胺类化合物在各领域应用广泛，金属配合物对于其合成具有良好的催化表现，而锕系金属配合物[(Me₃Si)₂N]₂Th[κ²?(N,C)?CH₂Si(CH₃)₂N(SiMe₃)] (Cpda)表现尤为突出。本论文在B3PW91泛函水平上，研究了苯溶剂中钍配合物催化腈的硼氢化反应的反应机理。我们将整个反应分为三个阶段：催化剂的形成、亚胺的形成和胺的形成。研究发现：（1）配合物Cpda并不能直接催化腈或亚胺的转化，真正有效的催化剂是Cpda与频哪醇硼烷（HBpin）反应得到的含有Th-H键的Cat1或Cat2，其中Cat1较为稳定，二者在室温下可以相互转化；（2）腈硼氢化生成亚胺时，反应分三步进行：C≡N插入催化剂的Th-H键生成亚胺配合物中间体；HBpin与亚胺中间体进行B-N耦合；Th-N分离以及H迁移释放亚胺；（3）相比于Cat1, 腈或亚胺倾向于与Cat2反应，反应的能垒更低；苯腈作为底物时，两次氢化过程的能垒分别为13.9 kcal/mol及27.0 kcal/mol，且反应为强放热过程。

Amine compounds are widely used in various fields, and metal complexes have been reported to have excellent performance in catalyzing their synthesis, among them is the complex [(Me₃Si)₂N]₂Th[κ²?(N,C)?CH₂Si(CH₃)₂N(SiMe₃)] (Cpda). In the present thesis, the borohydrization mechanism of nitrile in benzene solvent catalyzed by Cpda was studied using B3PW91 functional. The whole reaction was divided into three stages: the formation of catalyst, the formation of imine and the formation of amine. The results indicated that Cpda did not directly catalyze the conversion of nitrile or imine and the effective catalyst was Cat1 or Cat2 containing Th-H bond generated by the reaction of Cpda with HBpin. Cat1 was more stable than Cat2 and these two conformers can transform to each other under room temperature. Our calculations also found that the borohydrization of nitrile leading to imine followed a three-step mechanism, including C≡N insertion into the Th-H bond to form the imine intermediate, the B-N coupling, and the Th-N dissociation accompanying with H migration to release imine and regenerate the catalyst Cat2. Compared with Cat1, nitrile or imine prefer to react with Cat2, with a lower energy barrier. When benzenitrile was used as the substrate, the energy barriers of the two hydrogenations were calculated to be 13.9 and 27.0 kcal/mol, respectively, with strong exothermicity.