Journal of the American Chemical Society,
Journal Year:
2024,
Volume and Issue:
146(5), P. 3396 - 3404
Published: Jan. 24, 2024
Covalent
organic
frameworks
(COFs),
with
the
features
of
flexible
structure
regulation
and
easy
introduction
functional
groups,
have
aroused
broad
interest
in
field
photocatalysis.
However,
due
to
low
light
absorption
intensity,
photoelectron
conversion
efficiency,
lack
suitable
active
sites,
it
remains
a
great
challenge
achieve
efficient
photocatalytic
aerobic
oxidation
reactions.
Herein,
based
on
reticular
chemistry,
we
rationally
designed
series
three-motif
molecular
junction
type
COFs,
which
formed
dual
photosensitizer
coupled
redox
junctions
containing
multifunctional
COF
photocatalysts.
Significantly,
strong
adsorption
ability
units
integrated
reduction
features,
PY-BT
exhibited
highest
activity
for
oxidation.
Especially,
achieved
benzylamine
efficiency
99.9%
2.5
h,
is
much
higher
than
that
two-motif
only
one
or
unit
lacking
COFs.
The
mechanism
selective
was
studied
through
comprehensive
experiments
density
theory
calculations.
results
showed
photoinduced
electron
transfer
occurred
from
PY
then
triphenylamine
BT.
Furthermore,
thermodynamics
energy
lower
others,
confirmed
synergistic
effect
This
work
provided
new
strategy
design
COFs
also
represented
insight
into
catalytic
Advanced Functional Materials,
Journal Year:
2022,
Volume and Issue:
32(52)
Published: Oct. 17, 2022
Abstract
This
study
proposes
a
strategy
based
on
heterovalent
ion
doping
that
gives
rise
to
synergistic
piezo‐phototronic
effect
with
significantly
improved
catalytic
activity
and
leads
selective
enhancement
for
specific
pollutants.
Owing
the
enhanced
light
absorption,
hydrogen
evolution
rates
are
as
high
3704
3178
µmolg
−1
h
in
0.01Li‐doped
BaTiO
3
0.02La‐doped
nanosheets,
respectively,
under
simultaneous
irradiation
by
ultrasound
light,
factor
of
4.6
3.9
times
higher
than
pure
.
The
performance
also
far
exceeds
single
piezocatalysis,
photocatalysis,
or
sum
two
Li/La‐doped
nanosheets
due
effects
piezoelectric
field
promoting
photo‐induced
separation
electron‐hole
pairs.
Further,
carefully
selecting
donor
acceptor
doping,
significant
catalyst
pollutants
is
obtained
controlling
band
structure.
Compared
,
possesses
anionic
dyes
such
Methyl
blue
Malachite
Green,
reaching
0.067
1.379
min
while
exhibits
better
cationic
Rhodamine
B
Orange,
degradation
up
0.274
0.029
respectively.
offers
path
design
efficient
piezocatalysts
applications.
Chemical Society Reviews,
Journal Year:
2023,
Volume and Issue:
52(22), P. 7949 - 8004
Published: Jan. 1, 2023
Photocatalytic
organic
reactions,
harvesting
solar
energy
to
produce
high
value-added
chemicals,
have
attracted
increasing
attention
as
a
sustainable
approach
address
the
global
crisis
and
environmental
issues.
Reticular
framework
materials,
including
metal-organic
frameworks
(MOFs)
covalent
(COFs),
are
widely
considered
promising
candidates
for
photocatalysis
owing
their
crystallinity,
tailorable
pore
environment
extensive
structural
diversity.
Although
design
synthesis
of
MOFs
COFs
been
intensively
developed
in
last
20
years,
applications
photocatalytic
transformations
still
preliminary
stage,
making
systematic
summary
necessary.
Thus,
this
review
aims
provide
comprehensive
understanding
useful
guidelines
exploration
suitable
MOF
COF
photocatalysts
towards
appropriate
reactions.
The
commonly
used
reactions
categorized
facilitate
identification
reaction
types.
From
practical
viewpoint,
fundamentals
experimental
design,
active
species,
performance
evaluation
external
conditions,
discussed
detail
easy
experimentation.
Furthermore,
latest
advances
COFs,
composites,
comprehensively
summarized
according
actual
sites,
together
with
discussion
structure-property
relationship.
We
believe
that
study
will
be
helpful
researchers
novel
reticular
various
synthetic
applications.
Advanced Healthcare Materials,
Journal Year:
2023,
Volume and Issue:
12(23)
Published: May 13, 2023
Abstract
The
increase
in
antibiotic
resistance
promotes
the
situation
of
developing
new
antibiotics
at
forefront,
while
development
non‐antibiotic
pharmaceuticals
is
equally
significant.
In
post‐antibiotic
era,
nanomaterials
with
high
antibacterial
efficiency
and
no
drug
make
them
attractive
candidates
for
materials.
Carbon
dots
(CDs),
as
a
kind
carbon‐based
zero‐dimensional
nanomaterial,
are
attracting
much
attention
their
multifunctional
properties.
abundant
surface
states,
tunable
photoexcited
excellent
photo‐electron
transfer
properties
sterilization
CDs
feasible
gradually
emerging
field.
This
review
provides
comprehensive
insights
into
recent
topics
include
mechanisms,
design,
optimization
processes,
potential
practical
applications
also
highlighted,
such
treatment
bacterial
infections,
against
biofilms,
surfaces,
food
preservation,
bacteria
imaging
detection.
Meanwhile,
challenges
outlook
field
discussed
proposed.
Carbon Energy,
Journal Year:
2022,
Volume and Issue:
5(2)
Published: May 18, 2022
Abstract
The
persistent
increase
of
CO
2
levels
in
the
atmosphere,
already
exceeding
400
ppm,
urges
exploration
emission
reduction
and
recycling
technologies.
Ideally,
photocatalytic
conversion
into
valuable
hydrocarbons
realizes
solar‐to‐chemical
energy
conversion,
which
is
a
desirable
“kill
two
birds
with
one
stone”
strategy;
namely,
photoreduction
can
simultaneously
tackle
shortage
keep
global
carbon
balance.
Graphitic
nitride
(g‐C
3
N
4
)
working
on
reaction
deserves
highlight
not
only
for
metal‐free
feature
that
endows
it
low
cost,
tunable
electronic
structure,
easy
fabrication
properties
but
also
because
its
strong
ability.
present
review
concisely
summarizes
latest
advances
g‐C
‐based
photocatalysts
toward
reduction.
It
starts
discussion
thermodynamics
dynamics
aspects
process.
Then
modification
strategies
to
promote
have
been
discussed
detail,
including
surface
functionalization,
molecule
structure
engineering,
crystallization,
morphology
loading
cocatalyst,
constructing
heterojunction.
Meanwhile,
intrinsic
factors
affecting
activity
selectivity
are
analyzed
summarized.
In
end,
challenges
prospects
future
development
highly
presented.
Deleted Journal,
Journal Year:
2022,
Volume and Issue:
1, P. e9120006 - e9120006
Published: May 12, 2022
Organic
synthesis
driven
by
heterogeneous
catalysis
is
a
central
research
theme
to
both
fundamental
and
industrial
production
of
fine
chemicals.
However,
the
employment
stoichiometric
strong
oxidizing
or
reducing
reagents
(e.g.,
K2Cr2O7
LiAlH4)
harsh
reaction
conditions
high
temperature
pressure)
always
leads
products
overreaction
other
by-product
residues
salt
acid
waste).
Thus
poor
control
product
selectivity
tremendous
energy
consumption
result
in
urgent
demand
develop
novel
technologies
for
catalysis.
Given
current
global
development
CO2
reduction
sustainable
utilization,
one
promising
protocol
photocatalysis.
It
enables
solar-to-chemical
conversion
under
mild
room
temperature,
ambient
pressure,
air
as
oxidant)
offers
unique
pathways
improved
control.
To
accurately
tailor
desired
products,
electronic
structure
positions
valence-band
maximum
conduction-band
minimum),
geometric
nanorod,
nanosheet,
porous
morphology),
surface
chemical
micro-environment
vacancy
sites
co-catalysts)
photocatalysts
require
rational
design
construction.
In
this
review,
we
will
briefly
analyze
some
effective
photocatalytic
systems
with
excellent
regulation
ability
organic
transformations
(mainly
oxidation
types)
visible
light
irradiation,
put
forward
opinions
on
optimal
fabrication
nanostructured
realize
selective
synthesis.
Nature Communications,
Journal Year:
2023,
Volume and Issue:
14(1)
Published: May 10, 2023
Direct
solar-driven
methane
(CH4)
reforming
is
highly
desirable
but
challenging,
particularly
to
achieve
a
value-added
product
with
high
selectivity.
Here,
we
identify
synergistic
ensemble
effect
of
atomically
dispersed
copper
(Cu)
species
and
partially
reduced
tungsten
(Wδ+),
stabilised
over
an
oxygen-vacancy-rich
WO3,
which
enables
exceptional
photocatalytic
CH4
conversion
formaldehyde
(HCHO)
under
visible
light,
leading
nearly
100%
selectivity,
very
yield
4979.0
μmol·g-1
within
2
h,
the
normalised
mass
activity
8.5
×
106
μmol·g-1Cu·h-1
HCHO
at
ambient
temperature.
In-situ
EPR
XPS
analyses
indicate
that
Cu
serve
as
electron
acceptor,
promoting
photo-induced
transfer
from
conduction
band
O2,
generating
reactive
•OOH
radicals.
In
parallel,
adjacent
Wδ+
act
hole
acceptor
preferred
adsorption
activation
site
H2O
produce
hydroxyl
radicals
(•OH),
thus
activate
methyl
(•CH3).
The
synergy
dual
active
sites
boosts
overall
efficiency
selectivity
process.
Environmental Science & Technology,
Journal Year:
2024,
Volume and Issue:
58(24), P. 10415 - 10444
Published: June 7, 2024
Persulfate
(PS)-based
advanced
oxidation
processes
(AOPs)
for
pollutant
removal
have
attracted
extensive
interest,
but
some
controversies
about
the
identification
of
reactive
species
were
usually
observed.
This
critical
review
aims
to
comprehensively
introduce
basic
concepts
and
rectify
cognitive
biases
appeals
pay
more
attention
experimental
details
in
PS-AOPs,
so
as
accurately
explore
reaction
mechanisms.
The
scientifically
summarizes
character,
generation,
different
species.
It
then
highlights
complexities
analysis
electron
paramagnetic
resonance,
uncertainties
use
probes
scavengers,
necessities
determination
scavenger
concentration.
importance
choice
buffer
solution,
operating
mode,
terminator,
filter
membrane
is
also
emphasized.
Finally,
we
discuss
current
challenges
future
perspectives
alleviate
misinterpretations
toward
mechanisms
PS-AOPs.