本文選題：生物氣溶膠 + 燃燒影響　； 參考：《中國(guó)科學(xué)技術(shù)大學(xué)》2017年博士論文

【摘要】：不同地區(qū)氣溶膠的成分差別很大,城市作為人口密度集中的聚居地,健康問題是我們不可忽視的部分。生物源的氣溶膠是大氣氣溶膠的重要組成部分,對(duì)全球的氣候變化和環(huán)境健康起著重要的作用。一方面可以通過反射太陽(yáng)輻射改變大氣層的溫度以及作為云凝結(jié)核和冰核從而直接或間接的影響氣候變化。另一方面存在于空氣中的病毒、細(xì)菌、真菌等會(huì)傳播動(dòng)植物疾病,威脅人類健康。隨著城市的發(fā)展,霧霾事件頻繁出現(xiàn),現(xiàn)代城市人感染哮喘和過敏的幾率也越來越大。傳統(tǒng)的生物氣溶膠的檢測(cè)手段通常耗時(shí)較長(zhǎng),且不能精確的統(tǒng)計(jì)其在大氣中的濃度,因此需要有高效的方法對(duì)城市生物氣溶膠進(jìn)行檢測(cè)。近年來熒光檢測(cè)技術(shù)得到了快速的發(fā)展,出現(xiàn)了在線檢測(cè)生物氣溶膠的儀器,但是目前在國(guó)內(nèi)的應(yīng)用范圍還很小。生物源揮發(fā)性有機(jī)物(BVOC)是生物源的二次有機(jī)氣溶膠(SOA)的前體物質(zhì),占全球揮發(fā)性有機(jī)物(VOC)排放的主要部分。海洋作為地表覆蓋率最高的區(qū)域,對(duì)全球氣候變化起著重要的調(diào)節(jié)作用,遠(yuǎn)洋大氣亦可以作為研究城市大氣環(huán)境的背景地區(qū),研究海洋上空BVOC可以更好的了解遠(yuǎn)洋SOA的生成。對(duì)遠(yuǎn)洋氣溶膠穩(wěn)定碳氮同位素的研究可以幫助探討遠(yuǎn)洋氣溶膠的來源和傳輸過程。本研究依據(jù)兩次國(guó)內(nèi)的野外監(jiān)測(cè)和第29次以及第30次南極科學(xué)考察,第一次使用熒光在線氣溶膠儀器對(duì)國(guó)內(nèi)污染城市進(jìn)行了生物氣溶膠的檢測(cè)并探討了海洋排放的BVOC及其對(duì)海洋SOA的貢獻(xiàn)以及遠(yuǎn)洋地區(qū)穩(wěn)定碳氮同位素的分布。得到主要內(nèi)容和結(jié)論如下:(1)城市地區(qū)的熒光氣溶膠的濃度高于背景地區(qū)1-2個(gè)數(shù)量級(jí)。南京和廈門地區(qū)寬頻綜合生物氣溶膠光譜儀(WIBS)在線檢測(cè)的熒光氣溶膠的濃度分別為 FL1:0.57 cm-3,FL2:3.35 cm-3,FL3:2.09 cm-3 和 FL1:0.24 cm-3,FL2:0.78 cm-3,FL3:0.40 cm-3。南京地區(qū)的熒光氣溶膠出現(xiàn)明顯的日夜變化特征,而廈門地區(qū)晝夜變化不明顯。熒光氣溶膠的濃度都隨著粒徑的增加而逐漸降低。粒徑在1-2 μm的顆粒物占熒光氣溶膠的主導(dǎo)地位,所有粒徑在3.8 μm以上的顆粒物都有FL2熒光信號(hào)。南京地區(qū)的熒光氣溶膠的AF(Asymmetry Factor)呈現(xiàn)單峰分布的模式,峰值為～24,而廈門地區(qū)的呈現(xiàn)雙峰分布的模式,峰值為～23和～30,說明南京地區(qū)熒光顆粒物的形狀分布比較單一。(2)熒光氣溶膠的濃度在一定程度上受當(dāng)?shù)貧庀髤?shù)的影響,一定的風(fēng)速會(huì)增加植物花粉和孢子的排放,導(dǎo)致生物氣溶膠的濃度上升。但當(dāng)風(fēng)速超過一定閾值時(shí),會(huì)加快大氣顆粒物的擴(kuò)散速度,導(dǎo)致當(dāng)?shù)厣餁馊苣z的濃度降低。降雨之前生物氣溶膠的濃度會(huì)上升,溫度和濕度也可以影響生物氣溶膠的釋放。(3)南京地區(qū)的生物氣溶膠顯著的高于一些森林等生物氣溶膠含量豐富的背景地區(qū),尤其是FL1熒光通道與MBC/PM0.8示了很好的正相關(guān)性(r=0.75),因此直接用WIBS儀器的三個(gè)熒光通道來代表生物氣溶膠并不合適。根據(jù)熒光強(qiáng)度和占總顆粒物的比例與MBC/PM0.8的相關(guān)性,將熒光氣溶膠分成了燃燒排放相關(guān)的和非燃燒相關(guān)的顆粒物兩類。燃燒排放相關(guān)的熒光顆粒物和非燃燒排放相關(guān)的熒光顆粒物分別占總顆粒物的～11%和～5%。非燃燒相關(guān)的顆粒物濃度為0.64 cm-3仍然高于其他文獻(xiàn)報(bào)道的南京地區(qū)生物氣溶膠的濃度,因此并不能確定非燃燒相關(guān)的熒光顆粒物就是生物氣溶膠,可能包含了灰塵等其他的顆粒物。(4)第29次南極科學(xué)考察航線上的異戊二烯和α蒎烯、β蒎烯的濃度分別為113 pptv、28 pptv和14 pptv。異戊二烯的濃度顯著高于單萜,三者之間有很好的相關(guān)性。整個(gè)航線上異戊二烯和單萜的地理分布沒有顯著性差異,普里茲灣表現(xiàn)出很高的異戊二烯和單萜濃度,和普利滋區(qū)域藍(lán)藻爆發(fā)有一定的關(guān)系。不同浮游植物的種類、風(fēng)速和溫度都會(huì)影響海洋大氣異戊二烯和蒎烯的濃度分布。普里茲灣異戊二烯生成的SOA占全球海洋排放異戊二烯生成SOA的0.03%。(5)第30次南極航線上氣溶膠總懸浮顆粒物中總碳的質(zhì)量濃度(TC)平均值為1±0.81 μgm-3 TC的濃度隨著緯度的升高逐漸降低(r=0.58,p0.01)低緯度的TC受到陸地的影響較大。整個(gè)航線上有29%的樣品未檢出總氮(TN),TN的平均濃度為0.49±0.74 μg m-3,整體濃度偏低,且遠(yuǎn)遠(yuǎn)低于大城市中的濃度。TN的濃度也隨著緯度的升高而降低(r=0.37,p0.01)。穩(wěn)定碳同位素δ13C的平均值為-27±3.3‰,且513C與TC有一定的相關(guān)性(r=0.34,p0.05)。穩(wěn)定氮同位素515N的平均值為0.9±3.3‰,與TN沒有相關(guān)性。δ13C和δ15N的分布與緯度都沒有相關(guān)性。低緯度的樣品受到亞洲大陸和菲律賓群島,澳洲大陸兩部分氣團(tuán)的影響,受亞洲大陸和菲律賓群島氣團(tuán)影響的樣品中的碳氮可能來源于陸地的生物質(zhì)燃燒。中緯度地區(qū)樣品可能受到南極大陸塵埃的影響。高緯度地區(qū)的碳氮與海洋浮游植物的排放有一定的關(guān)系。
[Abstract]:The composition of aerosol is very different in different regions. As a place where population density is concentrated, the health problem is the part that we can not ignore. The aerosol of the biogenic source is an important part of the atmospheric aerosol. It plays an important role in the global climate change and environmental health. The temperature of the atmosphere, as well as as a cloud of nodules and ice nuclei, directly or indirectly affects climate change. On the other hand, the virus, bacteria and fungi in the air can spread animal and plant diseases and threaten human health. With the development of the city, the haze events frequently occur, and the risk of asthma and allergy in modern urban people is also increasing. The traditional detection methods of biological aerosol are usually time-consuming and can not accurately count their concentration in the atmosphere. Therefore, it is necessary to have a high efficient method for the detection of urban bioaerosols. In recent years, the fluorescence detection technology has been developed rapidly, and the instrument for on-line detection of biological aerosol has appeared, but it should be in the country at present. The biological volatile organic compounds (BVOC) are the precursors of the two organic aerosol (SOA) of the biogenic source, which account for the major part of the global emissions of volatile organic compounds (VOC). As the region with the highest surface coverage, the ocean plays an important role in the global climate change, and the ocean atmosphere can also be used as a research city. The study of BVOC over the ocean can better understand the formation of ocean SOA in the background of the air environment. The study of the stable carbon and nitrogen isotopes of the sols can help to explore the source and transmission process of oceanic aerosols. This study was based on two domestic field monitoring and twenty-ninth and thirtieth Antarctic scientific expedition, for the first time. The BVOC and its contribution to marine SOA and the distribution of stable carbon and nitrogen isotopes in ocean areas are discussed. The main contents and conclusions are as follows: (1) the concentration of fluorescent gas solution in urban areas is 1-2 orders of magnitude higher than that in the background area. The concentration of fluorescent aerosol detected on line by WIBS in Beijing and Xiamen region was FL1:0.57 cm-3, FL2:3.35 cm-3, FL3:2.09 cm-3 and FL1:0.24 cm-3, FL2:0.78 cm-3. The fluorescent aerosols in Nanjing region showed obvious diurnal change characteristics, while the day and night changes in Xiamen were not obvious. The concentration of the fluorescent aerosol gradually decreases with the increase of the particle size. The particles with a particle size of 1-2 mu m occupy the dominant position of the fluorescent aerosol, and all the particles with a particle size of more than 3.8 m have FL2 fluorescence signals. The AF (Asymmetry Factor) of the fluorescent aerosol in Nanjing region shows a single peak distribution pattern, the peak value is 24, and the Xiamen region has a peak value. The pattern of Shuangfeng distribution is 23 and 30, which indicates that the shape distribution of the fluorescent particles in Nanjing is relatively simple. (2) the concentration of the fluorescent aerosol is influenced by the local meteorological parameters to a certain extent. A certain wind speed will increase the emission of pollen and spores of plants and lead to the increase of the concentration of the biological aerosol. When a certain threshold is passed, the diffusion rate of atmospheric particles will be accelerated and the concentration of the local biological aerosol is reduced. The concentration of biological aerosols will rise before rainfall, and the temperature and humidity can also affect the release of biological aerosols. (3) the biological aerosols in the Nanjing region are significantly higher than those of some forests and other bioaerosols. The region, especially the FL1 fluorescent channel, shows good positive correlation with MBC/PM0.8 (r=0.75), so it is not appropriate to represent the biological aerosols directly with the three fluorescent channels of the WIBS instrument. According to the correlation of the fluorescence intensity and the proportion of the total particles to the MBC/PM0.8, the fluorescence aerosol is divided into the combustion emission related and non combustion phase. Two kinds of particulate matter. The emission related emission related fluorescent particles and non combustion emission related fluorescent particles accounted for 11% of the total particles and the concentration of non combustion related particles of 0.64 cm-3 were higher than those of other literature reported in Nanjing. Therefore, the non combustion related fluorescence was not determined. Particles are bioaerosols, which may contain other particles such as dust. (4) the concentration of isoprene and alpha pinene on the twenty-ninth Antarctic scientific voyage routes, the concentration of beta pinene is 113 pptv, 28 pptv and 14 pptv. isoprene are significantly higher than monoterpene, and the three are well correlated. There is no significant difference in the geographical distribution of terpenes. Prisi Bay shows a high concentration of isoprene and monoterpene, which has a certain relationship with the explosion of cyanobacteria in the prisi region. The species of phytoplankton, wind speed and temperature will affect the concentration distribution of isoprene and pinene in the ocean atmosphere. The SOA of the isoprene in prise Bay accounts for the global sea. The mass concentration of total carbon in aerosol total suspended particulate matter (TC) on 0.03%. (5) on the thirtieth Antarctic route of isoprene generated SOA was 1 + 0.81 mu GM-3 TC as the latitude increased gradually (r=0.58, P0.01), and the low latitude TC was greatly affected by land. 29% samples were not detected total nitrogen (TN), TN on the whole route. The average concentration is 0.49 + 0.74 g M-3, the whole concentration is low, and the concentration of.TN is also lower than that in the large cities (r=0.37, P0.01). The average value of the stable carbon isotope Delta 13C is -27 + 3.3 per thousand, and 513C and TC have some correlation (r=0.34, P0.05). The average value of the stable nitrogen isotope 515N is 0.9 + 3.3 per thousand. There is no correlation with TN. The distribution of delta 13C and delta 15N has no correlation with latitude. The low latitude samples are affected by the Asian continent and Philippines islands, the two parts of the Australian continent, and the carbon and nitrogen in the samples affected by the Asian continent and the Philippines archipelago may be derived from the biomass burning on the land. The influence of the dust on Antarctica is related to the carbon and nitrogen in high latitudes and the discharge of marine phytoplankton.

【學(xué)位授予單位】：中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：X513

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