Summary: | Herein, a highly N-rich covalent triazine framework (CTF) is applied as support for a Ru<sup>III</sup> complex. The bipyridine sites within the CTF provide excellent anchoring points for the [Ru(acac)<sub>2</sub>(CH<sub>3</sub>CN)<sub>2</sub>]PF<sub>6</sub> complex. The obtained robust Ru<sup>III</sup>@bipy-CTF material was applied for the selective tandem aerobic oxidation–Knoevenagel condensation reaction. The presented system shows a high catalytic performance (>80% conversion of alcohols to α, β-unsaturated nitriles) without the use of expensive noble metals. The bipy-CTF not only acts as the catalyst support but also provides the active sites for both aerobic oxidation and Knoevenagel condensation reactions. This work highlights a new perspective for the development of highly efficient and robust heterogeneous catalysts applying CTFs for cascade catalysis.
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