2011年生質燃燒期間越南山羅高地和台灣鹿林山氣膠特性

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張家宏(JIA HONG CHANG) 查詢紙本館藏

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環境工程研究所

論文名稱

2011年生質燃燒期間越南山羅高地和台灣鹿林山氣膠特性
(Aerosol characteristics at Son La Height in Vietnam and at Mountain Lulin in Taiwan during biomass burning or non-biomass burning period in 2011)

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摘要(中)

本文於2011年3月在越南山羅(海拔682公尺)及台灣鹿林山(海拔2,862公尺)以採集PM10及PM2.5濾紙氣膠進行化學分析，目的是瞭解近生質燃燒源及生質燃燒氣團經過長程傳輸後氣膠特性。。
結果發現越南山羅觀測前期(3月18至21日)同時受到生質燃燒和傳輸沙塵影響，PM10-2.5及PM2.5氣膠成分以碳成分為主，且PM10-2.5及PM2.5氣膠質量濃度高於PM2.5；觀測後期(3月22至31日)則同時受到生質燃燒和中國南方污染傳輸影響，水溶性離子比例上升並主導氣膠質量，特別是SO42-佔PM2.5質量的改變最為明顯。觀測後期C3/C4比值(0.40)略高於觀測前期(0.34)，顯示中國南方氣膠成分較溶於水且受到光化氧化程度較高。觀測期間，生質燃燒指標物nss-K+與levoglucosan、Char-EC/Soot-EC相關性(R2>0.5)良好，印證受到生質燃燒的影響。
受到生質燃燒傳輸氣流影響時，鹿林山PM2.5氣膠質量濃度增加為4.1倍，PM2.5總碳濃度增加為3.8倍，左旋葡萄糖增加為4.3倍，PM2.5水溶性離子增加3.1倍，其中以nss-K+增加5.4倍最多，顯示左旋葡萄糖及nss-K+都是生質燃燒氣膠指標物。越南山羅及鹿林山受生質燃燒影響時，有氨氣不足的現象，鹿林山未受生質燃燒傳影響時，則是趨近完全中和，顯示生質燃燒煙團氣膠較偏酸性。
越南山羅觀測前期PM2.5氣膠在大氣相對濕度60%以上主要的固體結合型態是Oxalic‧2H2O(s)，觀測後期則是(NH4)2SO4和(NH4)3(H)(SO4)2，鹿林山PM2.5氣膠無論是否受到生質燃燒傳輸氣流影響，在大氣相對濕度60%以上主要的固體結合型態都是(NH4)2SO4。這些不同化合物對太陽輻射衰減程度也會有所差別，在評估環境效應有重要的意義。
氣膠含水量可表示在高濕度大氣下氣膠吸濕粒徑增大能力，因而對太陽輻射衰減程度評估也是重要因子。本文彙整2008年至2011年在鹿林山量測的氣膠含水量，多元迴歸分析顯示PM10氣膠含水量無論在BB及NBB時期都選SO42-及WSOC-HULIS_C (代表WSOC扣減掉重要疏水性成分)為重要預測因子，PM2.5氣膠含水量則無論在任何時期最主要的影響因子都是NH4+，顯示氣膠成分對對氣膠含水量的貢獻取決於物種和濃度。

摘要(英)

This work collected filter-based PM10 and PM2.5 samples at Son La (682 m a.s.l., Vietnam) in March 2011 and Mt. Lulin (2,862 m a.s.l., Taiwan) from March to April 2011 for analyzing their chemical compositions. The aim of this work is to understand aerosol characteristics from near-source biomass burning (BB) and BB plume after long-range transport.
The results showed that Son La aerosol was simultaneously influenced by BB and transported dust in the front observation period to result in the dominance of carbonaceous content both in PM10-2.5 and PM2.5 as well as higher PM10-2.5 mass than PM2.5 from March 18 to 21, 2011. In contrast, the proportion of water-soluble ions was increased to dominate aerosol chemical speciation in the rear observation period from March 22 to 31, 2011, especially for the apparent change of SO42- over PM2.5 mass, which was due to the influence of BB coupling with the pollution transported from the southern China. The slight greater C3/C4 ratio (0.4) in rear than front (0.34) periods implies aerosol component is inclined to be more water-soluble and with greater degree of photochemical oxidation. The moderate high correlations (R2>0.5) for nss-K+ vs. levoglucosan and Char-EC/Soot-EC, respectively, validate the influence of BB activities during the observation period.
The enhancements of Mt. Lulin PM2.5 mass, total carbon, total ion, levoglucosan, and K+ were 4.1, 3.8, 3.1, 4.3, and 5.4 folds when under the influence of BB plume transport. This fact identifies aerosol BB tracers from transported airmasses. Ammonia deficient was found for Son La and Mt. Lulin aerosols under the influence of BB; however, aerosol was almost completely neutralized when Mt. Lulin was not affected by the transported BB plume. This indicates that BB plume aerosol tends to be acidic.
For Son La aerosol, PM2.5 copound form was Oxalic‧2H2O(s) when atmospheric relative humidity (RH) exceeded 60% in the front period and were (NH4)2SO4 and (NH4)3(H)(SO4)2 in the rear period. For comparison, the copound form of Mt. Luin PM2.5 was always (NH4)2SO4 regardless of the influences of BB. Different compound forms of aerosol exert deviations in the degradation of solar radiation and thus important in the assessment of environmental effect.
Aerosol water content is capable of representlin hygroscopic growth under high atmospheric RH and consequently plays an important role for evaluating solar radiation attenuation. This work compiled aerosol water content measured at Mt. Luin from 2008 to 2011. Linear regression analyses show that SO42- and WSOC-HULIS_C are chosen as significant predictors for BB and NBB periods in PM10, while NH4+ is considered as the important predictor for all time. The results imply aerosol water content is determined by speciation and concentration.

關鍵字(中)

★ 生質燃燒氣膠
★ 越南山羅氣膠
★ 生質燃燒氣膠長程傳輸
★ 氣膠結合型態
★ 氣膠含水量

關鍵字(英)

★ Biomass burning aerosol
★ Vietnam Son La aerosol
★ Long-range transported biomass burning aerosol
★ Aerosol compound form
★ Aerosol water content

論文目次

摘要..........i
Abstract..........ii
目錄..........iii
圖目錄..........v
表目錄..........viii
一、前言..........1
1.1研究緣起..........1
1.2研究目的..........2
二、文獻回顧..........3
2.1生質燃燒..........3
2.1.1亞洲生質燃燒..........3
2.1.2燃燒源指標..........5
2.2高山氣體與氣膠..........6
2.3越南氣膠特性..........7
2.5大氣氣膠含水特性..........10
2.5.1無機氣膠含水特性..........10
2.5.2有機氣膠含水特性..........11
2.5.3氣膠中和型態與氣膠含水特性..........12
2.6氣膠中和狀況與結合型態..........13
三、實驗方法..........14
3.1研究架構..........14
3.2採樣地點與採樣週期..........15
3.2.1越南山羅..........16
3.2.2鹿林山大氣背景監測站..........18
3.3採樣方法與採樣器..........21
3.3.1採樣儀器..........21
3.3.2儀器與濾紙配置..........24
3.4樣本分析方法..........27
3.4.1氣膠質量濃度分析..........27
3.4.2氣膠含水量分析..........28
3.4.3氣膠水溶性離子分析..........31
3.4.4氣膠碳成分分析..........34
3.4.5氣膠有機成分分析-單醣無水化合物..........36
3.4.6氣膠水可溶有機碳分析..........38
3.4.7似腐植質氣膠分析..........40
3.5氣膠中和探討-【NH4+】meas/【NH4+】calc 計算方式..........42
3.6判別生質燃燒發生的方法..........43
3.6.1美國太空總署(NASA)自然災害網..........43
3.6.2氣流軌跡模式(NOAA HYSPLIT) ..........43
3.6.3觀測期間逆推軌跡分類..........44
四、結果與討論..........48
4.1越南山羅當地氣膠特性..........48
4.1.1 PM10-2.5及PM2.5氣膠濃度質量..........48
4.1.2 PM10-2.5及PM2.5氣膠水溶性離子與揮發性離子濃度..........51
4.1.3氣膠碳成分濃度..........53
4.2鹿林山觀測期間氣膠特性..........59
4.2.1 PM10-2.5及PM2.5氣膠質量濃度..........59
4.2.2 PM10-2.5及PM2.5氣膠水溶性離子與PM2.5氣膠揮發性離子濃度..........61
4.2.3氣膠碳成分濃度..........64
4.3越南氣膠來源判斷..........72
4.4氣流來源類型與氣膠特性的差異..........77
4.4.1各觀測地點氣膠組成比例..........77
4.4.2氣流來源類型與氣膠特性的差異..........82
4.4.3氣膠中和狀況與結合型態..........91
4.5氣膠含水量..........101
4.5.1大氣氣膠含水量與化學成分..........101
4.5.2多元迴歸分析氣膠含水量..........109
4.5.3有機物質對氣膠含水量的影響..........115
五、結論與建議..........118
5.1結論..........118
5.2建議..........120
六、參考文獻..........121
附錄一、口試委員意見回覆..........129
附錄二、2011年密集觀測時期鹿林山氣流逆軌跡..........137
附錄三、2011年越南山羅密集觀測期間氣流逆軌跡..........141
附錄四、2011年越南山羅密集觀測期間CALIPSO衛星資料..........143

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指導教授

李崇德(Chung-Te Lee)

審核日期

2013-1-29

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