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首页> 外文期刊>Organometallics >Zirconium-Catalyzed Amine Borane Dehydrocoupling and Transfer Hydrogenation
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Zirconium-Catalyzed Amine Borane Dehydrocoupling and Transfer Hydrogenation

机译：锆催化的胺硼烷脱氢偶联和转移加氢

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摘要

kappa(5)-(Me3SiNCH2CH2)(2)N-(CH2CH2NSiMe2CH2)Zr (1) has been found to dehydrocouple amine borane substrates, RR'NHBH3 (R = R' = Me; R = Bu-t, R' = H; R = R' = H), at low to moderate catalyst loadings (0.5-5 mol %) and good to excellent conversions, forming mainly borazine and borazane products. Other zirconium catalysts, (N3N)ZrX [(N3N) = N-(CH2CH2NSiMe2CH2)(3), X = NMe2 (2), Cl (3), and (OBu)-Bu-t (4)], were found to exhibit comparable activities to that of 1. Compound 1 reacts with Me2NHBH3 to give (N3N)Zr-(NMe2BH3) (5), which was structurally characterized and features an eta(2) B-H sigma-bond amido borane ligand. Because 5 is unstable with respect to borane loss to form 2, rather than beta-hydrogen elimination, and 2-4 do not exhibit X ligand loss during catalysis, dehydrogenation is hypothesized to proceed via an outer-sphere-type mechanism. This proposal is supported by the catalytic hydrogenation of alkenes by 2 using amine boranes as the sacrificial source of hydrogen.
机译：已发现kappa（5）-（Me3SiNCH2CH2）（2）N-（CH2CH2NSiMe2CH2）Zr（1）对胺硼烷底物进行脱氢偶联，RR'NHBH3（R = R'= Me; R = Bu-t，R'= H ; R = R'= H），在低至中等的催化剂负载量（0.5-5 mol％）以及良好至优异的转化率下，主要形成硼嗪和硼氮烷产品。发现其他锆催化剂（N3N）ZrX [（N3N）= N-（CH2CH2NSiMe2CH2）（3），X = NMe2（2），Cl（3）和（OBu）-Bu-t（4）]表现出与1相当的活性。化合物1与Me2NHBH3反应生成（N3N）Zr-（NMe2BH3）（5），具有结构特征并具有eta（2）BHσ键合氨基硼烷配体。因为5相对于硼烷的生成2不稳定，而不是β-氢的消除，并且2-4在催化过程中不表现出X配体的丢失，所以假设脱氢是通过外球型机理进行的。该提案得到了使用胺硼烷作为氢的牺牲源通过2催化烯烃加氢的支持。

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