發(fā)布時間：2018-08-07 14:56

【摘要】：有機氣溶膠能夠影響大氣顆粒物的物理化學特性,如粒徑、光學特性和吸濕性等,進而通過對太陽光的散射和吸收影響大氣能見度和氣候變化。當前大量的研究主要集中針對中國華北地區(qū)重度灰霾大氣中氣溶膠的物理化學特性,卻忽略了發(fā)生最頻繁的輕及中度霾中氣溶膠顆粒的物理化學特性。近20年,中國華北平原頻繁發(fā)生輕及中度霾,這些顆粒物中占比最大的有機物氣溶膠的形貌和混合狀態(tài)目前還未知�；诖�,了解輕及中度霾中大氣氣溶膠的物理化學特性,對進一步評估它們對氣候和人體健康的影響具有重要的科學意義。本研究于2014年12月13至23日進行了一次大規(guī)模區(qū)域性氣溶膠外場觀測實驗,采樣地點選擇在城市點-濟南(S1)、高山站點-泰山(S2)和區(qū)域性污染的大氣背景點-長島(S3)。本研究采集了氣溶膠單顆粒樣品和PM2.5樣品,應用離子色譜分析儀和OCEC分析儀分析了各采樣點灰霾天及清潔天的無機水溶性離子組分和OC、EC濃度。針對單顆粒樣品分析,本研究使用帶能譜的透射電子顯微鏡(TEM-EDX)、原子力顯微鏡(AFM)和納米二次離子質(zhì)譜分析儀(NanoSIMS)等微觀分析儀器,分析了華北平原輕及中度灰霾中有機物氣溶膠單顆粒的粒徑、形貌和混合狀態(tài)。該研究還進一步結(jié)合氣流后向軌跡(HYSPLIT)模型獲得華北平原輕及中度霾中有機氣溶膠來源及老化過程,并對不同采樣點有機物的特性進行對比分析。此外,本研究初步探索了華北平原冬季輕及中度霾大氣中幾種典型有機氣溶膠顆粒物的耐熱特性。透射電鏡分析結(jié)果顯示,在灰霾期間顆粒物的主要類型有六種:硫酸鹽(包括鉀鹽和硫酸銨)、金屬、飛灰、礦物顆粒、煙塵和有機物。其中,含有機物的顆粒物在所有灰霾樣品(共5090個單顆粒)中最為豐富,占比約為70%。基于有機顆粒的形貌特征,將其分為六種類型:圓形(類型1)、近圓形(類型2)、不規(guī)則狀(類型3)、半透明穹頂狀(類型4)、濺射狀(類型5)和有機包裹物(類型6)。華北平原輕及中度霾大氣中類型1-3的有機物占比最大,并且大部分是內(nèi)部混合于非有機氣溶膠�；谕干潆婄R的較高分辨率,本研究發(fā)現(xiàn)華北平原冬季區(qū)域性灰霾中約86%的有機物內(nèi)部混合于非有機氣溶膠,如煙塵、礦物、金屬、飛灰和硫酸鹽顆粒。根據(jù)混合組分的不同,將有機物內(nèi)混顆粒分為四類:有機物-煙塵顆�；旌项w粒、有機物-飛灰/金屬混合顆粒、有機物-硫酸鹽混合顆粒和有機物-礦物混合顆粒。研究結(jié)果顯示,約83%的類型1-4有機物與煙塵顆粒、礦物、金屬和硫酸鹽顆粒發(fā)生內(nèi)混,只有17%的類型1-4有機物是外部混合,而類型5-6有機物都是與無機鹽以內(nèi)混形式存在。S2和S3采樣點采集的含有機物的單顆粒粒徑分析顯示二者顆粒物的粒徑峰值一致,約400nm,而S1站點則是在600nm。此結(jié)果表明本地源直接排放的含有機物顆粒粒徑比長距離傳輸后的顆粒粒徑大。本研究中,進一步獲得三個采樣點采集的類型1-3有機物的粒徑分布,結(jié)果顯示在同一灰霾事件中類型1-3有機物的粒徑峰值是一致的(約350nm)。本研究發(fā)現(xiàn)華北平原同一灰霾事件中不同采樣點的有機物來源具有很大相似性。本研究討論了華北平原區(qū)域性輕及中度霾中有機氣溶膠顆粒物的來源。結(jié)果顯示冬季華北平原大量存在的類型1-3有機物是由缺乏控制措施的家用燃爐或小型鍋爐燃煤或燃燒秸稈所排放,尤其是具有高圓度和低長寬比的近圓形有機物占比較大,它們是在燃煤或秸稈燃燒排放出來的污染煙氣的冷卻過程中形成。本研究中為了評估有機物的來源,與室內(nèi)實驗進行結(jié)合,采集實驗室燃煤和秸稈燃燒排放出來的新鮮顆粒物,對比分析了灰霾大氣、燃煤及秸稈燃燒產(chǎn)生的有機物中Si、O、C的比值。結(jié)果發(fā)現(xiàn)71%的類型1-3有機物與燃煤排放的有機物相符。本研究結(jié)果顯示在華北平原,缺乏控制措施的家用燃爐或小型鍋爐的燃煤污染物排放是個從城市至農(nóng)村廣泛存在的污染源。此外,本研究分析了華北平原有機氣溶膠的老化過程,發(fā)現(xiàn)有機包裹物的平均厚度從S1至S2至S3顯示出微弱的增長,或間接表明低濕度條件下輕及中度霾大氣中氣溶膠和氣體之間的非均相反應和光化學反應的程度較弱。這與本研究中發(fā)現(xiàn)的一次有機物(類型1-3)占比較高,二次有機物(類型6)占比較小的結(jié)果相一致。本研究對華北平原冬季輕及中度霾大氣中幾種典型有機氣溶膠單顆粒的耐熱特性做了研究,結(jié)果發(fā)現(xiàn)經(jīng)過300攝氏度及500攝氏度的加熱過程之后,類型1圓形有機物的形貌相對穩(wěn)定,類型6有機包裹物的厚度變薄。有機物-煙塵混合顆粒在溫度為300度至500度的加熱過程中粒徑縮小。類型4穹頂狀有機物含有300度下?lián)]發(fā)和不揮發(fā)的有機物,類型5濺射狀有機物含有在500度下?lián)]發(fā)和不揮發(fā)的有機物。對于類型5濺射狀有機物和類型6有機包裹物中混合的無機鹽則在加熱至300攝氏度的過程中揮發(fā)完全。本論文研究了華北平原冬季常見灰霾中有機氣溶膠單顆粒的物理化學特性,通過分析灰霾大氣中有機物與室內(nèi)燃煤及秸稈燃燒排放出的有機物中C-O-Si含量的比值,得出結(jié)論:缺乏控制措施的家用燃爐和小型鍋爐的直接排放對華北平原冬季區(qū)域性輕及中度霾有重要影響。這個發(fā)現(xiàn)為華北平原地區(qū)進一步治霾提供重要的事實依據(jù),對探究不同灰霾事件形成及評估它們對氣候變化和人類健康的影響提供重要參考。
[Abstract]:Organic aerosols can affect the physical and chemical properties of atmospheric particles, such as particle size, optical properties and hygroscopicity, and then influence the atmospheric visibility and climate change through the scattering and absorption of solar light. A large number of current studies focus on the physical and chemical properties of the aerosol in the heavy haze atmosphere in North China, but ignore the physical and chemical properties of the aerosol. The physical and chemical properties of aerosol particles in the most frequent light and moderate haze occurred. In recent 20 years, light and moderate haze occurred frequently in the North China Plain. The morphology and mixing state of the largest organic aerosols in these particles were unknown. Based on this, the physical and chemical properties of atmospheric aerosols in light and medium haze were understood. One step to assess their impact on climate and human health is of great scientific significance. In this study, a large-scale regional aerosol outfield observation experiment was conducted on 13 to 23 December 2014. The sampling sites were selected at the city point Ji'nan (S1), the alpine site Taishan (S2) and the regional pollution atmospheric background - Long Island (S3). The aerosol single particle samples and PM2.5 samples were collected. The inorganic water-soluble ionic components and OC, EC concentration of the haze days and cleaning days were analyzed by ion chromatography and OCEC analyzer. For single particle sample analysis, this study used transmission electron microscopy (TEM-EDX) with energy spectrum, atomic force microscopy (AFM) and two nanoscale times. The particle size, morphology and mixing state of organic aerosol particles in light and moderate haze in North China Plain were analyzed by microanalysis instruments such as ion mass spectrometry (NanoSIMS), and the source and aging process of organic aerosols in light and medium haze in North China Plain were further combined with the HYSPLIT model. In addition, the heat resistance of several typical organic aerosol particles in the light and moderate haze atmosphere in the North China Plain was preliminarily investigated. The transmission electron microscope analysis showed that there were six main types of particulate matter during the haze: sulphate (including potassium and ammonium sulfate), metal, and fly. Ash, mineral particles, smoke and organic matter. Among them, the particles containing the machine are the most abundant in all the haze samples (5090 single particles). The proportion is about 70%. based on the morphology of organic particles. It is divided into six types: round (type 1), near circular (type 2), irregular (type 3), translucent dome like (type 4), sputtering (Class 4). Type 5) and organic inclusions (type 6). The type 1-3 organic matter in the light and moderate haze atmosphere of the North China Plain is the largest, and most of them are mixed in the non organic aerosol. Based on the high resolution of transmission electron microscopy, this study found that about 86% of the organic matter in the regional haze in the North China Plain is mixed with non organic aerosols in winter. Smoke, minerals, metals, fly ash and sulphate particles. According to the difference of the mixed components, the mixed particles in the organic matter are divided into four types: organic matter - dust particles, organic matter - fly ash / metal mixed particles, organic matter sulfate mixed particles and organic matter - mineral mixture particles. The results show that about 83% of the 1-4 organic compounds and tobacco Dust particles, minerals, metals and sulphate particles have internal mixing. Only 17% of the type 1-4 organic compounds are external mixed, and type 5-6 organic matter is the single particle size analysis of the organic matter in the form of.S2 and S3 sampling in the form of inorganic salts, which shows that the particle size peak of the two particles is the same, about 400nm, while the S1 site is in 600nm. The results show that the particle size of the local source has a larger particle size than the long distance transmission. In this study, the particle size distribution of the type 1-3 organic matter collected at three sampling points is further obtained. The results show that the peak diameter of type 1-3 organic matter in the same haze event is the same (about 350nm). The sources of organic matter from different sampling points in the same haze event in the North China Plain are very similar. The source of organic aerosol particles in the light and moderate haze in the North China Plain is discussed. The results show that a large number of 1-3 organic compounds in the North China Plain in winter are burned by a household burning furnace or a small boiler which is not controlled. Coal or burning stalks, especially the near circular organic compounds with high roundness and low width and width ratio, are relatively large, they are formed during the cooling process of the polluted flue gas emitted by coal or straw combustion. In this study, in order to evaluate the source of organic matter, combined with laboratory experiments, the emission of coal and straw combustion in the laboratory is collected. The ratio of Si, O and C in the organic matter produced by the haze atmosphere, coal and straw combustion was compared and analyzed. The results showed that 71% of the type 1-3 organic matter was in accordance with the coal fired organic matter. The results of this study showed that the emission of coal combustion in the household combustion furnace or small boiler which was not controlled in the North China Plain was from the North China Plain. In addition, this study analyzed the aging process of organic aerosols in the North China Plain, and found that the average thickness of organic inclusions showed a weak increase from S1 to S2 to S3, or indirectly showed the heterogeneous reaction and photochemical reaction between gas soluble gas and gas in light and moderate haze atmosphere under low humidity. The degree of stress is weak. This is higher than the one found in this study (type 1-3), and the two organic matter (type 6) accounts for a relatively small result. This study has studied the heat resistance of several typical organic aerosol particles in the light and moderate haze atmosphere in the North China Plain in winter. The results were found to be 300 degrees centigrade and 500 subjects. After the heating process, the morphology of type 1 circular organic matter is relatively stable, and the thickness of type 6 organic inclusions is thinner. The mixture particles of organic matter and dust are reduced in the heating process of 300 degrees to 500 degrees. Type 4 dome contains 300 degrees of volatilization and non volatilization organic matter, type 5 sputter organic matter contains The volatilization and non volatilization of organic compounds at 500 degrees. The inorganic salts mixed in type 5 sputter organics and type 6 organic inclusions are volatilized completely during heating to 300 degrees centigrade. The physical and chemical properties of organic aerosol particles in common haze in winter in the North China Plain are studied in this paper. The ratio of C-O-Si content in organic matter and organic matter discharged from coal and straw combustion shows that the direct emission of household burning furnace and small boiler which lacks control measures has important influence on regional light and moderate haze in North China Plain in winter. This discovery provides an important basis for further haze treatment in the North China Plain. It is important to explore the formation and assessment of different haze events and their impact on climate change and human health.
【學位授予單位】：山東大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X513

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