Xiong Mo, Kong Chuncai, Yang Zhimao, Yang Tao
MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi'an Jiaotong University, Xi'an 710049, Shaanxi, China.
Phys Chem Chem Phys. 2024 Aug 7;26(31):21282-21289. doi: 10.1039/d4cp02082k.
The exploration of endohedral fullerenes has garnered significant attention recently due to their distinctive chemical, electrochemical, and optoelectronic properties. Charge transfer, which usually occurs from encapsulated species to fullerenes, importantly affects the structures and properties of endohedral fullerenes. In this study, we theoretically investigated endohedral superhalogen fullerenes X@C (X = BO, BeF; 2 = 60, 70), in which the charge is reversely transferred from the fullerene to the superhalogen, by using density functional theory calculations and molecular dynamics simulations. Both natural population analysis and the quantum theory of atoms in molecules confirm about one electron transfer from the fullerene to the superhalogen, resulting in the formal valence state of X@C. Energy decomposition analysis on the interaction between the superhalogen and fullerene revealed that electrostatic energy contributes predominantly to the total interaction energy. These endohedral superhalogen fullerenes with cationic fullerenes were predicted to be able to serve as building blocks for one dimensional fullerene-based nanowires when combined with endohedral alkali-metallofullerenes with anionic fullerenes.
由于其独特的化学、电化学和光电性质，内嵌富勒烯的探索近来备受关注。电荷转移通常从被包裹的物种发生到富勒烯上，这对内嵌富勒烯的结构和性质有重要影响。在本研究中，我们通过使用密度泛函理论计算和分子动力学模拟，从理论上研究了内嵌超卤素富勒烯X@C（X = BO，BeF； 2 = 60，70），其中电荷从富勒烯反向转移到超卤素。自然布居分析和分子中的原子量子理论均证实从富勒烯到超卤素约有一个电子的转移，并导致了X@C的形式价态。对超卤素与富勒烯之间相互作用的能量分解分析表明，静电能对总相互作用能的贡献最大。这些带有阳离子富勒烯的内嵌超卤素富勒烯预计与带有阴离子富勒烯的内嵌碱金属富勒烯结合时，能够作为基于富勒烯的一维纳米线的构建单元。
