2019及2020年高山與都市環境氣膠化學及光學特性定稿

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許博鈞(XU-BO JUN) 查詢紙本館藏

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論文名稱

2019及2020年高山與都市環境氣膠化學及光學特性定稿

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摘要(中)

本文於2019年秋季(10月)在南投縣鹿林山(海拔2,862公尺)以及2020年春季(3至5月)在鹿林山和台中市中山醫學大學(海拔50公尺)分別採集氣動直徑為1.0 μm、2.5 μm、10 μm (PM1、PM2.5、PM10)大氣氣膠，並解析氣膠化學成分和光學特性。
2019年鹿林山秋季PM2.5和 PM10質量濃度分別為 7 ± 3 和9 ± 3 μg m-3，2020年春季PM1、PM2.5和 PM10質量濃度則分別為 18 ± 9、21 ± 10、24 ± 11 μg m-3，兩季氣膠粒徑分布都偏向由細粒徑主導。春季氣流軌跡分類以生質燃燒類型(BB)發生頻率最高，PM2.5 總碳成分與K+的線性相關性高(R2 =0.93; n=25, p < 0.01)，顯示受到生質燃燒傳輸影響；弱生質燃燒人為排放類型(WBB-AN)的SO42-濃度比秋季自由大氣類型(F-FT)高0.8 μg m-3，可視為境外傳輸人為排放增多的貢獻量。分析2003-2020年觀測數據，春季最高PM2.5濃度出現在2004年，BB類型的人為排放影響有逐年上升趨勢。
中山醫PM1、PM2.5、PM10的質量濃度分別為23 ± 9、31 ± 11、47 ± 16 μg m-3，中山醫細粒徑顆粒也是主導氣膠質量濃度，但不及鹿林山顯著。中山醫PM2.5低濃度(CSMU-LC)主要污染源是工業活動，工業活動貢獻量隨粒徑變小(PM1)而增加；相對地，交通活動是中山醫高濃度(CSMU-HC) PM2.5主要污染源，交通活動貢獻隨粒徑變大(PM10)而增加，高濃度的形成主要受擴散不佳及發生光化學反應影響。
以Revised IMPROVE方程式估算鹿林山及中山醫氣膠化學成分貢獻的大氣消光係數(bext)與儀器測量結果相關性都很好(R2 =0.84, n=20, p < 0.01; R2 =0.80, n=17, p<0.01)，顯示氣膠化學成分與bext有密切關係。鹿林山秋季bext由硫酸銨(AS)和空氣分子(RS)共同主導，春季則由有機物(OM)主導。中山醫bext主要由AS和硝酸銨(AN)貢獻，CSMU-HC bext高於CSMU-LC主要原因為AN占比提升。吸收光徑370 nm和880 nm黑碳濃度差異提供另類方法推測受生質燃燒影響，所推估出鹿林山受到較強烈生質燃燒日期，與氣流軌跡分類日期相近。鹿林山氣膠光學厚度(AOD)受PM2.5中AS及元素碳影響較大，且鹿林山高AOD採樣日通常伴隨較細的粒徑分布。
綜合而言，歷年數據分析顯示春季最高PM2.5濃度出現在2004年，2020年春季鹿林山仍受到東南亞生質燃燒傳輸影響，秋季bext由AS和RS共同主導，春季則由OM主導。中山醫採樣期間bext主要由AS和AN貢獻，CSMU-LC受工業源影響大，CSMU-HC則是受交通源、擴散不佳、光化學反應影響。

摘要(英)

This study collected PM1, PM2.5, and PM10 (particulate matter with an aerodynamic less than or equal to 1, 2.5, and 10 μm) in fall (October) of 2019 and spring (March to May) of 2020 at Mt. Lulin (2862 m above sea level). PM1, PM2.5, and PM10 were also collected at Chung Shan Medical University (CSMU) (50 m a.s.l.) in the spring of 2020. The chemical composition was resolved, and optical properties were computed from the collected PM.
The mass concentrations of PM2.5 and PM10 at Mt. Lulin in fall of 2019 were 7 ± 3 and 9 ± 3 μg m-3, respectively, and the mass concentrations of PM1, PM2.5, and PM10 in spring of 2020 were 18 ± 9, 21 ± 10, and 24 ± 11 μg m-3, respectively. Fine PM both dominated the particle size distribution of the two seasons. In spring, the biomass burning (BB) type occurred highest in the airmass trajectory classification. High linear correlation (R2 =0.93; n=25, p <0.01) between the total carbon content and K+ of PM2.5 indicated the influence of transported BB smoke. In contrast, the SO42- concentration of the weak BB anthropogenic type (WBB-AN) was 0.8 μg m-3 more than that of the free troposphere type (F-FT) in fall, which could be counted as an additional contribution from anthropogenic emissions by transboundary transport. The highest spring PM2.5 concentration appeared in 2004, and the impact from anthropogenic emissions of BB type had an upward trend year by year from 2003 to 2020.
The mass concentrations of PM1, PM2.5, and PM10 at CSMU were 23 ± 9, 31 ± 11, and 47 ± 16 μg m-3, respectively. The fine particle size at CSMU also dominated the aerosol mass concentration but was not as significant as that of Mt. Lulin. The main PM2.5 pollution source of CSMU-LC was industrial activity, which contributed more with reduced particle size (PM1). In contrast, traffic activity was the primary pollution source of CSMU-HC, and the contribution of traffic activity increased as the particle size became larger (PM10). The formation of high concentration events was influenced by poor ventilation and photochemical reactions.
The atmospheric extinction coefficient (bext) contributed by the aerosol chemical components, estimated by using the Revised IMPROVE equation, correlated well (R2 = 0.84, n = 20, p <0.01; R2 = 0.80, n = 17, p <0.01) with measurements both at Mt. Lulin and CSMU. The results indicate that aerosol chemical composition is closely related to bext. The bext was jointly dominated by ammonium sulfate (AS) and Rayleigh scattering (RS) at Mt. Lulin in fall, while it was led by organic matter (OM) in spring. The bext at CSMU was mainly contributed by AS and ammonium nitrate (AN). The higher value of bext at CSMU-HC than that of CSMU-LC is because of the greater proportion of AN. The difference in black carbon concentrations between 370 and 880 nm provided an alternative method for inferring dates influenced by intense BB because the dates were similar to those of the air trajectory classification method. The aerosol optical depth (AOD) at Mt. Lulin was greatly affected by the AS and elemental carbon (EC) in PM2.5, and finer particle size spectra usually accompanied high AOD sampling days.
In summary, the highest PM2.5 concentration at the Mt. Lulin site in spring occurred in 2004 from historical data. Mt. Lulin is still under the influence of the transported BB from Southeast Asia in spring 2020. The bext was dominated by AS and RS in fall and OM in spring in 2020. During the CSMU sampling period, the bext was primarily contributed by AS and AN with industrial activity as the main pollution source of CSMU-LC in contrast to traffic activity at CSMU-HC plus poor ventilation and photochemical reactions.

關鍵字(中)

★ 鹿林山測站
★ 生質燃燒
★ 長程傳輸
★ 都市氣膠
★ 氣膠化學與光學

關鍵字(英)

★ Mt. Lulin
★ biomass burning
★ long-range transport
★ urban aerosol
★ aerosol chemistry and optical properties

論文目次

摘要 I
Abostract III
致謝 V
目錄 VI
圖目錄 X
表目錄 XIV
第一章前言 1
1.1 研究緣起 1
1.2 研究目的 3
第二章文獻回顧 4
2.1鹿林山相關研究 4
2.2都市氣膠特性 6
2.3生質燃燒說明 8
2.4氣膠碳成分說明 11
2.5氣膠水溶性無機離子說明 16
2.6化學成分粒徑分布說明 19
2.7氣膠光學特性 20
第三章研究方法 23
3.1 研究流程與步驟 23
3.2 採樣地點與採樣週期 24
3.3採樣儀器 27
3.4儀器與濾紙 29
3.4.1濾紙前處理 29
3.4.2樣本運送與保存 30
3.5樣本分析方法 30
3.5.1 質量濃度分析 30
3.5.2氣膠碳成分分析 32
3.5.3 水溶性無機離子分析 36
3.5.4 氣膠微粒揮發成分補償校正 39
3.6氣膠水溶性離子非海洋來源 42
3.7 NOAA 氣膠觀測系統 42
3.7.1 積分式散光儀 (TSI Model 3563 Integrating Nephelometer) 43
3.7.2 微粒碳吸收光度計 (PSAP) 46
3.7.3 黑碳儀(Aethalometer AE-31, Magee Scientific) 50
3.7.4 長光徑能見度透射儀(Long path visibility transmissometer) 54
3.8 環保署測站其他自動監測儀器 56
3.9 判別生質燃燒發生的方法 56
3.9.1 美國太空總署 (NASA) 自然災害網 57
3.9.2 美國太空總署全球火災監測中心 58
3.9.3 氣流軌跡模式 (NOAA HYSPLIT) 58
3.10 光學計算方法 59
3.10.1 Revised IMPROVE 公式計算消光係數 59
3.10.2 Ångström exponent(AE) 62
第四章結果與討論 63
4.1鹿林山氣流軌跡分類依據 63
4.2 2020年鹿林山氣膠特性分析 67
4.2.1秋季與春季PM2.5氣膠碳成分解析 69
4.2.2秋季與春季PM2.5氣膠水溶性無機離子解析 72
4.2.3鹿林山PM2.5碳成分生質燃燒貢獻OC及EC探討 75
4.2.4鹿林山歷年化學成分變化討論 77
4.3 2020都市春季氣膠化學成分特性分析 82
4.3.1高濃度判斷事件成因與組成變化探討 84
4.3.2都市PM2.5氣膠碳成分及都市與高山測站碳成分差異 90
4.3.3都市PM2.5水溶性無機離子及都市與高山測站水溶性無機離子差異 93
4.3.4高山與都市春季衍生碳污染物濃度與占比差異 96
4.4高山與都市氣膠不同粒徑區間化學成分占比與特性探討 99
4.4.1鹿林山春季BB氣流軌跡類型PM1、PM1-2.5、PM2.5-10化學成分探討 99
4.4.2中山醫PM1、PM1-2.5、PM2.5-10化學成分分布與高山、都市差異探討 103
4.4.3鹿林山春季PM1、PM1-2.5、PM2.5-10各成分相關性與SO42-來源 107
4.4.4高山與都市環境各粒徑污染源特徵比探討 109
4.5氣膠化學成分與大氣光學關係 111
4.5.1鹿林山秋季與春季量測吸光與散光係數變化探討 111
4.5.2 鹿林山氣膠化學成分與大氣消光係數關係 114
4.5.3高山與都市環境氣膠消光與化學成分貢獻差異探討 118
4.5.4黑碳和元素碳差異性與黑碳判斷生質燃燒影響方法探討 122
4.5.5氣膠光學厚度(AOD)與鹿林山化學成分關係 125
第五章結論與建議 129
5.1結論 129
5.2建議 132
參考文獻 133
附錄一秋季採樣期間氣流軌跡圖 151
附錄二春季採樣期間氣流軌跡圖 158
附錄三春季採樣期間火點圖 178
附錄四鹿林山2003年至2020年成分變化趨勢 180
附錄五鹿林山相關化學成分相關性矩陣 181
附錄六採樣期間每日分析成分及註備事項 184
附錄七採樣期間平均化學成分濃度 187
附錄八口試委員意見回覆 190

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指導教授

李崇德(Chung-Te Lee)

審核日期

2021-9-29

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