The Journal of Physical Chemistry Letters,
Journal Year:
2023,
Volume and Issue:
14(34), P. 7690 - 7696
Published: Aug. 22, 2023
Artificial
photosynthesis
of
H2O2
by
TiO2-based
semiconductors
is
a
promising
approach
for
production.
However,
the
efficiency
pristine
TiO2
still
limited
rapid
charge
separation
and
low
O2
adsorption
capacity.
Here,
we
found
that
synergy
between
bulk
surface
defects
on
could
overcome
this
demanding
bottleneck.
The
introduced
act
as
hole
acceptors
to
induce
directional
transfer,
efficiently
boosting
electron-hole
separation.
Furthermore,
strengthened
defects.
Consequently,
significantly
improves
photocatalytic
performance,
with
production
rate
4560
μmol
h-1
g-1,
outperforming
most
reported
photocatalysts.
This
work
not
only
provides
new
insight
into
mechanism
surface/bulk
in
photocatalysis
but
also
highlights
regulation
holds
great
promise
achiveing
efficient
conversion.
Angewandte Chemie International Edition,
Journal Year:
2023,
Volume and Issue:
62(26)
Published: April 25, 2023
Abstract
Photocatalytic
oxygen
reduction
reaction
(ORR)
offers
a
promising
hydrogen
peroxide
(H
2
O
)
synthetic
strategy,
especially
the
one‐step
two‐electron
(2e
−
ORR
route
holds
great
potential
in
achieving
highly
efficient
and
selectivity.
However,
2e
is
rarely
harvested
underlying
mechanism
for
regulating
pathways
remains
greatly
obscure.
Here,
by
loading
sulfone
units
into
covalent
organic
frameworks
(FS‐COFs),
we
present
an
photocatalyst
H
generation
via
from
pure
water
air.
Under
visible
light
irradiation,
FS‐COFs
exert
superb
yield
of
3904.2
μmol
h
−1
g
,
outperforming
most
reported
metal‐free
catalysts
under
similar
conditions.
Experimental
theoretical
investigation
reveals
that
accelerate
separation
photoinduced
electron‐hole
(e
‐h
+
pairs,
enhance
protonation
COFs,
promote
adsorption
Yeager‐type,
which
jointly
alters
process
two‐step
to
one,
thereby
with
high
Advanced Functional Materials,
Journal Year:
2023,
Volume and Issue:
34(12)
Published: Dec. 6, 2023
Abstract
As
a
chemical
product
with
rapidly
expanding
demand
in
the
field
of
modern
energy
and
environmental
applications,
hydrogen
peroxide
(H
2
O
)
has
garnered
widespread
attention.
However,
existing
industrial
production
H
is
plagued
by
high
consumption,
harmful
waste
emission,
severe
safety
issues,
making
it
difficult
to
satisfy
environmental/economic
concept.
Artificial
photosynthesis
offers
viable
strategy
for
green
sustainable
since
uses
sunlight
as
an
source
initiate
reaction
oxygen
water
produce
.
Among
various
photocatalysts,
covalent
organic
frameworks
(COFs),
featuring
highly
ordered
skeletons
well‐defined
active
sites,
have
emerged
promising
photocatalysts
production.
This
review
presents
nascent
burgeoning
area
photocatalytic
based
on
COFs.
First,
brief
overview
technology
provided,
followed
detailed
introduction
principles
evaluation
generation.
Subsequently,
latest
research
progress
judicious
design
COFs
expounded,
particular
emphasis
manipulating
electronic
structures
redox
sites.
Finally,
outlook
challenges
future
opportunities
proposed,
hope
stimulating
further
explorations
novel
molecular‐designed
photosynthesis.
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(22)
Published: Feb. 28, 2024
Abstract
The
solar‐driven
photocatalytic
production
of
hydrogen
peroxide
(H
2
O
)
from
water
and
oxygen
using
semiconductor
catalysts
offers
a
promising
approach
for
converting
solar
energy
into
storable
chemical
energy.
However,
the
efficiency
H
is
often
restricted
by
low
photo‐generated
charge
separation,
slow
surface
reactions
inadequate
stability.
Here,
we
developed
mixed‐linker
strategy
to
build
donor‐acceptor‐acceptor
(D–A–A)
type
covalent
organic
framework
(COF)
photocatalyst,
FS‐OHOMe‐COF.
FS‐OHOMe‐COF
structure
features
extended
π–π
conjugation
that
improves
mobility,
while
introduction
sulfone
units
not
only
as
active
sites
facilitates
with
but
also
bolsters
stability
through
increased
interlayer
forces.
resulting
has
exciton
binding
energy,
long
excited‐state
lifetime
high
photo‐stability
leads
performance
(up
1.0
mM
h
−1
an
output
19
after
72
hours
irradiation.
Furthermore,
catalyst
demonstrates
stability,
which
sustained
activity
over
192
experiment.
Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: March 26, 2024
Hydrogen
peroxide
photosynthesis
suffers
from
insufficient
catalytic
activity
due
to
the
high
energy
barrier
of
hydrogen
extraction
H2O.
Herein,
we
report
that
mechanochemically
synthesized
keto-form
anthraquinone
covalent
organic
framework
which
is
able
directly
synthesize
H2O2
(4784
μmol
h-1
g-1
at
λ
>
400
nm)
oxygen
and
alkaline
water
(pH
=
13)
in
absence
any
sacrificial
reagents.
The
strong
alkalinity
resulted
formation
OH-(H2O)n
clusters
water,
were
adsorbed
on
keto
moieties
within
then
dissociated
into
O2
active
hydrogen,
because
was
largely
lowered.
produced
reacted
with
generate
anthrahydroquinone,
subsequently
oxidized
by
produce
H2O2.
This
study
ultimately
sheds
light
importance
H2O
for
demonstrates
synthesis
achievable
under
conditions.
Proceedings of the National Academy of Sciences,
Journal Year:
2023,
Volume and Issue:
120(6)
Published: Feb. 2, 2023
Photosynthesis
of
hydrogen
peroxide
(H2O2)
by
selective
oxygen
reduction
is
a
green
and
cost-effective
alternative
to
the
energy-intensive
anthraquinone
process.
Although
inexpensive
polymeric
graphitic
carbon
nitride
(g-C3N4)
exhibits
ability
produce
H2O2,
its
disordered
amorphous
structure
leads
high
recombination
rate
photogenerated
carriers
hinders
charge
transfer
between
layers.
Herein,
we
predict
that
stacked
g-C3N4
with
ion
intercalation
(K+
I-)
can
improve
carrier
separation
multiscale
computational
simulations.
The
electronic
structures
were
tailored
modified
intercalating
K+
I-
into
layer-by-layer
structures.
Guided
predictions,
achieved
efficient
solar-driven
H2O2
production
employing
this
facile
ion-intercalated
crystalline
g-C3N4.
An
13.1
mM
g-1
h-1
an
apparent
quantum
yield
23.6%
at
400
nm
obtained.
synergistic
effects
crystallinity
regulation
dual
interstitial
doping
engineering
triggered
formation
new
light
absorption
centers,
establishment
rapid
diffusion
channels,
enhancement
two-electron
characteristics.
This
work
sheds
on
tuning
broadens
design
principles
organic-conjugated
polymer
photocatalysts
for
environmental
remediation
energy
conservation.
Nature Communications,
Journal Year:
2024,
Volume and Issue:
15(1)
Published: June 22, 2024
Abstract
Circumventing
the
conventional
two-electron
oxygen
reduction
pathway
remains
a
great
problem
in
enhancing
efficiency
of
H
2
O
photosynthesis.
A
promising
approach
to
achieve
outstanding
photocatalytic
activity
involves
utilization
redox
intermediates.
Here,
we
engineer
polyimide
aerogel
photocatalyst
with
photoreductive
carbonyl
groups
for
non-sacrificial
production.
Under
photoexcitation,
on
surface
are
reduced,
forming
an
anion
radical
intermediate.
The
produced
intermediate
is
oxidized
by
produce
and
subsequently
restores
group.
high
catalytic
ascribed
cycle
mediated
anion,
which
not
only
promotes
adsorption
but
also
lowers
energy
barrier
reaction
generation.
An
apparent
quantum
yield
14.28%
at
420
±
10
nm
solar-to-chemical
conversion
0.92%
achieved.
Moreover,
demonstrate
that
mere
0.5
m
self-supported
exposed
natural
sunlight
6
h
yields
significant
production
34.3
mmol
−2
.
