The
concurrent
evolution
of
value-added
benzimidazole
compounds
and
hydrogen
within
the
domain
chemical
synthesis
is
paramount
importance.
utilization
photocatalysis
enhances
both
efficiency
environmental
benignity
synthetic
process.
However,
it
profoundly
challenging
a
photocatalytic
system
to
simultaneously
augment
number
active
sites
internal
transport
rate
photogenerated
charge
carriers.
To
address
this
issue,
template-free,
step-by-step
assembly
strategy
has
been
proposed
for
planar
crystalline
carbon
nitride
(CCN)
incorporated
with
nitrogen
vacancy
(Nv).
In
contrast
simultaneous
method,
sequential
process
encompasses
progressive
crystallization
mechanism.
This
method
conducive
mitigation
incidence
structural
disarray,
thereby
precluding
genesis
non-ordered
defects
throughout
whole
bulk
phase.
ordered
in-plane
arrangement
facilitates
spatial
segregation
electrons
holes,
decoupling
redox
sites.
separation
minimizes
likelihood
back
reactions
suppresses
recombination
process,
which
advantageous
coupling
reactions.
Certified
by
multiscale
characterization
theoretical
simulations,
incorporation
Nv
energy
band
structure
provides
unsaturated
coordination
adsorption
activation
ethanol
molecules.
interfacial
synergistic
effect
co-catalyst
Pt
as
Lewis
site
achieves
efficient
partners.
obtained
CCN
demonstrates
significant
bifunctional
activity,
achieving
yield
at
5.0
mmol
g-1
conversion
selectivity
99%.
Simultaneously,
measured
9.1
4
h.
assembled
utilized
in
study
new
perspectives
on
developing
highly
photocatalysts
molecular
level.
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.
Small,
Journal Year:
2025,
Volume and Issue:
unknown
Published: Feb. 21, 2025
Abstract
Efficient
separation
of
photogenerated
charges
at
the
surface
photocatalysts
is
vital
for
achieving
high
photocatalytic
activity.
Here,
a
Bi/Bi
4
NbO
8
Cl
heterostructure
piezo‐photocatalyst
with
an
amorphous/crystalline
interface
(acBi/BNC)
prepared
by
in
situ
reduction
using
Bi
as
self‐sacrificial
template.
This
ingenious
design
synergistically
utilizes
advantages
structure,
localized
plasmon
resonance
effect,
and
piezoelectric
field.
The
formation
interfaces
induces
generation
oxygen
vacancies,
subsequently
lattice
distortions,
thus
improving
properties.
Theoretical
experimental
results
demonstrate
that
combination
field
promotes
effective
migration
between
bulk
catalysts.
Under
simultaneous
light
ultrasound,
optimal
(acBi/BNC‐3)
exhibit
superior
photodegradation
efficiency
tetracycline
reached
80%
within
5
min,
reaction
rate
(2.78
×
10
−1
min
)
7.8
5.4
times
pure
(BNC)
crystalline
(cBi/BNC),
respectively.
Furthermore,
piezo‐photocatalytic
degradation
surpasses
those
under
individual
photocatalysis
piezocatalysis
conditions.
work
provides
novel
rational
to
improve
spatial
charge
Bi‐based
catalysts
prepare
high‐performance
piezo‐photocatalysts
via
engineering.
