Nano Letters,
Journal Year:
2024,
Volume and Issue:
24(18), P. 5444 - 5452
Published: April 19, 2024
We
report,
for
the
first
time,
a
new
synthetic
strategy
preparation
of
crystalline
two-dimensional
olefin-linked
covalent
organic
frameworks
(COFs)
based
on
aldol
condensation
between
benzodifurandione
and
aromatic
aldehydes.
Olefin-linked
COFs
can
be
facilely
crystallized
through
either
pyridine-promoted
solvothermal
process
or
benzoic
anhydride-mediated
flux
synthesis.
The
resultant
COF
leaf
with
high
in-plane
π-conjugation
exhibits
efficient
visible-light-driven
photoreduction
carbon
dioxide
(CO
Journal of CO2 Utilization,
Journal Year:
2024,
Volume and Issue:
81, P. 102727 - 102727
Published: March 1, 2024
In
the
face
of
escalating
global
climate
challenges,
effective
carbon
dioxide
(CO₂)
capture
techniques
remain
at
forefront
mitigating
anthropogenic
greenhouse
gas
emissions.
This
comprehensive
review
elucidates
latest
advancements
in
CO₂
capture,
emphasizing
two
predominant
methodologies:
absorption
and
adsorption.
We
delve
into
mechanisms
underlying
each
process,
highlighting
novel
materials
technologies
that
have
emerged
over
recent
years.
For
absorption,
focus
is
placed
on
material
design
strategy,
identifying
new
class
amines,
ionic
liquids
(ILs)
nanofluids
for
enhanced
CO2
capacities
reduced
energy
requirements.
realm
adsorption,
synthesis
innovative
adsorbents,
such
as
metal
organic
framework
(MOF),
polymers,
inorganic
silicon-based
biochar
byproducts
from
biomass
with
superior
selectivity
stability,
explored.
Additionally,
addresses
challenges
associated
method,
offering
insights
potential
avenues
further
research.
By
providing
a
holistic
overview
current
landscape
this
article
serves
pivotal
resource
researchers
industry
professionals
aiming
to
advance
sustainable
solutions
combat
change.
Advanced Functional Materials,
Journal Year:
2024,
Volume and Issue:
unknown
Published: March 10, 2024
Abstract
Covalent
organic
frameworks
(COFs)
attract
significant
attention
due
to
their
ordered,
crystalline,
porous,
metal‐free,
and
predictable
structures.
These
unique
characteristics
offer
great
opportunities
for
the
diffusion
transmission
of
photogenerated
charges
during
photocatalysis.
Currently,
a
considerable
number
COFs
are
used
as
metal‐free
semiconductor
photocatalysts.
This
review
aims
understand
relationships
between
structure
photocatalysis
performance
provides
in‐depth
insight
into
synthetic
strategy
improve
performance.
Subsequently,
focuses
on
structural
motif
in
sustainable
photocatalytic
hydrogen
evolution,
carbon
dioxide
reduction,
peroxide
generation,
compound
transformations.
Last,
conjunction
with
progress
achieved
challenges
yet
be
overcome,
candid
discussion
is
undertaken
regarding
field
COF
photocatalysis,
accompanied
by
presentation
potential
research
avenues
future
directions.
seeks
provide
readers
comprehensive
understanding
pivotal
role
robust
guidance
innovative
utilization
Advanced Energy Materials,
Journal Year:
2023,
Volume and Issue:
14(5)
Published: Dec. 11, 2023
Abstract
The
development
of
efficient
photocatalysts
for
artificial
photocatalytic
energy
conversion
is
an
intriguing
strategy.
Promisingly,
conjugated
polymers
(CPs)
have
been
actively
investigated
as
alternatives
to
traditional
inorganic
semiconductors
photocatalysis
due
their
molecularly
tunable
optoelectronic
properties,
thus
providing
a
great
platform
molecular
design.
Incorporating
donor
(D)
and
acceptor
(A)
units
into
the
backbone
CPs
ensures
adequate
D−A
interface,
which
essential
facilitating
charge
separation.
This
approach
also
allows
bandgaps
leading
significant
progress
in
conversions
recent
years.
Here,
fundamentals
D–A
type
are
initially
outlined,
followed
by
advanced
experimental
methods
density
functional
theory
(DFT)
calculations
investigating
carrier
dynamics.
Then,
detailed
exposition
synthetic
strategies
carried
out.
Their
extensive
applications
diverse
energy‐related
conversions,
such
hydrogen
evolution,
oxygen
overall
water
splitting,
CO
2
reduction,
N
H
O
evolution
comprehensively
presented.
review
provides
new
comprehensive
insights
molecular‐level
design
catalysts
boosted
conversion,
expected
further
advance
photocatalysis.
ACS Catalysis,
Journal Year:
2023,
Volume and Issue:
14(1), P. 138 - 147
Published: Dec. 12, 2023
Solar-driven
reduction
of
CO2
to
valuable
carbon
products
is
an
attractive
pathway
for
energy
production.
The
photoreduction
efficiency
determined
by
the
mass
transfer
and
charge
carrier
recombination
efficiency.
Herein,
we
propose
a
Bi2WO6–C3N4
heterojunction
with
hydrophobic–hydrophilic
diphase
promote
separation.
amphipathic
achieved
high-efficiency
photocatalytic
conversion
into
CO
CH4
in
H2O
vapor,
yielding
up
25.54
7.69
μmol
h–1
g–1
CH4,
respectively.
well-designed
increased
concentration
on
hydrophobic
surface
enhanced
adsorption
hydrophilic
surface.
Consequently,
reactant
gases
could
be
directly
fed
system
consume
photogenerated
charges.
In
situ
diffuse
reflectance
infrared
Fourier
transform
spectroscopy
molecular
dynamics
simulations
elucidated
activity
reaction
mechanism
during
photocatalysis.
serves
as
template
development
reliable
solar-powered
systems
reduction.
Journal of the American Chemical Society,
Journal Year:
2023,
Volume and Issue:
145(28), P. 15473 - 15481
Published: July 8, 2023
Three-dimensional
covalent
organic
frameworks
(3D
COFs),
with
interconnected
pores
and
exposed
functional
groups,
provide
new
opportunities
for
the
design
of
advanced
materials
through
postsynthetic
modification.
Herein,
we
demonstrate
successful
annulation
3D
COFs
to
construct
efficient
CO2
reduction
photocatalysts.
Two
COFs,
NJU-318
NJU-319Fe,
were
initially
constructed
by
connecting
hexaphenyl-triphenylene
units
pyrene-
or
Fe-porphyrin-based
linkers.
Subsequently,
moieties
within
postsynthetically
transformed
into
π-conjugated
hexabenzo-trinaphthylene
(pNJU-318
pNJU-319Fe)
enhance
visible
light
absorption
photoreduction
activity.
The
optimized
photocatalyst,
pNJU-319Fe,
shows
a
CO
yield
688
μmol
g-1,
representing
2.5-fold
increase
compared
that
unmodified
NJU-319Fe.
Notably,
direct
synthesis
hexabenzo-trinaphthylene-based
COF
catalysts
was
unsuccessful
due
low
solubility
conjugated
This
study
not
only
provides
an
effective
method
photocatalysts
but
also
highlights
unlimited
tunability
structural
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
34(43)
Published: Oct. 15, 2023
Abstract
Photochemical
CO
2
reduction
using
ubiquitous
sunlight
akin
to
natural
photosynthesis
is
an
effective
approach
for
conversion
of
renewable
energy
into
useful
chemical
feedstock.
Driven
by
the
need
earth‐abundant,
inexpensive,
and
sustainable
photocatalysts
with
practical
applicability,
covalent
organic
frameworks
(COFs)
have
emerged
as
a
new
generation
molecularly
defined
semiconductors
tunable
optoelectronic
properties.
These
reticular
highly
ordered,
porous
crystalline
structures
can
be
tailor‐made
covalently
combining
building
blocks
target
specific
functions.
To
date,
numerous
COFs
been
reported,
which
show
promising
activity
photocatalytic
allowing
derive
structure–property–function
relationships.
In
this
review,
different
reported
strategies
are
comprehensively
analyzed
categorized
active
site
engineering
in
COF
synthetic
rationale
resulting
catalytic
each
discussed.
The
recent
advancements
terms
tailored
photocatalyst
design
then
critically
assessed,
aspects
advanced
materials
characterization
analyzed,
future
perspectives
challenges
field
highlighted.
Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: June 26, 2024
Abstract
Suppressing
the
kinetically
favorable
lattice
oxygen
oxidation
mechanism
pathway
and
triggering
adsorbate
evolution
at
expense
of
activity
are
state-of-the-art
strategies
for
Ru-based
electrocatalysts
toward
acidic
water
oxidation.
Herein,
atomically
dispersed
Ru
species
anchored
into
an
stable
vinyl-linked
2D
covalent
organic
framework
with
unique
crossed
π-conjugation,
termed
as
COF-205-Ru.
The
π-conjugated
structure
COF-205-Ru
not
only
suppresses
dissolution
through
strong
Ru-N
motifs,
but
also
reduces
state
by
multiple
π-conjugations,
thereby
activating
coordinated
to
stabilizing
vacancies
during
process.
Experimental
results
including
X-ray
absorption
spectroscopy,
in
situ
Raman
powder
diffraction
patterns,
theoretical
calculations
unveil
activated
elevated
energy
level
O
2
p
band,
decreased
vacancy
formation
energy,
promoted
electrochemical
stability,
significantly
reduced
barrier
potential
determining
step
Consequently,
obtained
displays
a
high
mass
2659.3
A
g
−1
,
which
is
32-fold
higher
than
commercial
RuO
retains
long-term
durability
over
280
h.
This
work
provides
strategy
simultaneously
promote
stability
catalysts