Journal of Materials Chemistry A,
Год журнала:
2024,
Номер
12(41), С. 28233 - 28246
Опубликована: Янв. 1, 2024
The
photogenerated
electrons
in
C
3
N
5
-CoPc
are
accurately
transferred
to
the
Co
atom
through
phosphate,
and
is
excited
as
a
catalytic
center
produce
H
2
O
.
The
solar-powered
photocatalytic
oxygen
reduction
reaction
is
considered
a
promising
alternative
method
for
H2O2
production
under
mild
conditions.
However,
the
intrinsic
competitive
pathway
grossly
inhibits
selectivity
and
final
yield
of
accompanying
loss
photogenerated
electrons
during
process.
Herein,
two-coordinate
nitrogen
(N2C)
vacancy-rich
g-C3N4
(DCN1.2)
was
developed
by
polymerization
pyrolysis
using
bottom-up
strategy.
DCN1.2
with
low-coordinated
N2C-vacancy
enabled
an
enhanced
in
wide
pH
range.
optimized
demonstrated
556.2
μmol·gcat–1·h–1
at
=
10,
which
approximately
3
times
higher
than
that
pristine
CN
(202.7
μmol
gcat–1·h–1).
DFT
calculations
photochemical
experimental
results
revealed
N2C-vacancies
induced
asymmetric
electron
distribution
DCN,
thereby
facilitating
transfer
promoting
O2
adsorption/activation
production.
Additionally,
EPR
situ
FTIR
measurements
indicated
could
produce
via
sequential
two-step
single-electron
pathway,
achieving
efficient
good
selectivity.
This
study
provides
guidance
rational
design
defect-engineering
catalysts
generation.
