A novel practical method for the gram scale preparation of melem possessing a nano rectangular prism morphology and improved specific surface area through a top-down depolymerization design was developed.
In
this work, the as-prepared 2,5,8-triamino-tri-s-triazine
(Melem), which possesses nanorectangular prism morphology,
the desired surface area, and photoluminescence properties, was combined
with the Keplerate {Mo72Fe30} nanocapsule to
produce a new heterojunction-like photocatalyst (M/K nanohybrid).
After full characterization of the as-prepared M/K nanohybrid, its
photocatalytic activity toward hydrogen peroxide (H2O2) dismutation was assessed under visible-light irradiation.
To study the significance of independent variables, a response surface
methodology based on a central composite design was employed to determine
the optimal conditions for decomposition of the H2O2 process. Efficient H2O2 decomposition
occurred within 3 h using a small amount of photocatalyst at pH =
3 and room temperature under a reptile light, rendering a high turnover
number of up to ∼53000. The visible-light-assisted photochemical
property of the M/K nanohybrid was confirmed by both the action spectra
and dark-light experiments. Kinetic studies using the M/K nanohybrid
revealed a first-order kinetic with a rate constant (k
1 = 3 × 10–4 s–1) 100-fold larger than that of the free cluster {Mo72Fe30} and an activation energy (64.14 kJ mol–1) half the amount obtained by the free cluster. A synergistic effect
between the {Mo72Fe30} nanocapsule and the
Melem nanorectangular prism through a type II heterojunction-like
mechanism sounds reasonable for promoting the photocatalytic activity
of the as-prepared M/K nanocomposite. A nonradical molecular mechanism
evidenced by the kinetic results and scavenging experiments was postulated.
The title hybrid exhibited prominent reusability in photocatalysis,
but disintegration of the Keplerate by H2O2 raised
some concerns regarding the nature of the true catalyst!
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