Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 5, 2024
Abstract
Lithium
(Li)
metal
batteries
with
remarkable
energy
densities
are
restrained
by
short
lifetime
and
low
Coulombic
efficiency
(CE),
resulting
from
the
accumulative
Li
dendrites
dead
during
cycling.
Here,
we
prepared
a
new
three‐dimensional
(3D)
covalent
organic
framework
(COF)
dense
lithiophilic
sites
(heteoatom
weight
contents
of
32.32
wt
%)
as
an
anodic
protective
layer
batteries.
The
3D
COF
was
synthesized
using
[6+4]
synthesis
strategy
inducing
flexible
6‐connected
cyclotriphosphazene
derivative
aldehyde
4‐connected
porphyrin‐based
tetraphenylamines.
Both
phosphazene
porphyrin
rings
in
served
electron‐rich
sites,
enhancing
homogeneous
+
flux
via
direction
towards
highly
smooth
compact
deposition.
Li/Por‐PN‐COF‐Cu
cells
achieved
record
average
CE
99.1
%
for
320
cycles
Meanwhile,
abundant
can
promote
fast
transport
transference
number
0.87,
enabling
LiFePO
4
full
cell
stable
stripping/plating
processes
even
at
harsh
rate
5
C.
Theoretical
calculations
revealed
that
strong
interaction
force
between
facilitated
dissolution
electrolyte,
migration
barrier
1.08
eV
indicated
favorable
ions
π‐electron
system.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 5, 2024
Lithium
(Li)
metal
batteries
with
remarkable
energy
densities
are
restrained
by
short
lifetime
and
low
Coulombic
efficiency
(CE),
resulting
from
the
accumulative
Li
dendrites
dead
during
cycling.
Here,
we
prepared
a
new
three-dimensional
(3D)
covalent
organic
framework
(COF)
dense
lithiophilic
sites
(heteoatom
weight
contents
of
32.32
wt
%)
as
an
anodic
protective
layer
batteries.
The
3D
COF
was
synthesized
using
[6+4]
synthesis
strategy
inducing
flexible
6-connected
cyclotriphosphazene
derivative
aldehyde
4-connected
porphyrin-based
tetraphenylamines.
Both
phosphazene
porphyrin
rings
in
served
electron-rich
sites,
enhancing
homogeneous
Advanced Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: Nov. 27, 2024
Abstract
Photocatalysis
leverages
solar
energy
to
overcome
the
thermodynamic
barrier,
enabling
efficient
chemical
reactions
under
mild
conditions.
It
can
greatly
reduce
reliance
on
traditional
sources
and
has
attracted
significant
research
interest.
Reticular
materials,
including
metal‐organic
frameworks
(MOFs)
covalent
organic
(COFs),
represent
a
class
of
crystalline
materials
constructed
from
molecular
building
blocks
linked
by
coordination
bonds,
respectively.
function
as
heterogeneous
catalysts,
combining
well‐defined
structures
high
tailorability
akin
homogeneous
catalysts.
In
this
review,
regulation
light
absorption,
charge
separation,
surface
in
photocatalytic
process
through
precise
molecular‐level
design
based
features
reticular
is
elaborated.
Notably,
for
MOFsmicroenvironment
modulation
around
catalytic
sites
affects
performance
delved,
with
emphasis
their
unique
dynamic
flexible
microenvironments.
For
COFs,
inherent
excitonic
effects
due
fully
nature
discussed
highlight
strategies
regulate
charge‐
and/or
energy‐transfer‐mediated
photocatalysis.
Finally,
current
challenges
future
directions
field,
aiming
provide
comprehensive
understanding
how
be
optimized
enhanced
photocatalysis
discussed.
Advanced Energy Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Jan. 19, 2025
Abstract
Photocatalytic
H
2
O
synthesis
from
and
is
considered
to
be
one
of
the
most
promising
alternative
approaches
for
manufacturing
.
Developing
highly
active
selective
photocatalysts
significant
in
achieving
efficient
photosynthesis.
Herein,
an
ethynyl‐linked
donor–acceptor
covalent
organic
framework
(COF),
named
EBBT‐COF,
prepared
condensation
reaction
between
electron‐deficient
unit
4,4′,4″‐(1,3,5‐benzenetriyltri‐2,1‐ethynediyl)tris‐benzenamine
electron‐rich
benzo[1,2‐b:3,4‐b′:5,6‐b″]trithiophene‐2,5,8‐tricarboxaldehyde.
Powder
X‐ray
diffraction
N
adsorption
isotherm
unveil
crystalline
porous
hcb
network
EBBT‐COF
with
pores
size
centered
at
ca
2.3
nm.
Spectroscopic
characterizations
demonstrate
excellent
visible‐light
absorption
capacity
enhanced
photo‐induced
charge
separation
transport
efficiency
owing
its
architecture.
Density
functional
theory
calculations
electrochemical
tests
indicate
high
activity
selectivity
toward
2e
−
reduction
water
oxidation
triethynylbenzene
trithiophene
moieties
accelerate
‐to‐H
O‐to‐H
conversion,
respectively.
These
merits
enable
a
photocatalyst
generation
yield
rate
5
686
µmol
g
−1
h
,
optimal
apparent
quantum
15.14%,
solar‐to‐chemical
conversion
1.17%
(λ
>
400
nm),
representing
best
performance
among
COF‐based
reported
thus
far.
Angewandte Chemie International Edition,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 9, 2025
Photo/electro-catalytic
CO2
reduction
into
high-value
products
are
promising
strategies
for
addressing
both
environmental
problems
and
energy
crisis.
Duo
to
their
advantageous
visible
light
absorption
ability,
adjustable
optic/electronic
properties,
definite
active
center,
post-modification
capability,
excellent
stability,
porphyrin-based
covalent
organic
frameworks
(COFs)
have
emerged
as
attractive
photo/electro-catalysts
towards
reduction.
In
this
review,
the
research
progress
of
COFs
photo/electro-catalytic
is
summarized
including
design
principles,
catalytic
performance,
reaction
mechanism.
addition,
review
also
presents
some
challenges
prospects
application
in
reduction,
laying
base
fundamental
efforts.
Advanced Functional Materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 17, 2025
Abstract
The
5–10
nm
exciton
diffusion
distance
for
most
organic
semiconductors
is
much
less
than
the
particle
size
of
2D
covalent
frameworks
(COFs).
As
a
result,
local
structure
change
in
small
domain
COFs,
rather
whole
particles,
could
effectively
promote
charge
transfer
photocatalysis.
Herein,
three‐component
condensation
used
to
preparing
four
mixed
imine‐
and
thiazole‐linked
donor‐acceptor
(D–A)
COFs.
In
contrast
100%
imine
ca.
90%
10%
materials
have
77–95%
higher
photocatalytic
hydrogen
peroxide
(H
2
O
)
production
rate
pure
water
due
more
prolonged
lifetime
excitation
state.
particular,
USTB‐10‐S
exhibits
H
generation
5041
µmol
g
−1
h
.
Coupling
with
benzyl
alcohol
as
sacrificial
reagent,
its
further
increased
16152
,
superior
COF‐based
photocatalysts.
This
work
illustrates
proof‐of‐concept
that
COFs
tiny
amount
able
significantly
enhance
separation
thus
performance,
inspiring
development
defect
engineering
field
Energy & environment materials,
Journal Year:
2025,
Volume and Issue:
unknown
Published: March 31, 2025
Photocatalytic
technology
has
attracted
much
attention
in
the
fields
of
clean
energy
and
environmental
governance.
However,
how
to
design
develop
highly
efficient
photocatalytic
materials
remains
an
urgent
scientific
problem
be
solved.
This
study
focuses
on
enhancing
activity
through
microstructure
modification.
Among
them,
ToRed‐4
showed
most
prominent
performance.
Under
illumination
condition
420
nm,
its
value
was
13
506
μmol
g
−1
h
,
which
approximately
18
times
that
CN550
(bulk
g‐C
3
N
4
)
(719
).
By
using
DFT
calculations,
performance
deeply
analyzed,
revealing
significant
advantages
ToRed
series
key
indicators
underlying
synergy
mechanisms,
including
reduction
HOMO‐LUMO
gap,
separation
electron
holes,
expansion
electronic
transition
range,
transformation
electrostatic
potential
distribution,
increase
dipole
moment,
optimization
Coulomb
attractive
energy.
The
research
results
this
provide
a
basis
for
opening
up
new
avenues
development
are
expected
play
important
role
related
fields.
