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Theoretical probing of twenty-coordinate actinide-centered boron molecular drums
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2021-11-18 , DOI: 10.1039/d1cp03900h
Juan Wang 1, 2 , Nai-Xin Zhang 1 , Cong-Zhi Wang 1 , Qun-Yan Wu 1 , Jian-Hui Lan 1 , Zhi-Fang Chai 1, 3 , Chang-Ming Nie 2 , Wei-Qun Shi 1
Affiliation  

The exploration of metal-doped boron clusters has a great significance in the design of high coordination number (CN) compounds. Actinide-doped boron clusters are probable candidates for achieving high CNs. In this work, we systematically explored a series of actinide metal atom (U, Np, and Pu) doped B20 boron clusters An@B20 (An = U, Np, and Pu) by global minimum structural searches and density functional theory (DFT). Each An@B20 cluster is confirmed to be a twenty-coordinate complex, which is the highest CN obtained in the chemistry of actinide-doped boron clusters so far. The predicted global minima of An@B20 are tubular structures with actinide atoms as centers, which can be considered as boron molecular drums. In An@B20, U@B20 has a relatively high symmetry of C2, while both Np@B20 and Pu@B20 exhibit C1 symmetry. Extensive bonding analysis demonstrates that An@B20 has σ and π delocalized bonding, and the U–B bonds possess a relatively higher covalency than the Np–B and Pu–B bonds, resulting in the higher formation energy of U@B20. Therefore, the covalent character of An–B bonding may be crucial for the formation of these high CN actinide-centered boron clusters. These results deepen our understanding of actinide metal doped boron clusters and provide new clues for developing stable high CN boron-based nanomaterials.

中文翻译:

二十坐标锕系中心硼分子鼓的理论探索

金属掺杂硼簇的探索对于高配位数(CN)化合物的设计具有重要意义。锕系元素掺杂的硼簇可能是实现高 CNs 的候选者。在这项工作中,我们通过全局最小结构搜索和密度泛函理论系统地探索了一系列锕系金属原子(U、Np 和 Pu)掺杂的 B 20硼团簇 An@B 20(An = U、Np 和 Pu)( DFT)。每个An@B 20簇都被证实是一个二十配位的络合物,这是迄今为止在锕系掺杂硼簇的化学中获得的最高CN。An@B 20的预测全局最小值是以锕系原子为中心的管状结构,可以认为是硼分子鼓。在 An@B如图20所示,U@B 20具有相对较高的C 2对称性,而Np@B 20和Pu@B 20 均表现出C 1对称性。大量的键合分析表明An@B 20具有σ 和π 离域键合,并且U-B 键比Np-B 和Pu-B 键具有相对更高的共价键,导致U@B 20 的形成能更高。因此,An-B 键的共价特性对于形成这些以高 CN 锕系元素为中心的硼簇至关重要。这些结果加深了我们对锕系金属掺杂硼团簇的理解,并为开发稳定的高 CN 硼基纳米材料提供了新的线索。
更新日期:2021-11-30
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