Departamento de Química, Módulo 13, Facultad de Ciencias and Institute for Advanced Research in Chemical Sciences (IAdChem), Universidad Autónoma de Madrid, Madrid, Spain.
CONACYT-Universidad Juárez Autónoma de Tabasco, Centro de Investigación de Ciencia y Tecnología Aplicada de Tabasco, Cunduacán, Tabasco, Mexico.
J Comput Chem. 2023 Jan 30;44(3):159-167. doi: 10.1002/jcc.26843. Epub 2022 Mar 17.
The interaction of ammonia with Be (n < 1-10) clusters has been investigated by density functional theory and ab initio calculations. The main conclusion is that, regardless of the size of the Be cluster, neither the structure of ammonia nor that of the Be clusters are preserved due to a systematic dissociation of its NH bonds and a spontaneous H-shift toward the available Be atoms. This H migration not only leads to rather stable BeH bonds, but dramatically enhances the strength of the BeN bonds as well. Accordingly, the maximum stability is found for the interaction with the beryllium trimer, leading to a complex with three NBe and three BeH bonds. Another maximum in stability, although lower than that reached for n = 3, is found for the Be heptamer, since from n = 6, a new NBe bond is formed, so that complexes from n = 6 to n = 10 are characterized by the formation of a NBe moiety, whose stability reaches a maximum at n = 7. The bonding characteristics of the different species formed are analyzed by means of AIM, NBO, ELF and AdNDP approaches.
采用密度泛函理论和从头算方法研究了氨与 Be(n < 1-10)团簇的相互作用。主要结论是，无论 Be 团簇的大小如何，由于其 NH 键的系统解离以及 H 原子自发向可用的 Be 原子迁移，氨的结构和 Be 团簇的结构都不会被保留。这种 H 迁移不仅导致相当稳定的 BeH 键，而且还显著增强了 BeN 键的强度。因此，与三原子 Be 相互作用的最大稳定性导致形成具有三个 NBe 和三个 BeH 键的复合物。尽管低于 n = 3 时达到的稳定性最大值，但对于七原子 Be 团簇也发现了另一个稳定性最大值，因为从 n = 6 开始，形成了新的 NBe 键，因此从 n = 6 到 n = 10 的复合物的特征在于形成了一个 NBe 部分，其稳定性在 n = 7 时达到最大值。通过 AIM、NBO、ELF 和 AdNDP 方法分析了形成的不同物种的成键特征。
