π电子碳烟成核反应路径的研究

Study on the Reaction Paths of π Electron Soot Nucleation

由于具有多自由基特性,两个多环芳烃能通过它们的π电子发生二聚,因而发生碳烟颗粒成核过程。本文使用量子化学方法研究了π电子碳烟成核的反应路径,计算得到了其开壳单重态的反应势能面,结果表明,由于多环芳烃的多自由基特性以及色散力的影响,该反应势能面的能垒低于反应物,因此π电子碳烟成核反应易发生。最后通过比较开壳单重态与闭壳单重态的反应路径,具体阐述了π电子在该成核路径中起到的重要作用。

Due to the multi-radical characteristics,two polycyclic aromatic hydrocarbon（PAH）moleculesmay form a dirner through their π electrons,which leads to soot nuclcuation.In this work,we studied the reaction paths of π electron soot nucleation using quantum-chemical methods,and obtained the potential energy surface of the open-shell singlet reaction path,which showsthe reaction energy barriers are lower than the energy of the reactants,because of the multi-radical characteristic and the dispersion force of the PAHs.Hence,the reactions of π electron soot nucleation are fast.Finally,the open-shell singlet reaction path was compared with the closed-shell singlet path to demonstrate the important role of the w electrons in this soot nucleation process.