罗勒烯臭氧化液相反应机制的量子化学模拟计算

Theoretical study of ocimene ozonolysis reaction mechanism in aqueous solution

挥发性有机物(VOCs)作为光化学反应的前体物对环境大气的组成有重要影响。其中罗勒烯与臭氧发生反应生成二次气溶胶和活性中间体,对整个大气环境和人体健康都会造成很大影响。采用PCM溶剂化模型,结合相应的量子化学计算在MPWB1K/6-31G**水平下计算了罗勒烯臭氧化的水相反应机理,提供了主要通道在气液相中的反应物和产物的吉布斯自由能数据。根据反应物和产物在不同相中的吉布斯自由能,得到气相和液相中各基元反应的平衡常数。本研究的理论计算结果可以为实验研究提供理论上的依据和预测。

Volatile organic compounds （VOCs） play an important role in the formation of secondary organic aerosol （SOA） Ocirnene reacts with ozone generating secondary organic aerosols and reactive intermediates which have a great impact on the atmospheric environment and human health. We probed into the ocimene ozonolysis reaction mechanisms at the MPWB1K level with the 6-31G（d, p） basis set, offered the main reaction channels, and used the polarized continuum model （PCM） to calculate the solvation energy. The equilibrium constants in both gas phases and in aqueous phase indicating the reaction trend were obtained according to the difference of Gibbs free energy. The results of our study will provide a theoretical basis for experimental research and forecast.