用于二甲胺硼烷催化脱氢的含2-膦基芳氧基配体的二茂钛(III)配合物
Titanocene(III) complexes with 2-phosphinoaryloxide ligands for the catalytic dehydrogenation of dimethylamine borane.
作者信息
Klahn Marcus, Hollmann Dirk, Spannenberg Anke, Brückner Angelika, Beweries Torsten
机构信息
Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert-Einstein-Str. 29a, 18059 Rostock, Germany.
出版信息
Dalton Trans. 2015 Jul 21;44(27):12103-11. doi: 10.1039/c5dt00275c.
A study of the dehydrogenation of dimethylamine borane using different titanocene(III) complexes with 2-phosphinoaryloxide ligands is presented. Complexes Cp2Ti(κ(2)-O, P-O-C6H4-PR2) (3a: R = i-Pr, 3b: R = Ph) (Cp = η(5)-cyclopentadienyl) and Cp2Ti(κ(1)-O-O-C6H4-PR2) (5a: R = i-Pr, 5b: R = Ph) (Cp = η(5)-pentamethylcyclopentadienyl) were prepared by reactions of the 2-phosphinophenol ligand with different titanocene sources and fully characterised. Their catalytic activity depends on the steric influence of the cyclopentadienyl ligand, the coordination mode of the 2-phosphinoaryloxide ligand and on the used solvent. Complex 3a showed a turnover number of 43.2 in the neat substrate after 24 hours. EPR investigations were used to elucidate the fate of the Ti(III) catalyst.
本文介绍了一项关于使用不同的含2-膦基芳氧基配体的二茂钛(III)配合物对二甲胺硼烷进行脱氢反应的研究。通过2-膦基苯酚配体与不同二茂钛源的反应制备了配合物Cp2Ti(κ(2)-O, P-O-C6H4-PR2) (3a: R = 异丙基, 3b: R = 苯基) (Cp = η(5)-环戊二烯基) 和Cp2Ti(κ(1)-O-O-C6H4-PR2) (5a: R = 异丙基, 5b: R = 苯基) (Cp = η(5)-五甲基环戊二烯基)，并对其进行了全面表征。它们的催化活性取决于环戊二烯基配体的空间影响、2-膦基芳氧基配体的配位模式以及所使用的溶剂。24小时后，配合物3a在纯底物中的周转数为43.2。采用电子顺磁共振研究来阐明Ti(III)催化剂的反应历程。
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