Cooperative Multifunctional Catalysts for Nitrone Synthesis: Platinum Nanoclusters in Amine‐Functionalized Metal–Organic Frameworks

Abstract Nitrones are key intermediates in organic synthesis and the pharmaceutical industry. The heterogeneous synthesis of nitrones with multifunctional catalysts is extremely attractive but rarely explored. Herein, we report ultrasmall platinum nanoclusters (PtNCs) encapsulated in amine‐functionalized Zr metal–organic framework (MOF), UiO‐66‐NH 2 (Pt@UiO‐66‐NH 2 ) as a multifunctional catalyst in the one‐pot tandem synthesis of nitrones. By virtue of the cooperative interplay among the selective hydrogenation activity provided by the ultrasmall PtNCs and Lewis acidity/basicity/nanoconfinement endowed by UiO‐66‐NH 2 , Pt@UiO‐66‐NH 2 exhibits remarkable activity and selectivity, in comparison to Pt/carbon, Pt@UiO‐66, and Pd@UiO‐66‐NH 2 . Pt@UiO‐66‐NH 2 also outperforms Pt nanoparticles supported on the external surface of the same MOF (Pt/UiO‐66‐NH 2 ). To our knowledge, this work demonstrates the first examples of one‐pot synthesis of nitrones using recyclable multifunctional heterogeneous catalysts.