Angewandte Chemie,
Journal Year:
2024,
Volume and Issue:
136(32)
Published: May 13, 2024
Abstract
Covalent
organic
frameworks
(COFs)
are
promising
photocatalysts
for
H
2
O
production
from
water
via
oxygen
reduction
reaction
(ORR).
The
design
of
COFs
efficient
indubitably
hinges
on
an
in‐depth
understanding
their
ORR
mechanisms.
In
this
work,
taking
imine‐linked
COF
as
example,
we
demonstrate
that
protonation
the
functional
units
such
imine,
amine,
and
triazine,
is
a
highly
strategy
to
upgrade
activity
levels
synthesis.
not
only
extends
light
absorption
but
also
provides
proton
sources
directly
participate
in
generation.
Notably,
simplifies
pathways
,
i.e.
indirect
superoxide
radical
(
)
mediated
route
direct
one‐step
two‐electron
route.
Theoretical
calculations
confirm
favors
synthesis
due
easy
access
protons
near
sites
removes
energy
barrier
generating
*OOH
intermediate.
These
findings
extend
mechanistic
insight
into
photosynthesis
provide
rational
guideline
upgradation
COFs.
Advanced Energy Materials,
Journal Year:
2024,
Volume and Issue:
14(23)
Published: April 3, 2024
Abstract
Solar
energy
can
be
utilized
in
photocatalysis
technology
to
realize
light‐driven
hydrogen
peroxide
(H
2
O
)
production,
a
green
chemical
synthesis
route.
Designing
high‐performance
photocatalysts
is
critical
achieving
practical
solar
H
production.
During
the
past
decade,
significant
research
progress
made
photocatalytic
materials
for
Particularly
2D
materials‐based
stand
out
due
their
unique
physical
and
properties.
This
review
highlights
intricate
relationship
between
material
innovation
photochemical
It
starts
with
fundamental
principles
of
generation,
focusing
on
crucial
steps
such
as
photon
absorption,
carrier
dynamics,
surface
reactions,
challenges
that
solve
at
each
step.
Then,
various
production
are
introduced
detail.
Engineering
strategies
optimize
performance
discussed
afterward.
Finally,
future
opportunities
designing
outlined.
expected
inspire
engineering
conversion
other
chemicals.
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
Angewandte Chemie International Edition,
Journal Year:
2024,
Volume and Issue:
63(32)
Published: May 13, 2024
Abstract
Covalent
organic
frameworks
(COFs)
are
promising
photocatalysts
for
H
2
O
production
from
water
via
oxygen
reduction
reaction
(ORR).
The
design
of
COFs
efficient
indubitably
hinges
on
an
in‐depth
understanding
their
ORR
mechanisms.
In
this
work,
taking
imine‐linked
COF
as
example,
we
demonstrate
that
protonation
the
functional
units
such
imine,
amine,
and
triazine,
is
a
highly
strategy
to
upgrade
activity
levels
synthesis.
not
only
extends
light
absorption
but
also
provides
proton
sources
directly
participate
in
generation.
Notably,
simplifies
pathways
,
i.e.
indirect
superoxide
radical
(
)
mediated
route
direct
one‐step
two‐electron
route.
Theoretical
calculations
confirm
favors
synthesis
due
easy
access
protons
near
sites
removes
energy
barrier
generating
*OOH
intermediate.
These
findings
extend
mechanistic
insight
into
photosynthesis
provide
rational
guideline
upgradation
COFs.
ACS Catalysis,
Journal Year:
2024,
Volume and Issue:
14(7), P. 5297 - 5304
Published: March 26, 2024
Photoelectrochemical
(PEC)
water
oxidation
to
hydrogen
peroxide
(H2O2)
is
an
alternative
route
the
conventional
anthraquinone
process,
but
it
still
restricted
by
prevailing
competitive
oxygen
evolution
reaction
(OER).
Here,
we
reveal
that
intrinsic
vacancies
(OVs)
of
BiVO4
photoanodes
are
detrimental
PEC
H2O2.
The
superabundant
OVs
photoanode
passivated
a
thermal
treatment
in
pressurized
O2
atmosphere
Parr
reactor.
with
least
OV
concentration
achieves
ca.
two
times
H2O2
selectivity
enhancement
than
introduced
OVs,
resulting
from
weakened
band
bending,
positively
shifted
quasi-Fermi
level,
and
suppressed
decomposition
as-formed
In
particular,
photoexcited
electrochemical
impedance
spectra
demonstrate
hole
distribution
rearrangement
OVs-passivated
BiVO4,
which
eliminates
OER-related
surface
states
steers
pathway
toward
formation.
This
work
reveals
importance
interfacial
energetics
induced
regulating
selective
oxidation.
