Bis(phosphinimino)methanide rare earth amides: synthesis, structure, and catalysis of hydroamination/cyclization, hydrosilylation, and sequential hydroamination/hydrosilylation |
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Authors: | Rastätter Marcus Zulys Agustino Roesky Peter W |
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Institution: | Institut für Chemie und Biochemie, Freie Universität Berlin, Fabeckstrasse 34–36, 14195 Berlin, Germany, Fax: (+49) 30-838-52440 |
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Abstract: | A series of yttrium and lanthanide amido complexes Ln{N(SiHMe(2))2}2{CH(PPh(2)NSiMe(3))2}] (Ln=Y, La, Sm, Ho, Lu) were synthesized by three different pathways. The title compounds can be obtained either from Ln{N(SiHMe(2))2}3(thf)2] and CH(2)(PPh(2)NSiMe(3))2] or from KN(SiHMe(2))2 and Ln{CH(PPh(2)NSiMe(3))2}Cl(2)]2, while in a third approach the lanthanum compound was synthesized in a one-pot reaction starting from K{CH(PPh(2)NSiMe(3))2}, LaCl3, and KN(SiHMe(2))2. All the complexes have been characterized by single-crystal X-ray diffraction. The new complexes, Ln{N(SiHMe(2))2}2{CH(PPh(2)NSiMe(3))2}], were used as catalysts for hydroamination/cyclization and hydrosilylation reactions. A clear dependence of the reaction rate on the ionic radius of the center metal was observed, showing the lanthanum compound to be the most active one in both reactions. Furthermore, a combination of both reactions--a sequential hydroamination/hydrosilylation reaction--was also investigated. |
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Keywords: | catalysis hydroamination hydrosilylation N P ligands rare earth metals |
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