Solid Molecular Frustrated Lewis Pairs in a Polyamine Organic Framework for the Catalytic Metal‐free Hydrogenation of Alkenes
Solid Molecular Frustrated Lewis Pairs in a Polyamine Organic Framework for the Catalytic Metal‐free Hydrogenation of Alkenes
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DOI：
10.1002/cctc.201701783
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发表时间：
2018-04
期刊：
影响因子：
4.5
通讯作者：
A. Willms;Hannah Schumacher;Tarnuma Tabassum;Long Qi;S. Scott;P. Hausoul;M. Rose
中科院分区：
文献类型：
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作者：
A. Willms;Hannah Schumacher;Tarnuma Tabassum;Long Qi;S. Scott;P. Hausoul;M. Rose
我们首次报道了使用半固体阻挫刘易斯对（FLP）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，其在亚苄基丙二酸二乙酯的催化氢化中原位形成半固定化FLP。11B NMR光谱证明了FLP成功的氢活化。此外，通过红外光谱和固体核磁共振光谱研究了多胺与BCF之间的B−N相互作用。FLP 1，4-二氮杂双环[2.2.2]辛烷（DABCO）/BCF结合了FLP和经典的刘易斯加合物的特征，在催化和表征中用作分子参考。此外，计算研究使通过DABCO/BCF和多胺/BCF的氢活化更好地了解。
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.