
and
shuttle
lithium
polysulfides
is
beneficial
for
constructing
highly
efficient
lithium-sulfur
batteries
(LSBs).
Although
2D
covalent
organic
frameworks
(COFs)
host
exhibit
promising
potential
LSBs,
their
performance
still
not
satisfactory.
Herein,
we
develop
polyimide
COFs
(PI-COF)
with
a
well-defined
lamellar
structure,
which
can
be
exfoliated
into
ultrathin
(∼1.2
nm)
nanosheets
(PI-CONs)
large
size
(∼6
μm)
quantity
(40
mg/batch).
Explored
sulfur
PI-COF
PI-CONs
deliver
high
capacities
(1330
1205
mA
h
g-1
at
0.1
C,
respectively),
excellent
rate
capabilities
(620
503
4
superior
cycling
stability
(96%
capacity
retention
0.2
C
PI-CONs)
by
virtue
synergy
robust
conjugated
strong
oxygen-lithium
interactions,
surpassing
vast
majority
organic/polymeric
battery
cathodes
ever
reported.
Our
finding
demonstrates
that
COF
carbonyl
groups
could
LSBs
electrochemical
performance.
