基于微波等离子体矩质谱技术的多环芳烃检测方法的研究

The Polycyclic aromatic hydrocarbons (PAHs) are the typical persistent organic pollutants with great toxicity, which mainly originating from the uncompleted combustation of black coal, oil, timber, tobacco and organic polymer compounds to produce the volatile hydrocarbons. PAHs are a kind of important environmental pollutants with long time of duration. And PAHs is strongly carcinogenic, continuously has strong carcinogenic, induced malformation and mutagenicity. With the increasing consumption of coal and oil in daily life, transportation and industrial processes, the pollution due to PAHs is more and more serious. Developing the fast and sensitive detection method for the PAHs in complicated environmental samples is urgent need and imperative, and also attracts many analytical chemists' research interests. This project put forward a novel study approach based on one of our recent developed mass spectrometry techniques, named the microwave plasma torch mass spectrometry (MPT-MS). As we have shown, the MPT-MS is more suitable for the analysis of complex matrix samples with high excited and ionization abilities. We attempt to investigate the efficient and the ionization pattern of MPT-MS for PAHs in complex real environment samples. Furthermore, these works, including several parameters involving MPT device, would provide the transfer mechanism of electron and energy in MPT plasma, and would provide the theoretical support for the prospective developing of MPT mass spectrometer for the particular application in the analysis real environment samples. The relationship between the ionization characteristics in MPT plasma and the PAHs spatial structure and the number of aromatic ring in PAHs molecules would be in-step studied. At the same time, the study of PAHs MPT characteristics spectral peak and the dissociation rules under the collision induced dissociation of molecular fragments corresponding to the spectral peak, combing with chemometrics to get the difference spectra analysis, to conclude the general laws that different PAHs aromatic ring number and space configuration for cracking and the effect of combining ability, and the results will be applied to the PAHs toxicology research.

本项目基于微波等离子体矩(MPT)对复杂基体样品良好的电离能力和激发能力，将其推广应用于对环境具有持续污染性的多环芳烃(PAHs)的质谱检测研究，研讨MPT电离源对PAHs离化效率的影响，考察样品直接检测时电离电压大小与极性、角度、距离、喷雾气体种类与出口压力、溶剂、温度、进样方式等对信号的影响，对技术平台的性能和技术参数进行优化，得到最佳的工作条件，建立快速灵敏的PAHs检测方法，进而为发展能适合应用于复杂的实际环境样品中PAHs的实时在线检测的MPT质谱仪奠定技术基础。同时，研究PAHs的MPT质谱行为特征，根据不同的PAHs芳香环数目及空间构型的不同，研究PAHs的MPT特征谱峰及其在碰撞诱导解离下的碎片谱峰的规律，结合化学计量学，得到谱图差异分析，从而总结得出不同的PAHs芳香环数目及空间构型对对裂解和结合能力影响的规律，并应用于PAHs的毒理研究。

本项目基于微波等离子体矩(MPT)对复杂基体样品良好的电离能力和激发能力，且结构简便，易于推广应用等特性，将其推广应用于对环境具有持续污染性的多环芳烃(PAHs)的快速质谱检测研究。具体研究了16种多环芳烃类物质，对其MPT-飞行时间质谱的特征做了深入系统的研究，从中发现了部分多环芳烃物质的二重聚体现象；另外还从多环芳烃类物质研讨中对分子的芳香性产生了新的认识，这可以为更进一步地理解芳香性本质铺开一条新的道路。但对多环芳烃的定量检测方面研究，因受限于多环芳烃的不溶于常见溶剂，进展不大。在本项目还继续研究了MPT对过渡金属的研究，其中在惰性金属的检测研究中，取得了一定的突破，成功得到惰性金属钯的特征MPT质谱及其定量分析数据。最后，本项目还研究了其他的一些有机小分子，并将其应用于实际工作中。