Advanced Functional Materials,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 2, 2025
Abstract
Inspired
by
the
mechanical
interlocking
principles
of
traditional
Chinese
mortise‐and‐tenon
structures,
a
3D
gradient
supramolecular
network
is
developed
through
oriented
self‐assembly
subphthalocyanine
(SubPc‐0)
arrays
on
La‐doped
Ag
3
PO
4
(La
0.01
2.99
).
This
bioinspired
design
synergistically
combines
π‐orbital
topological
extension
with
dynamic
B–La
coordination
bonds
to
construct
an
S‐scheme
heterojunction
dual‐phase
charge
modulation
capability.
Mechanistic
studies
reveal
that
La
3+
doping
induces
anisotropic
electron
delocalization
for
directional
bulk
transfer,
while
interfacial
coupling
establishes
ultrafast
(<10
ps)
atomic‐scale
transport
channels
orbital
hybridization.
The
optimized
SubPc‐0/La
system
demonstrates
2.2‐
and
2.1‐fold
improvements
in
tetracycline
oxytetracycline
degradation
efficiencies,
respectively,
94%
activity
retention
after
five
cycles.
Advanced
characterization
techniques
including
femtosecond
transient
absorption
spectroscopy
(fs‐TAS)
Kelvin
probe
force
microscopy
(KPFM),
combined
theoretical
calculations,
elucidated
intricate
photocatalytic
mechanism
transfer
pathways.
work
delivers
effective
strategy
mechanistic
insights
stacking
engineering
materials.
ACS Nano,
Год журнала:
2024,
Номер
18(31), С. 20435 - 20448
Опубликована: Июль 26, 2024
Photocatalytic
H2O2
production
has
attracted
much
attention
as
an
alternative
way
to
the
industrial
anthraquinone
oxidation
process
but
is
limited
by
weak
interaction
between
catalysts
and
reactants
well
inefficient
proton
transfer.
Herein,
we
report
on
a
hydrogen-bond-broken
strategy
in
carbon
nitride
for
enhancement
of
photosynthesis
without
any
sacrificial
agent.
The
promoted
hydrogen
bond
formation
exposed
N
atoms
H2O
molecules,
which
enhances
proton-coupled
electron
transfer
therefore
photocatalytic
activity.
serve
buffering
sites
from
molecules
nitride.
also
enhanced
through
adsorption
reduction
O2
gas
toward
because
nitrogen
vacancies
(NVs)
cyano
groups
after
intralayer
breaking
A
high
light-to-chemical
conversion
efficiency
(LCCE)
value
3.85%
achieved.
are
found
undergo
one-step
two-electron
pathway
photogenerated
hot
electrons
four-electron
produce
gas,
respectively.
Density
functional
theory
(DFT)
calculations
validate
reaction
pathways.
This
study
elucidates
significance
catalyst
reactants,
greatly
increases
tunneling
dynamics.
Increasing
active
sites
in
catalysts
is
of
utmost
importance
for
catalytic
processes.
In
this
regime,
single‐atom
dispersing
on
graphitic
carbon
nitrides
(g‐C
3
N
4
)
to
produce
fine
chemicals,
such
as
hydrogen
peroxide
(H
2
O
),
current
interest
due
not
only
enhancing
performance
but
also
reducing
the
loading
necessary
metals.
Herein,
g‐C
engineered
by
atomically
aluminum
(Al)
or
indium
(In)
provide
centers
via
one‐step
thermal
shock
polymerization.
The
addition
Al
and
can
accelerate
efficacy
owing
Lewis
acid–base
interactions
between
these
metals
oxygen
(O
).
Under
conditions,
formation
oxygenic
radicals
will
strongly
be
associated
with
enhanced
H
,
confirmed
situ
electron
paramagnetic
resonance
spectroscopy.
Furthermore,
empirical
analyses
from
positron
annihilation
spectroscopy
show
that
atoms
occupy
near
positions
vacancies
(V
C
form
NV
@InO
bonds.
This
replacement
highest
energy
based
density
functional
theory
calculations,
improving
stability
atom‐dispersive
materials.
Therefore,
combination
experimental
theoretical
proofs,
study
suggests
exact
location
structures,
which
help
boost
production
.
