Industrial & Engineering Chemistry Research,
Год журнала:
2024,
Номер
63(47), С. 20621 - 20632
Опубликована: Ноя. 14, 2024
N-rich
carbon
nitride
(g-C3N5)
became
a
promising
photocatalyst
due
to
its
narrower
band
gap,
larger
π-conjugate
network,
and
better
visible
light
responsive
hydrogen
precipitation
activity
compared
with
g-C3N4.
However,
the
inherent
shortcomings
still
limited
development
of
g-C3N5.
To
reasonably
address
this
issue,
N
defects
surface
amino
groups
were
successfully
introduced
into
pristine
g-C3N5
through
facile
one-step
calcination.
Systematical
characterizations
theoretical
calculation
confirmed
that
synergy
surface-grafted
group
achieved
dual-capture
strategy,
endowing
higher
hydrophilicity
faster
photogenerated
carrier
separation
transfer
efficiency.
With
modification
urea,
as-prepared
samples
exhibited
specific
area
further
provide
more
active
sites
during
photocatalysis.
The
experimental
results
proved
photocatalytic
evolution
(PHE)
performance
novel
material
was
significantly
enhanced,
optimal
reaching
5000.6
μmol·h–1·g–1,
which
24.5
4.5
times
than
comparison
sample,
respectively.
stability
reusability
N-defected
verified
by
recycling
tests
without
an
obvious
decrease
after
continuous
30
h
irradiation.
This
work
provided
perspective
insight
for
designing
fabricating
functionalized
photocatalysts.
Chemocatalytic
synthesis
of
lactic
acid
(LA)
from
biomass
sugars
involves
heat-absorbing
multistep
cascade
reactions
mediated
by
different
active
sites,
often
encountering
unsatisfactory
selectivity.
Here,
a
hole-localized
carbon
nitride-based
photocatalyst
(C-CNN)
is
constructed
covalent
binding
heptazine
and
triazole
skeleton
via
C─N
bonds
further
conjugated
interaction
with
activated
carbon,
achieving
the
complete
conversion
various
to
LA
(up
98.6%
selectivity)
at
room
temperature
for
2
h.
The
introduced
electron
donor
in
C-CNN
can
not
only
enhance
adsorption
sugar
enhanced
aldose-to-ketose
isomerization
over
localized
hole
(Lewis
acid)
on
skeleton,
but
also
modulate
valence
band
oxidation
circumvent
formation
•OH
•O2
‒
selective
C3‒C4
cleavage
ketose,
thus
realizing
exclusive
LA.
Moreover,
near-infrared
light
absorption
endowed
supply
sufficient
interface
photothermal
effect
ambient
production.
Life
cycle
assessment
shows
that
photocatalytic
system
has
good
prospects
industrialization
terms
both
energy
environment.
This
work
offers
novel
insights
into
multidirectional
utilization
solar
value-added
through
rational
modulation
sites.
Abstract
Utilizing
polymeric
catalysts
to
generate
hydrogen
peroxide
(H
2
O
)
via
photocatalysis
for
various
industrial
applications
is
a
promising
avenue,
but
the
application
potential
constrained
by
their
low
charge
separation
efficiency
and
capacity
oxygen
adsorption
activation.
Herein,
catalyst
(NiRF)
modified
with
Ni
metal
sites
on
resorcinol‐formaldehyde
(RF)
resin
presented,
which
can
efficiently
produce
H
through
in
pure
water.
The
optimal
NiRF‐5
exhibits
an
impressive
generation
rate
of
up
31.75
m
g
−1
h
under
visible
light
irradiation,
significantly
outperforming
most
reported
date.
Experimental
results
coupled
theoretical
calculations
simulation,
indicate
that
incorporation
nickel
ions
modulates
band
structure
NiRF
provides
active
conducive
transformation
oxygen.
regulate
ensure
suitable
configuration
energy.
This
work
novel
design
concept
RF‐based
photocatalysts
offers
approach
development
methods
efficient
photocatalytic
production
.
