静水压力对系列多环芳烃三维荧光光谱的影响

发布时间：2019-03-02 15:55

【摘要】：多环芳烃(Polycyclic aromatic hydrocarbons,PAHs)在高压条件下的物理化学性质的研究对于探究地球早期有机物质的来源、生命的起源具有十分重要的意义,同时对推动超高压合成技术的发展也有一定的积极意义。三维荧光光谱(Three dimensional fluorescence spectrum,3DFS)能够同时反应荧光强度随着激发波长和发射波长的变化情况,相对于二维荧光可以提供多十倍或几十倍以上的数据,这对于分析荧光光谱的细微变化有重大意义。本文利用3DFS研究了PAHs的高压荧光性质。本文对处于室温下、压力范围为0.1-60 MPa、浓度为10-6 mol L-1,10-5 mol L-1,和10-4 mol L-1的6种单一多环芳烃(萘、芴、菲、苊、荧蒽、蒽)的3DFS进行了研究。根据得到的常压下3DFS发现,所选取的6个多环芳烃的特征峰数量有很大的差别,从2个(萘)到12个(蒽)不等。本实验通过分析在不同压力下各个多环芳烃的荧光峰位置和峰强度来探讨压力对荧光光谱的影响。结果显示,随着压力的不断升高,6种多环芳烃的荧光峰位置并没有发生改变,但是荧光强度发生了巨大的变化,并且荧光强度随压力的增加或减小随着被测荧光物质的改变有巨大的差别,同时发现荧光物质的浓度变化也会对实验结果产生显著的影响,浓度的增加加剧了压力对荧光光谱的影响。本文还对处于常温、压力范围为0.1-60 MPa、浓度比为1:1的蒽-芴、蒽-萘、蒽-菲、蒽-苊、蒽-荧蒽、萘-芴、萘-菲、萘-苊、萘-荧蒽、芴-菲、芴-苊、芴-荧蒽、菲-苊、菲-荧蒽、苊-荧蒽的二元混合溶液的3DFS进行了测定。实验结果显示,在常压下,第二种PAHs的加入对原PAHs的荧光峰峰位置没有影响,随着压力的上升,PAHs二元混合溶液中2个组分的荧光峰峰位置都没有漂移,但是压力的增加对PAHs二元混合溶液中2个组分的特征峰荧光强度产生了显著影响,并且与该PAHs二元混合溶液中2个组分单独存在时的特征峰荧光强度-压力变化曲线不同。
[Abstract]:The study of the physicochemical properties of polycyclic aromatic hydrocarbons (Polycyclic aromatic hydrocarbons,PAHs) under high pressure is of great significance for exploring the origin of early organic substances and the origin of life. At the same time, it has some positive significance to promote the development of ultra-high pressure synthesis technology. Three-dimensional fluorescence spectrum (Three dimensional fluorescence spectrum,3DFS) can reflect the change of fluorescence intensity with excitation wavelength and emission wavelength at the same time, and can provide more than ten or more times more data than two-dimensional fluorescence. This is of great significance to the analysis of subtle changes in fluorescence spectra. In this paper, the high pressure fluorescence properties of PAHs have been studied by 3DFS. The 3DFS of six single polycyclic aromatic hydrocarbons (naphthalene, fluorene, phenanthrene, acenaphthene, fluoranthene, anthracene) in the pressure range of 0.1 脳 60 MPa, 10 ~ 5 mol / L, and 10 ~ 4 mol / L ~ (1) have been studied at room temperature. According to the obtained 3DFS at atmospheric pressure, it was found that the number of characteristic peaks of the six polycyclic aromatic hydrocarbons (PAHs) selected varied greatly from 2 (naphthalene) to 12 (anthracene). The effect of pressure on fluorescence spectra was investigated by analyzing the position and intensity of fluorescence peaks of polycyclic aromatic hydrocarbons under different pressures. The results showed that the fluorescence peaks of the six PAHs did not change with the increasing pressure, but the fluorescence intensity changed greatly. With the increase or decrease of the pressure, the fluorescence intensity has great difference with the change of the measured fluorescent substance, and it is found that the concentration change of the fluorescent substance will also have a significant effect on the experimental results. The effect of pressure on fluorescence spectrum was increased with the increase of concentration. For anthracene-fluorene, anthracene-naphthalene, anthracene-phenanthrene, anthracene-fluoranthene, naphthalene-fluorene, naphthalene-phenanthrene, naphthalene-acenaphthene, naphthalene-fluoranthene, fluorene-phenanthrene, fluorene-acenaphthene, naphthene-fluoranthene, fluorene-acenaphthene, The 3DFS of fluorene-fluoranthene, phenanthrene-acenaphthene, phenanthrene-fluoranthene and acenaphthene-fluoranthene was determined by 3DFS. The experimental results show that the addition of the second PAHs has no effect on the position of the fluorescence peak of the original PAHs under atmospheric pressure. With the increase of the pressure, the fluorescence peaks of the two components in the binary mixed solution of PAHs do not drift, and there is no change in the fluorescence peak position of the two components in the binary mixed solution of PAHs. However, the fluorescence intensity of the characteristic peaks of the two components in the binary mixed solution of PAHs was significantly influenced by the increase of pressure, and the fluorescence intensity-pressure curves of the characteristic peaks were different from those of the two components in the binary mixed solution of PAHs.
【学位授予单位】：浙江工业大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.3;O625.15

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