鹿林山背景大氣及受生質燃燒事件影響的氣膠化學特性

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許紹鵬(Shao-peng Hsu) 查詢紙本館藏

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論文名稱

鹿林山背景大氣及受生質燃燒事件影響的氣膠化學特性
(Aerosol chemical characteristics at Mt. Lulin during background and biomass burning event)

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摘要(中)

鹿林山標高2,862公尺，是一個評估東亞大陸污染傳輸和西太平洋背景的適當地點。本研究於2008年9月~2009年4月在鹿林山採集大氣氣膠樣本，並將採集樣本歸類為生質燃燒期間與非生質燃燒期間。兩個期間氣膠水溶性離子優勢物種均為硫酸根離子與銨根離子，但在生質燃燒期間，硝酸根離子與鉀離子濃度會顯著增加。生質燃燒期間，氣膠碳成分分別以OC3和EC1-OP為有機碳(OC)及元素碳(EC)主要物種；非生質燃燒期間，氣膠有機碳的OC1及元素碳的EC2是兩個優勢氣膠碳成分物種。生質燃燒期間與非生質燃燒期間左旋葡萄糖是氣膠無水單醣化合物唯一優勢物種，但以生質燃燒期間濃度增加顯著。生質燃燒期間與非生質燃燒期間氣膠二元酸優勢物種均為oxalic acid，表示oxalic acid是二元酸前驅有機物或是其他二元酸的最終產物，在生質燃燒期間oxalic acid濃度也是增加的。
本研究於觀測期間特別觀測氣膠水可溶有機碳(WSOCp)，發現WSOCp主要由低揮發性的OC2、OC3構成，WSOCp在生質燃燒期間與生質燃燒指標有較好的相關性，顯示WSOCp也可作為評估生質燃燒事件的指標。大氣溫度與WSOCp有良好相關性，降雨會顯著降低WSOCp濃度，但不會影響氣相水可溶有機碳(WSOCg)濃度。去除掉降雨事件後，當相對濕度大於70%時，WSOCp佔(WSOCp+WSOCg)比例會顯著上升。鹿林山氣膠中，硫酸根離子主要與銨根離子(線性相關R2=0.90)結合，少部分與鈣離子、鈉離子結合，硫酸根離子與銨根離子結合型態為(NH4)3(H)(SO4)2。
採樣期間氨氣對硫酸氣和硝酸氣有中和不足現象，雖然生質燃燒期間有較多硝酸鹽產生，但硝酸氣並非中和氨氣的主要氣體。2007~2009年鹿林山氣膠量測和中和所需的銨根離子莫耳比(NH4+?meas/NH4+?calc)平均值為0.79，與歐洲瑞士少女峰1999~2005年觀測的0.8差異不大，顯示中歐及東亞地區氨氣均不足以完全中和硫酸氣和硝酸氣。從2009年春季鹿林山受生質燃燒影響時間較長且?NH4+?meas/?NH4+?calc與硫酸鹽、硝酸鹽相關性(線性相關R2=0.53、0.32)較前兩年為佳；顯示氨氣中和硫酸氣和硝酸氣，可能需要較長的反應時間以形成足夠的氣膠硫酸鹽和硝酸鹽。
本研究總計進行五次雲霧事件的前、中、後氣膠採樣觀測，有四次事件雲霧氣流有挾帶氣膠過來；在雲霧事件中，未中和的銨根離子多，硝酸根離子被活化形成雲滴的效率最好，其次為硫酸根離子，銨根離子的效率最低。氣膠碳成分中，OC的滌除率在不同期間相近。雲霧事件過後，可能有乾淨氣團過來使PM1氣膠濃度下降。

摘要(英)

Mt. Lulin (2,862m a.s.l.) is a suitable site to assess pollution transport from East Asian continent and West Pacific background. This study observed atmospheric aerosol at Mt. Lulin from September 2008 to April 2009 and split the collected samples into from biomass-burning (BB) and non-biomass-burning (NBB) periods. Aerosol water-soluble ions are dominated by sulfate and ammonium ions during both BB and NBB periods. However, aerosol nitrate and potassium ion levels were noticeably increased during BB period. For aerosol carbons during BB period, OC3 and EC1-OP were the major fractions in organic carbon (OC) and elemental carbon (EC), respectively. In contrast, OC1 in OC and EC2 in EC were the two dominant carbon fractions during NBB period. Aerosol levoglucosan was the only dominant species in aerosol anhydrous monosaccharide during both BB and NBB periods. The level of aerosol levoglucosan was significantly increased during BB period. Oxalic acid was the dominant dicarboxylic acids during both BB and NBB periods. This implies that oxalic acid is the precursor species or the end product of other dicarboxylic acids. The concentration of aerosol oxalic acid was also increased during BB period.
Aerosol water-soluble organic carbon (WSOCp) was specifically observed during observation period. The analysis reveals that low-temperature volatiled OC2 and OC3 are the major fractions of WSOCp. The concentration of WSOCp had a better correlation with BB tracers during BB period. It indicates that the WSOCp can be a good tracer for BB event. Atmospheric temperature is found having a good correlation with WSOCp. Rain fall may significantly reduce WSOCp concentration but not for gaseous water-soluble organic carbon (WSOCg). By excluding raining events, the fraction of WSOCp in (WSOCp+WSOCg) is increased when the relative humidity is above 70%. In Mt. Lulin aerosol, sulfate ion is mainly combined with ammonium ion (R2=0.90) and less with calcium and sodium ions. The compound form of sulfate and ammonium ions is (NH4)3(H)(SO4)2.
During the study period, ammonia gas was found insufficient in neutralizing sulfuric and nitric gases. Although more aerosol nitrate was observed during BB period, nitric gas is not a major acidic gas in neutralizing ammonia gas. The mole ratio of measured over calculated aerosol ammonium ions (?NH4+?meas/?NH4+?calc) is averaged at 0.79 for the period of 2007－2009. This value is not deviated too much from 0.8 at Jungfracjoch in European Swiss Alps observed during 1999－2005. It indicates that the ammonia gas in middle Europe and East Asia is insufficient in neutralizing sulfuric and nitric gases. By considering longer BB period and higher linear correlation for ?NH4+?meas/?NH4+?calc with aerosol sulfate and nitrate (R2=0.53 and 0.32, respectively) in 2009 spring, this study infers that ammonia gas probably needs more time in neutralizing sulfuric and nitric gases to form sufficient aerosol sulfate and nitrate.
Five cloud events were observed to collect aerosols at pre-cloud, in-cloud, and post-cloud periods in this study, respectively. Four cloud events transported aerosols to the collection site. Excess ammonium ion not neutralized is found in cloud event. The activation efficiency of water-soluble ions in the cloud event is the best for nitrate ion, followed by sulfate and ammonium ions. For aerosol carbon fractions, the scavenging ratio of OC is similar in different time periods. PM1 concentration is observed to drop after cloud event, which is probably due to cleaner air masses transported to the site.

關鍵字(中)

★ 高山測站
★ 氣膠水可溶有機碳
★ 氣膠中和
★ 雲霧事件
★ 生質燃燒

關鍵字(英)

★ Biomass burning
★ Cloud events
★ Aerosol neutralization
★ Aerosol water-soluble organic carbons
★ High-elevation site

論文目次

摘要 I
Abstract II
致謝 IV
圖目錄 VIII
表目錄 XII
第一章前言 1
1.1 研究緣起 1
1.2 研究目的 2
第二章文獻回顧 3
2.1 高山氣膠 3
2.2 水可溶有機碳 4
2.3 氣膠中和 6
2.4 雲霧事件 8
2.4.1 雲霧事件對於氣膠成分影響 8
2.4.2 活化效率 8
2.5 生質燃燒指標物 10
2.5.1 生質燃燒氣體特性 10
2.5.2 生質燃燒氣膠化學特性 10
(1) 氣膠水溶性離子 10
(2) 氣膠碳成分 11
(3) 氣膠左旋葡萄糖 12
2.6 歷年鹿林山研究成果 14
2.6.1 生質燃燒期間 14
2.6.2 非生質燃燒期間 15
第三章研究方法 16
3.1 研究架構 16
3.2 採樣方法與採樣器 18
3.2.1 採樣地點描述 18
3.2.2 採樣儀器 20
(1) 人工採樣器 20
(2) 自動監測儀器 20
(3) PILS (Particle-Into-Liquid Sampler) 22
3.2.3 採樣濾紙選擇及前處理程序 23
(1) 儀器與濾紙配置 23
(2) 濾紙的前處理 25
(3) 樣本的運送與保存 26
3.3 樣本分析方法 27
3.3.1 氣膠質量濃度分析 27
3.3.2 氣膠水溶性離子與氣膠二元酸分析 27
(1) 水溶性離子與二元酸濾紙萃取步驟 27
(2) 水溶性離子與有機酸分析儀器 28
3.3.3 氣膠碳成分 30
(1) 氣膠碳成分分析 30
(2) 揮發性有機碳(VOC)與氣膠揮發性有機碳(PVOC)推估 32
3.3.4 氣膠有機成分分析－左旋葡萄糖 32
3.3.5 水可溶有機碳分析 34
(1) 水可溶有機碳濾紙萃取步驟 34
(2) 水可溶有機碳分析儀器 35
3.3.6 氣膠酸鹼中和分析-?NH4+?meas/?NH4+?calc計算 36
3.4雲霧氣膠的收集 37
3.4.1 氣膠受雲霧事件活化效率計算方式 37
3.5判別事件發生方法 38
3.5.1 NOAA HYSPLIT軌跡模式 38
3.5.2 美國太空總屬(NASA)自然災害網 39
3.5.3 全球火災監測中心(GFMC) 40
3.5.4 NCEP Global Tropospheric Analyses資料 40
3.6 本文採樣期間逆推軌跡分類 41
第四章結果與討論 43
4.1觀測期間氣膠各成分變化 46
4.1.1 PM10及PM2.5氣膠質量濃度 46
4.1.2 PM2.5氣膠水溶性離子與前驅氣體濃度 47
4.1.3 PM2.5氣膠碳成分濃度 50
4.1.4 PM2.5氣膠單醣無水化合物濃度 52
4.1.5 PM2.5氣膠二元酸濃度 53
4.1.6 生質燃燒期間與非生質燃燒期間氣膠各成分變化 53
4.1.7 觀測期間各氣流軌跡氣膠各化學成分變化 58
4.2 歷年鹿林山站氣膠化學成分變化 61
4.2.1 歷年鹿林山站氣膠質量濃度與氣膠化學成分變化 61
4.2.2 歷年鹿林山站各氣流軌跡對PM2.5氣膠化學成分變化 64
4.3氣膠水可溶有機碳 69
4.3.1 鹿林山站採樣觀測期間PM2.5 氣膠相水可溶有機碳 69
4.3.2 PM2.5 氣膠相水可溶有機碳與相關氣體污染物及氣象因子 70
4.3.3 生質燃燒和非生質燃燒煙團對PM2.5氣膠相水可溶有機碳的影響 72
4.3.4 密集觀測期間PM2.5 水可溶有機碳氣固相變化 75
4.4 PM2.5 氣膠酸度與氨氣中和硫酸氣、硝酸氣狀態 79
4.4.1 PM2.5 氣膠結合型態 79
4.4.2 鹿林山採樣觀測期間PM2.5氣膠?NH4+?meas/?NH4+?calc莫耳濃度比 83
4.4.3 2007~2009年不同事件下鹿林山PM2.5氣膠?NH4+?meas/?NH4+?calc莫耳濃度比 84
4.4.4 2007~2009年春季鹿林山不同氣流來源 ?NH4+?meas/?NH4+?calc莫耳濃度比 85
4.5 雲霧事件 89
4.5.1 雲霧事件發生前後鹿林山氣膠變化 89
(1) 第一次雲霧事件 (30 Oct 2008) 92
(2) 第二次雲霧事件 (01 Nov 2008) 98
(3) 第三次雲霧事件 (08 Feb 2009) 104
(4) 第四次雲霧事件 (10Feb 2009) 110
(5) 第五次雲霧事件 (17Apr 2009) 117
4.5.2 不同氣流來源雲霧事件鹿林山氣膠變化 126
4.5.3 不同風向雲霧事件鹿林山氣膠變化 128
4.5.4 氣膠受雲霧事件活化效率 130
第五章結論與建議 131
5.1 結論 131
5.1.1 生質燃燒期間與非生質燃燒期間氣膠化學成分差異 131
5.1.2 水可溶有機碳 132
5.1.3 PM2.5 氣膠酸度與氨氣中和硫酸氣、硝酸氣狀態 132
5.1.4 雲霧事件 134
5.2 建議 135
第六章參考文獻 136
附錄一口試委員意見回覆 147
附錄二 2008年9月到2009年4月觀測期間鹿林山站氣流逆推軌跡 159

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指導教授

李崇德(Chung-te Lee)

審核日期

2010-1-27

推文