We report for the first time a metal‐free heterogeneously catalyzed hydrogenation using a semi‐solid frustrated Lewis pair (FLP). The catalyst consists of a solid polyamine organic framework and molecular tris(pentafluorophenyl)borane (BCF) that form a semi‐immobilized FLP in situ in the catalytic hydrogenation of diethyl benzylidenemalonate. ¹¹B NMR spectroscopy proves the successful hydrogen activation by the FLP. Furthermore, the B−N interactions between the polyamine and BCF are investigated by IR and solid state NMR spectroscopy. The FLP 1,4‐diazabicyclo[2.2.2]octane (DABCO)/BCF, which combines the features of a FLP and a classical Lewis adduct, functions as molecular reference in both, catalysis and characterization. Furthermore, computational studies enable a better insight into the hydrogen activation through DABCO/BCF and polyamine/BCF.

中文翻译：

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多胺有机骨架中的固体分子沮丧的路易斯对，用于烯烃的无催化金属加氢

我们首次报告了使用半固态受阻路易斯对（FLP）进行的无金属非均相催化氢化。该催化剂由固体多胺有机骨架和分子三（五氟苯基）硼烷（BCF）组成，它们在苄基亚甲基丙二酸二乙酯的催化加氢反应中原位形成半固定的FLP。¹¹B NMR光谱证明FLP成功地激活了氢。此外，通过IR和固态NMR光谱研究了多胺和BCF之间的BN相互作用。FLP 1,4-二氮杂双环[2.2.2]辛烷（DABCO）/ BCF结合了FLP和经典的路易斯加合物的特征，在催化和表征中均充当分子参考。此外，计算研究使您可以更好地了解通过DABCO / BCF和多胺/ BCF进行的氢活化。