本文選題：深圳市PM2.5 + 有機(jī)硫酸酯�。� 參考：《哈爾濱工業(yè)大學(xué)》2015年碩士論文

【摘要】：有機(jī)硫酸酯類物質(zhì)(Organosulfates,OSs)是近幾年來發(fā)現(xiàn)的一種存在于大氣顆粒物上的新興有機(jī)組分。有研究表明,在環(huán)境空氣中SO_2濃度較高的地區(qū),大氣顆粒物中OSs的比重也較大。我國大氣中SO_2污染嚴(yán)重,因此對我國大氣顆粒物中OSs進(jìn)行污染特征研究,評估OSs對大氣顆粒物的貢獻(xiàn)具有重要意義。本文建立了一種間接測定大氣顆粒物中OSs的方法,通過間接地測定OSs的共有基團(tuán)硫酸根的含量,并基于從煙霧箱獲得的OSs中有機(jī)碳與有機(jī)硫的摩爾比,估算出OSs的含碳量。本文選用十二烷基硫酸鈉作為OSs的替代標(biāo)準(zhǔn)物,建立和優(yōu)化了OSs的解離方法,利用離子色譜測定解離前后顆粒物中硫酸根含量,同時通過差減法得到顆粒物中OSs中硫酸根的含量。為確定此方法在測定實(shí)際大氣顆粒物中OSs含量的適用性,本文設(shè)計(jì)了一系列不同摩爾比的無機(jī)硫與有機(jī)硫的混合體系,評價了該方法用于測定混合體系中無機(jī)硫酸根(Inorganic Sulfates,IS)和總硫酸根(Total Sulfates,TS)的回收率和精密度,并對獲得的OSs中硫酸根含量進(jìn)行了誤差分析。結(jié)果表明,本文建立的OSs中硫酸根定量方法的誤差范圍為5.74%～37.71%。本文選取α-蒎烯、β-蒎烯和異戊二烯三種生物源前體物臭氧氧化所生成的二次顆粒物作為研究對象,通過測定煙霧箱中在相同酸性不同硫含量無機(jī)種子氣溶膠存在的條件下,三種生物源前體物臭氧氧化生成的顆粒物中有機(jī)硫與有機(jī)碳的變化量,確定OSs中有機(jī)碳與有機(jī)硫的相關(guān)性關(guān)系,實(shí)驗(yàn)數(shù)據(jù)的線性擬合結(jié)果表明OSs中有機(jī)碳與有機(jī)硫的摩爾比為10:1。另外,無機(jī)種子氣溶膠酸度對二次有機(jī)氣溶膠中有機(jī)硫酸根(Organic Sulfates,OS)含量和產(chǎn)率的影響大于其硫含量。本文針對深圳市四個不同特征污染源地區(qū)的PM2.5樣品中OSs的污染特征進(jìn)行了分析,發(fā)現(xiàn)深圳市冬季大氣環(huán)境中OSs的質(zhì)量濃度平均為2.71μgC/m~3,占顆粒物TOC的29.42%;深圳市夏季大氣環(huán)境中OSs的質(zhì)量濃度平均為1.18μgC/m~3,占顆粒物TOC的13.76%,占PM2.5質(zhì)量的2.43%;四個不同特征污染源采樣點(diǎn)的OSs的質(zhì)量濃度大小依次為某電廠龍華西麗HITSZ,OSs占顆粒物TOC的大小依次為龍華某電廠西麗HITSZ。另外,對PM2.5各組分進(jìn)行相關(guān)性分析,發(fā)現(xiàn)OSs中OS與顆粒物上的IS呈現(xiàn)顯著正相關(guān)性,說明OSs可能是由IS通過一系列大氣化學(xué)反應(yīng)轉(zhuǎn)化而形成的。
[Abstract]:Organic Sulfate compounds (Organo sulfates) is a new organic component found in atmospheric particulate matter in recent years. Some studies have shown that the proportion of OSs in atmospheric particulate matter is also larger in the area with higher concentration of SO2 in ambient air. So it is of great significance to study the characteristics of OSs pollution and evaluate the contribution of OSs to atmospheric particulates in China. In this paper, an indirect method for the determination of OSs in atmospheric particulates is established. By indirectly determining the content of common group sulfate in OSs, and based on the molar ratio of organic carbon to organic sulfur in OSs obtained from smoke box, the carbon content of OSs is estimated. In this paper, sodium dodecyl sulfate was chosen as the substitute standard of OSs, and the dissociation method of OSs was established and optimized. The content of sulfate in particles before and after dissociation was determined by ion chromatography. At the same time, the content of sulfate in OSs was obtained by differential subtraction. In order to determine the applicability of this method to the determination of OSs in actual atmospheric particulates, a series of mixed systems of inorganic and organic sulfur with different molar ratios have been designed in this paper. The method was used to determine the recovery and precision of Inorganic Sulfatesl (ISS) and Total Sulfatesl (TS) in the mixed system. The error analysis of the content of sulfate in the obtained OSs was carried out. The results show that the error range of the established quantitative method of sulfate in OSs is 5.74 ~ 37.71. The secondary particles produced by ozone oxidation of three biological precursors, 偽 -pinene, 尾 -pinene and isoprene, were selected as the research object. The change of organic sulfur and organic carbon in particulate matter produced by ozonation of three biological precursors and the correlation between organic carbon and organic sulfur in OSs were determined. The linear fitting results of experimental data showed that the molar ratio of organic carbon to organic sulfur in OSs was 10: 1. In addition, the effect of the acidity of inorganic seed aerosol on the content and yield of organic sulfate in secondary organic aerosol is greater than that of sulfur content. In this paper, the characteristics of OSs pollution in PM2.5 samples from four different pollution source areas in Shenzhen were analyzed. It was found that the average mass concentration of OSs in the atmospheric environment in winter in Shenzhen was 2.71 渭 g / m ~ (-1), accounting for 29.42% of the TOC of particulate matter, and that in the atmospheric environment of Shenzhen in summer was 1.18 渭 g C / m ~ (3), which accounted for 13.76 渭 g / m ~ (3) of TOC and 2.43% of the mass of PM2.5. The quality concentration of OSs at the source sampling point was in turn the size of the TOC of the particles occupied by HITSZOSs in a power plant was the same as that of Xiili HITSZ of a power plant in Longhua power plant. In addition, the correlation analysis of PM2.5 components showed that OS in OSs was positively correlated with is in particulate matter, which suggested that OSs might be formed by a series of atmospheric chemical reactions.
【學(xué)位授予單位】：哈爾濱工業(yè)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X513

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