|Title||beta-SiH-Containing Tris(silazido) Rare-Earth Complexes as Homogeneous and Grafted Single-Site Catalyst Precursors for Hydroamination|
|Publication Type||Journal Article|
|Year of Publication||2017|
|Authors||Eedugurala, N, Wang, ZR, Yan, KK, Boteju, KC, Chaudhary, U, Kobayashi, T, Ellern, A, Slowing, II, Pruski, M, Sadow, AD|
|Type of Article||Article|
|Keywords||chemistry, eta-2-silanimine complexes, h bond activation, hydroamination, intramolecular, lanthanide catalysts, mesoporous silica, molecular-structures, nmr-spectroscopy, structural-characterization, surface organometallic chemistry, Zirconium|
ng with THF and protonated silazido as HN(SiHMe2)tBu and H(2)NtBu. The surface species are characterized by multinuclear and multidimensional solid-state (SS) NMR spectroscopic techniques, as well as diffuse reflectance FTIR, elemental analysis, and reaction stoichiometry. A key (1)J(SiH) SSNMR measurement reveals that the grafted sites most closely resemble Ln.THF adducts, suggesting that siloxane coordination occurs in grafted compounds. These species catalyze the hydroamination/bicyclization of aminodialkenes, and both solution-phase and interfacial conditions provide the bicyclized product with equivalent cis:trans ratios. Similar diastereoselectivities mediated by catalytic sites under the two conditions suggest similar effective environments.
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