由氮杂环卡宾稳定的阳离子氧代钼亚烷基：从分子体系到高效负载型复分解催化剂
Cationic molybdenum oxo alkylidenes stabilized by N-heterocyclic carbenes: from molecular systems to efficient supported metathesis catalysts.
作者信息
Musso Janis V, De Jesus Silva Jordan, Benedikter Mathis J, Groos Jonas, Frey Wolfgang, Copéret Christophe, Buchmeiser Michael R
机构信息
Institute of Polymer Chemistry, University of Stuttgart Pfaffenwaldring 55 D-70569 Stuttgart Germany
Department of Chemistry and Applied Biosciences, ETH Zürich Vladimir-Prelog-Weg 1-5 CH-8093 Zürich Switzerland
出版信息
Chem Sci. 2022 Jul 12;13(29):8649-8656. doi: 10.1039/d2sc03321f. eCollection 2022 Jul 29.
Cationic d group 6 olefin metathesis catalysts have been recently shown to display in most instances superior activity in comparison to their neutral congeners. Furthermore, their catalytic performance is greatly improved upon immobilization on silica. In this context, we have developed the new family of molecular cationic molybdenum oxo alkylidene complexes stabilized by N-heterocyclic carbenes of the general formula [Mo(O)(CHCMe)(IMes)(OR)[X]] (IMes = 1,3-dimesitylimidazol-2-ylidene; R = 1,3-dimesityl-CH, CF; X = B(3,5-(CF)CH) , B(Ar), tetrakis(perfluoro--butoxy)aluminate (PFTA)). Immobilization of [Mo(O)(CHCMe)(IMes)(O-1,3-dimesityl-CH)B(Ar) ] on silica surface organometallic chemistry yields an active alkene metathesis catalyst that shows the highest productivity towards terminal olefins amongst all existing molybdenum oxo alkylidene catalysts.
最近研究表明，在大多数情况下，第6族阳离子烯烃复分解催化剂比其中性同类物表现出更高的活性。此外，将它们固定在二氧化硅上后，其催化性能会大大提高。在此背景下，我们开发了一类新的分子阳离子氧代钼亚烷基配合物，该配合物由通式为[Mo(O)(CHCMe)(IMes)(OR)[X]]的N-杂环卡宾稳定（IMes = 1,3-二甲基苯基咪唑-2-亚基；R = 1,3-二甲基苯基-CH、CF；X = B(3,5-(CF)CH) 、B(Ar)、四(全氟丁氧基)铝酸酯(PFTA)）。将[Mo(O)(CHCMe)(IMes)(O-1,3-二甲基苯基-CH)B(Ar) ]固定在二氧化硅表面有机金属化学上，得到一种活性烯烃复分解催化剂，在所有现有的氧代钼亚烷基催化剂中，该催化剂对末端烯烃表现出最高的产率。
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