【摘要】：多環(huán)芳烴(Polycyclic aromatic hydrocarbons,PAHs)在高壓條件下的物理化學(xué)性質(zhì)的研究對于探究地球早期有機物質(zhì)的來源、生命的起源具有十分重要的意義,同時對推動超高壓合成技術(shù)的發(fā)展也有一定的積極意義。三維熒光光譜(Three dimensional fluorescence spectrum,3DFS)能夠同時反應(yīng)熒光強度隨著激發(fā)波長和發(fā)射波長的變化情況,相對于二維熒光可以提供多十倍或幾十倍以上的數(shù)據(jù),這對于分析熒光光譜的細微變化有重大意義。本文利用3DFS研究了PAHs的高壓熒光性質(zhì)。本文對處于室溫下、壓力范圍為0.1-60 MPa、濃度為10-6 mol L-1,10-5 mol L-1,和10-4 mol L-1的6種單一多環(huán)芳烴(萘、芴、菲、苊、熒蒽、蒽)的3DFS進行了研究。根據(jù)得到的常壓下3DFS發(fā)現(xiàn),所選取的6個多環(huán)芳烴的特征峰數(shù)量有很大的差別,從2個(萘)到12個(蒽)不等。本實驗通過分析在不同壓力下各個多環(huán)芳烴的熒光峰位置和峰強度來探討壓力對熒光光譜的影響。結(jié)果顯示,隨著壓力的不斷升高,6種多環(huán)芳烴的熒光峰位置并沒有發(fā)生改變,但是熒光強度發(fā)生了巨大的變化,并且熒光強度隨壓力的增加或減小隨著被測熒光物質(zhì)的改變有巨大的差別,同時發(fā)現(xiàn)熒光物質(zhì)的濃度變化也會對實驗結(jié)果產(chǎn)生顯著的影響,濃度的增加加劇了壓力對熒光光譜的影響。本文還對處于常溫、壓力范圍為0.1-60 MPa、濃度比為1:1的蒽-芴、蒽-萘、蒽-菲、蒽-苊、蒽-熒蒽、萘-芴、萘-菲、萘-苊、萘-熒蒽、芴-菲、芴-苊、芴-熒蒽、菲-苊、菲-熒蒽、苊-熒蒽的二元混合溶液的3DFS進行了測定。實驗結(jié)果顯示,在常壓下,第二種PAHs的加入對原PAHs的熒光峰峰位置沒有影響,隨著壓力的上升,PAHs二元混合溶液中2個組分的熒光峰峰位置都沒有漂移,但是壓力的增加對PAHs二元混合溶液中2個組分的特征峰熒光強度產(chǎn)生了顯著影響,并且與該PAHs二元混合溶液中2個組分單獨存在時的特征峰熒光強度-壓力變化曲線不同。
[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.
【學(xué)位授予單位】：浙江工業(yè)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O657.3;O625.15

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