ACS Materials Letters,
Год журнала:
2023,
Номер
5(3), С. 694 - 703
Опубликована: Янв. 31, 2023
Covalent
organic
frameworks
(COFs)
have
attracted
much
attention
in
porous
materials
because
of
their
structural
tunability
and
stability.
However,
the
problems
low
transmittance
large
light
scattering
due
to
difficulty
powder
phase
processing
severely
limited
practical
applications
third-order
nonlinear
optics
(NLO).
Herein,
we
report
first
successful
synthesis
a
series
donor–acceptor
(D–A)
COFs
films
(thickness
∼100
nm)
with
uniform
transparency
narrow
optical
band
gap
by
solvothermal
solid–liquid
interface
methods
for
NLO
applications.
Most
importantly,
designed
PT–PA
film
exhibits
excellent
performance,
including
normalized
transmission
value
∼2.55
at
beam
focus,
modulation
depth
(As)
139%,
high
absorption
coefficient
(β)
1.83
×
106
cm
GW–1
pulse
energy
1
μJ,
which
is
superior
most
recently
reported
materials.
The
properties
are
mainly
attributed
homogeneous
extended-ordered
conjugated
structure
films,
enhance
charge
transfer
structures
thus
yield
behavior.
This
work
provides
an
option
development
high-performance
devices
opens
new
path
future
fields.
Advanced Materials,
Год журнала:
2023,
Номер
35(26)
Опубликована: Март 25, 2023
Photocatalytic
CO2
conversion
for
hydrocarbon
fuel
production
has
been
known
as
one
of
the
most
promising
strategies
achieving
carbon
neutrality.
Yet,
its
efficiency
remains
unsatisfactory
mainly
due
to
severe
charge-transfer
resistance
and
slow
charge
kinetics.
Herein,
a
tunable
interfacial
transfer
on
an
oxygen-vacancies-modified
bismuth
molybdate
nanoflower
assembled
by
2D
nanosheets
(BMOVs)
bismuthene
composite
(Bi/BMOVs)
is
demonstrated
photocatalytic
conversion.
Specifically,
meticulous
design
Ohmic
contact
formed
between
BMOVs
can
allow
modulation
resistance.
According
density
functional
theory
(DFT)
simulations,
it
ascertained
that
such
exceptional
kinetics
attributed
built-in
electric
field
(IEF)
contact.
As
such,
reduction
performance
optimized
Bi/BMOVs
(CO
CH4
productions
rate
169.93
4.65
µmol
g-1
h-1
,
respectively)
ca.
10
times
higher
than
pristine
BMO
rates
16.06
0.51
respectively).
The
reported
in
this
work
shed
some
important
light
highly
efficient
photocatalysts
both
energy
environmental
applications.
Charge
separation
efficiency
of
photocatalysts
is
still
the
key
scientific
issue
for
solar-to-chemical
energy
conversion.
In
this
work,
an
electron
donor-acceptor
(D-A)
interface
with
high
charge
between
TPPS
(tetra(4-sulfonatophenyl)porphyrin)
and
PDI
(perylene
diimide)
successfully
constructed
boosting
photocatalytic
H
The
identity
of
charge
transfer
process
at
the
heterogeneous
interface
plays
an
important
role
in
improving
stability,
activity,
and
selectivity
heterojunction
catalysts.
And,
situ
irradiation
X-ray
photoelectron
spectroscopy
(XPS)
coupled
with
UV
light
optical
fiber
measurement
setup
is
developed
to
monitor
observe
between
heterojunction.
However,
in-depth
relationship
binding
energy
wavelength
missing
based
on
fact
that
incident
formed
by
coupling
different
wavelengths.
Furthermore,
a
quantitative
understanding
numbers
remains
elusive.
Herein,
g-C3
N4
/SnO2
model
catalyst,
wavelength-dependent
Boltzmann
function
describe
changes
through
utilizing
continuously
adjustable
monochromatic
XPS
technique
established.
Using
this
method,
study
further
reveals
electrons
number
can
be
readily
calculated
forming
asymptotic
model.
This
methodology
provides
blueprint
for
deep
charge-transfer
rules
facilitates
future
development
highly
active
advanced
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
62(29)
Опубликована: Май 25, 2023
Electrocatalytic
nitrogen
reduction
reaction
(ENRR)
has
emerged
as
a
promising
approach
to
synthesizing
green
ammonia
under
ambient
conditions.
Tungsten
(W)
is
one
of
the
most
effective
ENRR
catalysts.
In
this
reaction,
protonation
intermediates
rate-determining
step
(RDS).
Enhancing
adsorption
crucial
increase
intermediates,
which
can
lead
improved
catalytic
performance.
Herein,
we
constructed
strong
interfacial
electric
field
in
WS2
-WO3
elevate
d-band
center
W,
thereby
strengthening
intermediates.
Experimental
results
demonstrated
that
led
significantly
Specifically,
exhibited
high
NH3
yield
62.38
μg
h-1
mgcat-1
and
promoted
faraday
efficiency
(FE)
24.24
%.
Furthermore,
situ
characterizations
theoretical
calculations
showed
upshifted
W
towards
Fermi
level,
leading
enhanced
-NH2
-NH
on
catalyst
surface.
This
resulted
rate
RDS.
Overall,
our
study
offers
new
insights
into
relationship
between
provides
strategy
enhance
during
process.
Angewandte Chemie International Edition,
Год журнала:
2023,
Номер
63(5)
Опубликована: Дек. 12, 2023
The
co-assembly
naphthalimide/perylene
diimide
(NDINH/PDINH)
supramolecular
photocatalysts
were
successfully
synthesized
via
a
rapid
solution
dispersion
method.
A
giant
internal
electric
field
(IEF)
in
structure
was
built
by
the
larger
local
dipole.
NDINH
coated
on
PDINH
could
reduce
reflected
over
to
improve
its
responsive
activity
ultraviolet
light.
Resultantly,
an
efficient
full-spectrum
photocatalytic
overall
water
splitting
with
H
Journal of the American Chemical Society,
Год журнала:
2023,
Номер
145(42), С. 23167 - 23175
Опубликована: Окт. 11, 2023
The
precise
tuning
of
components,
spatial
orientations,
or
connection
modes
for
redox
units
is
vital
gaining
deep
insight
into
efficient
artificial
photosynthetic
overall
reaction,
yet
it
still
hard
achieve
heterojunction
photocatalysts.
Here,
we
have
developed
a
series
molecular
junction
covalent
organic
frameworks
(COFs)
(M-TTCOF-Zn,
M
=
Bi,
Tri,
and
Tetra)
reaction.
between
TAPP-Zn
multidentate
TTF
endows
various
water
photo-oxidation
(multidentate
TTF)
CO2
photoreduction
(TAPP-Zn)
centers
that
can
serve
as
desired
platforms
to
study
the
possible
interactions
centers.
Notably,
Bi-TTCOF-Zn
exhibits
high
CO
production
rate
11.56
μmol
g-1
h-1
(selectivity,
∼100%),
which
more
than
2
6
times
higher
those
Tri-TTCOF-Zn
Tetra-TTCOF-Zn,
respectively.
As
revealed
by
theoretical
calculations,
facilitates
uniform
distribution
energy-level
orbitals,
faster
charge
transfer,
stronger
*OH
adsorption/stabilization
ability
Tetra-TTCOF-Zn.
