ACS Catalysis,
Год журнала:
2024,
Номер
14(13), С. 10204 - 10213
Опубликована: Июнь 21, 2024
Precisely
engineering
point
defects
holds
promise
for
the
development
of
state-of-the-art
photocatalysts
CO2
conversion.
This
study
demonstrates
controllable
creation
nitrogen
vacancies
(VNs)
in
centers
heptazine
rings
graphitic
carbon
nitrides
(g-C3N4)
via
a
photochemical-assisted
etching
strategy.
Spectroscopic
analyses
and
theoretical
simulations
elucidate
photochemical
process
to
hydrogenate
situated
at
center
g-C3N4
ring
then
release
an
ammonia
molecule,
accompanied
by
photooxidation
sacrificial
agents.
The
catalyst
with
optimal
VNs
concentration
achieves
CO
generation
rate
35.2
μmol
g–1
h–1
nearly
100%
selectivity,
comparable
performance
reported
materials.
remarkably
improved
photoactivity
is
due
adjustments
electronic
structures
midgap
states
delocalized
π
electron
cloud
created
12-membered
surrounding
VN,
which
maximizes
light-harvesting
efficiencies
suppresses
recombination
photogenerated
electrons
holes.
also
activates
neighboring
catalytic
reduce
energy
barrier
reduction.
work
provides
good
design
concept
regulate
activity
defects.
ACS ES&T Engineering,
Год журнала:
2022,
Номер
2(4), С. 564 - 585
Опубликована: Янв. 24, 2022
Heterogeneous
photocatalytic
reactions
have
experienced
many
efforts
in
developing
new
materials
to
tackle
environmental
and
energy
crises
through
utilizing
appropriate
photocatalysts
wastewater
treatment,
H2
generation,
organic
transformations,
CO2
reduction,
N2
photofixation,
biomass
conversion.
While
these
processes
are
addressed
the
literature
separately,
a
recent
innovative
viewpoint
is
employ
system
achieve
simultaneously
two
or
more
functions.
The
challenging
point
that
combination
of
functions
one
requires
novel
design
engineering
an
semiconductor
photocatalyst
with
special
characteristics
for
each
application
particular
environment.
Recently,
graphitic
carbon
nitride
(g-C3N4)
its
unique
physicochemical
properties
has
gained
tremendous
attention
among
researchers
due
great
potential
utilization
as
dual-functional
photocatalyst.
In
this
study,
role
morphological
band
gap
manipulation
heterojunction
formation
g-C3N4
will
be
considered.
These
newly
applied
strategies
useful
improve
activity
different
simultaneous
reactions.
Furthermore,
detailed
information
on
g-C3N4-based
discussed
reactions:
namely,
(i)
generation
combined
oxidation
pollutants,
(ii)
mineralization
pollutants
reduction
obtained
CO2,
(iii)
removal
mixture
heavy
metals,
(iv)
H+
(v)
conjunction
substrates/biomass
value-added
products,
(vi)
H2O2
production.
approaches
could
provide
efficient
sustainable
involved
both
issues.
Advanced Functional Materials,
Год журнала:
2022,
Номер
32(29)
Опубликована: Фев. 23, 2022
Abstract
Sparked
by
natural
photosynthesis,
solar
photocatalysis
using
metal‐free
graphitic
carbon
nitride
(g‐C
3
N
4
)
with
appealing
electronic
structure
has
turned
up
as
the
most
captivating
technique
to
quest
for
sustainable
energy
generation
and
pollution‐free
environment.
Nonetheless,
low‐dimensional
g‐C
is
thwarted
from
sluggish
kinetics
rapid
recombination
of
photogenerated
carriers
upon
light
irradiation.
Among
multifarious
modification
strategies,
engineering
2D
cocatalysts
anticipated
accelerate
redox
kinetics,
augment
active
sites
ameliorate
electron–hole
separation
boosted
activity
thanks
its
face‐to‐face
contact
surface.
It
timely
technological
significance
review
2D/2D
interfaces
state‐of‐the‐art
cocatalysts,
spanning
carbon‐containing
phosphorus‐containing,
metal
dichalcogenide,
other
cocatalysts.
Fundamental
principles
each
photocatalytic
application
will
be
introduced.
Thereafter,
recent
advances
cocatalyst‐mediated
systems
critically
evaluated
based
on
their
interfacial
engineering,
emerging
roles,
impacts
toward
stability
catalytic
efficiency.
Importantly,
mechanistic
insights
into
charge
dynamics
structure–performance
relationship
deciphered.
Last,
noteworthy
research
directions
are
prospected
deliver
insightful
ideas
future
development
.
Overall,
this
serve
a
scaffold
cornerstone
in
designing
dimensionality‐dependent
cocatalyst‐assisted
renewable
ecologically
green
Advanced Materials,
Год журнала:
2022,
Номер
34(28)
Опубликована: Май 5, 2022
Ammonia
and
nitrates
are
the
most
fundamental
significant
raw
ingredients
in
human
society.
Till
now,
industrial
synthetic
ammonia
by
Haber-Bosch
process
Ostwald
have
encountered
increasingly
serious
challenges,
i.e.,
high
energy
consumption,
cost,
environment-harmful
gas
emissions.
Therefore,
developing
alternative
approaches
to
achieve
nitrogen
fixation
overcome
inherent
deficiencies
of
well-established
processes
has
fascinated
scientists
for
many
years,
especially
simultaneous
formation
nitrate
directly
from
N2
molecules,
which
been
rarely
studied.
Herein,
a
heterojunction-based
photocatalytic
system
is
designed
successfully
"overall
fixation,"
sustainable
conversion
molecules
into
products
under
mild
conditions.
In
this
heterojunction,
interfacial
charge
redistribution
(ICR)
promotes
selective
accumulations
photogenerated
electrons
holes
CdS
WO3
components.
As
result,
can
be
activated
reduced
with
yields
35.8
µmol
h-1
g-1
multi-electron
process,
synchronously
oxidized
14.2
hole-induced
oxidation
coupling
process.
This
work
provides
novel
insight
promising
approach
realize
artificial
condition.
ACS Catalysis,
Год журнала:
2022,
Номер
12(9), С. 5077 - 5093
Опубликована: Апрель 14, 2022
To
improve
the
photocatalytic
hydrogen
evolution
activity
of
palladium-assisted
graphitic
carbon
nitride
(g-C3N4),
here,
palladium-single-atom-coordinated
cyano-group-rich
g-C3N4
(Pd/DN-UCN)
are
synthesized,
and
synthesis
process
includes
copolymerization
urea-derived
supramolecular
aggregates
NH4Cl
followed
by
wet
impregnation.
By
combining
powerful
characteristic
results
theoretical
calculations,
formation
mechanism
Pd
single
atoms
on
ultrathin,
mesoporous
nanosheets
is
proposed,
highlighting
that
firmly
stabilized
in
interlayers
caused
combination
physical
confinement
effect
coordination
bonding
cyano
groups
with
atoms;
additionally,
Pd–N3
Pd/DN-UCN
heterojunctions
confirmed,
which
one
atom
coordinates
N
group
two
sp2-hybridized
adjacent
layer.
The
presence
Pd–N
induces
a
midgap
state
band
structure
g-C3N4.
At
optimal
loading
levels
(0.16%),
synthesized
0.16%Pd/DN-UCN0.50
exhibits
enhanced
production
as
compared
to
electrostatically
"sixfold
cavities"
g-C3N4,
apparent
quantum
yield
values
at
stationary
point
concentration
(1.2
g
L–1)
can
reach
up
14.6,
15.8,
4.69,
3.05%
under
monochromatic
light
irradiation
365,
400,
450,
550
nm,
respectively.
cooperation
significantly
boosted
transfer
photoexcited
electrons
atomically
dispersed
sites
via
as-built
interlayer
delivery
channels
maximal
utilization
efficiency
dominates
Pd/DN-UCN.
