Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(49)
Published: Oct. 26, 2023
The
semiconducting
properties
and
applications
of
three
dimensional
(3D)
covalent
organic
frameworks
(COFs)
are
greatly
hampered
because
their
long-ranged
non-conjugated
skeletons
relatively
unstable
linkages.
Here,
a
robust
imidazole-linked
fully
conjugated
3D
framework
(BUCT-COF-7)
is
synthesized
through
the
one-pot
multicomponent
Debus-Radziszewski
reaction
saddle-shaped
aldehyde-substituted
cyclooctatetrathiophene,
pyrene-4,5,9,10-tetraone,
ammonium
acetate.
BUCT-COF-7,
as
metal-free
catalyst,
shows
excellent
two
electron
oxygen
reduction
(ORR)
activity
in
alkaline
medium
with
high
hydrogen
peroxide
(H2
O2
)
selectivity
83.4
%.
When
BUCT-COF-7
cathode
catalyst
assembled
into
electrolyzer,
devices
showed
electrochemical
production
rate
H2
up
to
326.9
mmol
g-1
h-1
.
accumulative
amount
could
totally
degrade
dye
methylene
blue
via
Fenton
for
wastewater
treatment.
This
first
report
about
intrinsic
COFs
efficient
synthesis
,
revealing
promising
environment-related
field.
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
13(10)
Published: Jan. 20, 2023
Abstract
Lithium–sulfur
batteries
are
recognized
as
one
of
the
most
promising
next‐generation
energy‐storage
technologies
owing
to
their
high
energy
density
and
low
cost.
Nevertheless,
shuttle
effect
polysulfide
intermediates
formation
lithium
dendrites
principal
reasons
that
restrict
practical
adoption
current
Li–S
batteries.
Adjustable
frameworks,
structural
variety,
functional
adaptability
covalent
organic
frameworks
(COFs)
have
potential
overcome
issues
associated
with
battery
technology.
Herein,
a
summary
is
presented
emerging
COF
materials
in
addressing
challenging
problems
terms
sulfur
hosts,
modified
separators,
artificial
solid
electrolyte
interphase
layers,
solid‐state
electrolytes.
This
comprehensive
overview
focuses
on
design
chemistry
COFs
used
upgrade
Furthermore,
existing
difficulties,
prospective
remedies,
research
directions
for
discussed,
laying
groundwork
future
advancements
this
class
fascinating
materials.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(19), P. 6715 - 6753
Published: Jan. 1, 2023
This
review
not
only
highlights
the
progress
of
emission
and
electronic
behaviour
new
pyrene-based
luminescence
molecules
in
aggregated
state,
but
also
provides
a
perspective
for
understanding
mechanism
optoelectronic
properties
pyrenes.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: June 26, 2023
To
achieve
high-efficiency
catalysts
for
CO2
reduction
reaction,
various
catalytic
metal
centres
and
linker
molecules
have
been
assembled
into
covalent
organic
frameworks.
The
amine-linkages
enhance
the
binding
ability
of
molecules,
ionic
frameworks
enable
to
improve
electronic
conductivity
charge
transfer
along
However,
directly
synthesis
with
is
hardly
achieved
due
electrostatic
repulsion
predicament
strength
linkage.
Herein,
we
demonstrate
reaction
by
modulating
linkers
linkages
template
framework
build
correlation
between
performance
structures
Through
double
modifications,
states
are
well
tuned,
resulting
in
controllable
activity
selectivity
reaction.
Notably,
dual-functional
achieves
high
a
maximum
CO
Faradaic
efficiency
97.32%
turnover
frequencies
value
9922.68
h-1,
which
higher
than
those
base
single-modified
Moreover,
theoretical
calculations
further
reveal
that
attributed
easier
formation
immediate
*CO
from
COOH*.
This
study
provides
insights
developing
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:
2023,
Volume and Issue:
145(14), P. 8141 - 8149
Published: March 29, 2023
Lithium-sulfur
batteries
(LSBs)
have
been
considered
as
a
promising
candidate
for
next-generation
energy
storage
devices,
which
however
still
suffer
from
the
shuttle
effect
of
intermediate
lithium
polysulfides
(LiPSs).
Covalent-organic
frameworks
(COFs)
exhibited
great
potential
sulfur
hosts
LSBs
to
solve
such
problem.
Herein,
pentiptycene-based
D2h
symmetrical
octatopic
polyaldehyde,
6,13-dimethoxy-2,3,9,10,18,19,24,25-octa(4'-formylphenyl)pentiptycene
(DMOPTP),
was
prepared
and
utilized
building
block
toward
preparing
COFs.
Condensation
DMOPTP
with
4-connected
tetrakis(4-aminophenyl)methane
affords
an
expanded
[8
+
4]
connected
network
3D-flu-COF,
flu
topology.
The
non-interpenetrated
nature
topology
endows
3D-flu-COF
high
Brunauer-Emmett-Teller
surface
area
2860
m2
g-1,
large
octahedral
cavities,
cross-linked
tunnels
in
framework,
enabling
loading
capacity
(∼70
wt
%),
strong
LiPS
adsorption
capability,
facile
ion
diffusion.
Remarkably,
when
used
host
LSBs,
delivers
1249
mA
h
g-1
at
0.2
C
(1.0
=
1675
g-1),
outstanding
rate
capability
(764
5.0
C),
excellent
stability,
representing
one
best
results
among
thus
far
reported
COF-based
materials
being
competitive
state-of-the-art
inorganic
materials.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(25), P. 13494 - 13513
Published: June 12, 2023
Redox-active
covalent
organic
frameworks
(COFs)
have
recently
emerged
as
advanced
electrodes
in
polymer
batteries.
COFs
provide
ideal
molecular
precision
for
understanding
redox
mechanisms
and
increasing
the
theoretical
charge-storage
capacities.
Furthermore,
functional
groups
on
pore
surface
of
highly
ordered
easily
accessible
interaction
sites,
which
can
be
modeled
to
establish
a
synergy
between
ex
situ/in
situ
mechanism
studies
computational
methods,
permitting
creation
predesigned
structure–property
relationships.
This
perspective
integrates
categorizes
functionalities
COFs,
providing
deeper
mechanistic
investigation
guest
ion
interactions
Additionally,
it
highlights
tunable
electronic
structural
properties
that
influence
activation
reactions
this
promising
electrode
material.
Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(13), P. 9385 - 9394
Published: March 21, 2024
The
shuttling
of
polysulfides
on
the
cathode
and
uncontrollable
growth
lithium
dendrites
anode
have
restricted
practical
application
lithium–sulfur
(Li–S)
batteries.
In
this
study,
a
metal-coordinated
3D
covalent
organic
framework
(COF)
with
homogeneous
distribution
nickel–bis(dithiolene)
N-rich
triazine
centers
(namely,
NiS4-TAPT)
was
designed
synthesized,
which
can
serve
as
bifunctional
hosts
for
both
sulfur
cathodes
anodes
in
Li–S
abundant
Ni
N-sites
NiS4-TAPT
greatly
enhance
adsorption
conversion
polysulfides.
Meanwhile,
presence
Ni–bis(dithiolene)
enables
uniform
Li
nucleation
at
anode,
thereby
suppressing
dendrites.
This
work
demonstrated
effectiveness
integrating
catalytic
sites
to
optimize
chemical
interactions
between
host
materials
redox-active
intermediates,
potentially
facilitating
rational
design
COF
high-performance
secondary
ACS Nano,
Journal Year:
2023,
Volume and Issue:
18(1), P. 28 - 66
Published: Dec. 20, 2023
Covalent
organic
frameworks
(COFs)
have
attracted
considerable
interest
in
the
field
of
rechargeable
batteries
owing
to
their
three-dimensional
(3D)
varied
pore
sizes,
inerratic
porous
structures,
abundant
redox-active
sites,
and
customizable
structure-adjustable
frameworks.
In
context
metal-ion
batteries,
these
materials
play
a
vital
role
electrode
materials,
effectively
addressing
critical
issues
such
as
low
ionic
conductivity,
limited
specific
capacity,
unstable
structural
integrity.
However,
electrochemical
characteristics
developed
COFs
still
fall
short
practical
battery
requirements
due
inherent
electronic
tradeoff
between
capacity
redox
potential,
unfavorable
micromorphology.
This
review
provides
comprehensive
overview
recent
advancements
application
COFs,
COF-based
composites,
derivatives
including
lithium-ion,
lithium-sulfur,
sodium-ion,
sodium-sulfur,
potassium-ion,
zinc-ion,
other
multivalent
batteries.
The
operational
mechanisms
are
elucidated,
along
with
strategies
implemented
enhance
properties
broaden
range
applications.
Chemical Reviews,
Journal Year:
2024,
Volume and Issue:
124(8), P. 4935 - 5118
Published: April 10, 2024
Rechargeable
metal-sulfur
batteries
are
considered
promising
candidates
for
energy
storage
due
to
their
high
density
along
with
natural
abundance
and
low
cost
of
raw
materials.
However,
they
could
not
yet
be
practically
implemented
several
key
challenges:
(i)
poor
conductivity
sulfur
the
discharge
product
metal
sulfide,
causing
sluggish
redox
kinetics,
(ii)
polysulfide
shuttling,
(iii)
parasitic
side
reactions
between
electrolyte
anode.
To
overcome
these
obstacles,
numerous
strategies
have
been
explored,
including
modifications
cathode,
anode,
electrolyte,
binder.
In
this
review,
fundamental
principles
challenges
first
discussed.
Second,
latest
research
on
is
presented
discussed,
covering
material
design,
synthesis
methods,
electrochemical
performances.
Third,
emerging
advanced
characterization
techniques
that
reveal
working
mechanisms
highlighted.
Finally,
possible
future
directions
practical
applications
This
comprehensive
review
aims
provide
experimental
theoretical
guidance
designing
understanding
intricacies
batteries;
thus,
it
can
illuminate
pathways
progressing
high-energy-density
battery
systems.