The Center for Modeling and Simulation Chemistry, School of Chemistry and Chemical Engineering, Shandong University, Jinan, People's Republic of China.
J Comput Chem. 2012 Aug 5;33(21):1773-80. doi: 10.1002/jcc.23018. Epub 2012 May 21.
Three classes of multi-Zn-expanded graphene patches in different shapes are computationally designed through introducing a Zn chain into the corresponding middle benzenoid chain. Both density functional theory and complete active space self-consistent field calculations predict that molecules of nnn-quasi-linear and nnn-slightly bent series have the open-shell broken-symmetry (BS) singlet diradical ground states, whereas those of n(n+1)n species possess quintet tetraradical as their ground state and become open-shell BS singlet tetraradicals when they are in a higher energy state. These results offer the first theoretical attempt to introduce multi-Zn into the small graphene patches to form Zn-expanded graphene patches, leading them to polyradical structures. This work provides an executable strategy to yield molecules which have stable polyradicaloid character and enhanced electronic properties of multi-Zn-expanded graphene patches.
通过在相应的中间苯环链中引入 Zn 链，计算设计了三种不同形状的多 Zn 扩展石墨烯补丁。密度泛函理论和完全活性空间自洽场计算都预测，nnn-准线性和 nnn-略弯曲系列的分子具有开壳破对称（BS）单重自由基基态，而 n(n+1)n 物种则具有五重态四自由基作为其基态，当它们处于较高的能量状态时，它们变成开壳 BS 单重四自由基。这些结果首次尝试将多 Zn 引入小石墨烯补丁中，形成 Zn 扩展石墨烯补丁，使其具有多自由基结构。这项工作为产生具有稳定的多自由基特征和增强的多 Zn 扩展石墨烯补丁电子性质的分子提供了一个可行的策略。
