2017~2018年台灣平地與高山氣膠水溶性無機離子短時間動態變化特性

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楊孟樵(Meng-Chiao Yang) 查詢紙本館藏

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論文名稱

2017~2018年台灣平地與高山氣膠水溶性無機離子短時間動態變化特性

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摘要(中)

大氣氣膠水溶性無機離子對大氣環境影響重大，這些無機離子特性在環境中變化迅速，需要進行短時間的觀測。本文於2017年11月在豐原高中、2018年3月至4月在鹿林山大氣背景觀測站、2018年4月及5月在中央大學，以半自動方法量測氣膠水溶性無機離子，大部分時間量測PM2.5，但在豐原高中和中央大學有些時段切換量測PM10水溶性無機離子。量測結果搭配測站相關監測數據，探討氣膠的化學、物理、光學特性、和污染來源。
2018年春季鹿林山測站主要有山谷風和生質燃燒事件，相較於非事件PM2.5質量濃度的10.2 ± 6.8 μg m-3，生質燃燒事件和山谷風事件的PM2.5質量濃度分別上升至21.8 ± 6.6和20.1 ± 1.3 μg m-3。PM2.5水溶性無機離子在非事件、生質燃燒事件、山谷風事件平均濃度別為4.9 ± 3.1 μg m-3、5.7 ± 2.0 μg m-3、9.9 ± 0.7 μg m-3，顯然污染事件帶來較多的PM2.5水溶性無機離子。在豐原高中和中央大學5月高濃度事件中，PM2.5質量濃度分別為23.7 ± 6.8和21.2 ± 2.6 μg m-3，在中央大學4月的PM10質量濃度事件則達80.6 ± 5.5 μg m-3，在中央大學和豐原高中量測期間PM2.5/PM10分別約為0.3至0.6以及0.2至0.4，顯示這兩個地方粗粒徑微粒在PM10占有較大比例。比較NO3-和SO42-在微粒中占比，在PM10中NO3-大於SO42-，但在PM2.5中卻是SO42-占比較大，表示在PM10中有很多的粗粒徑NO3-。在平地監測到的NO2-多在夜間生成，且與相對濕度以及NO2濃度有較大的相關性。鹿林山的PM2.5事件主要受到生質燃燒煙團長程傳輸以及人為傳輸污染影響，在中央大學以及豐原高中的高微粒濃度普遍受到海陸風影響，特別是在夜間常因風速和邊界較低而導致污染累積。
本文發現在低相對濕度、非靜風、無雲霧的環境條件下，鹿林山大氣氣膠化學特性和山頂以上的大氣氣膠光學厚度(Aerosol Optical Depth, AOD)相關性良好(R2=0.68，p< 0.05)；即使在平地地區，非靜風的環境下，大氣氣膠化學特性和整層大氣氣膠光學厚度也具有關聯性(R2=0.5，p< 0.05)。本文使用ISORROPIA Ⅱ 模式進行氣膠酸度模擬，顯示在高山主要為酸性氣膠而平地多為酸性或是中性氣膠，利用各離子莫耳濃度計算的相關性對高山或是平地氣膠水溶性無機離子結合型態做推估，顯示鹿林山在生質燃燒事件有較多的硫酸鉀、硝酸鉀，平地在微粒高濃度事件則以硝酸銨為主。

摘要(英)

Water-soluble inorganic ions (WSIIs) of atmospheric aerosol have a significant effect on the atmospheric environment. These inorganic ions need to observe with high time-resolution as they change their properties rapidly in the environment. This study measured PM2.5 WSIIs with the semi-automated method at the Fengyuan High School (FHS) in November 2017, Lulin Atmospheric Background Station (LABS) in March-April 2018, and at National Central University (NCU) in April-May 2018. The measurements were toward PM2.5 most of the time; however, for some time, the system switched to PM10 WSIIs. The results accompanying related monitoring data at the stations were suitable for investigating aerosol chemistry, physics, optical properties, and source contributions.
The averages of PM2.5 mass concentrations for the events of biomass burning (BB) and mountain-valley (M-V) wind were 21.8 ± 6.6 and 20.1 ± 1.3 μg m-3, respectively, in contrast to that of non-event PM2.5 mass concentration of 10.2 ± 6.8 μg m-3. Meanwhile, the averages of PM2.5 WSIIs at non-event period, BB, and M-V wind events were 4.9 ± 3.1 μg m-3, 5.7 ± 2.0 μg m-3, and 9.9 ± 0.7 μg m-3, respectively. Obviously, pollution events brought more PM2.5 WSIIs from the comparison. In high concentration events at the FHS and NCU (May), the averages of PM2.5 mass concentrations were 23.7 ± 6.8 and 21.2 ± 2.6 μg m-3, respectively. In contrast, the high concentration event at NCU (April) was as high as 80.6 ± 5.5 μg m-3 in PM10. The PM2.5/PM10 ratios were 0.3-0.6 and 0.2-0.4 at NCU and FHS, respectively. Evidently, coarse particles were more in PM10 at both sites. Comparing the fraction of NO3- and SO42- in particles, NO3- is higher than SO42- in PM10, but the reverse is true in PM2.5. It implies that a lot of coarse NO3- existing in PM10. For monitoring results in the ground level, NO2- observed to form during nighttime and correlated well with relative humidity (RH) and NO2 concentration. The PM2.5 events were under the influences of long-range transport of BB smoke and anthropogenic pollution transports at LABS. In contrast, the land-sea breeze was mainly responsible for high particulate concentrations at NCU and FHS, especially for pollution accumulation from low wind speed and shallow boundary layer at night.
As revealed from this study, low RH, non-calm wind, and non-fog environment provided a good correlation between aerosol chemical properties and aerosol optical depth (AOD) at the summit of LABS (R2=0.7, p< 0.05). Even in the ground level, aerosol chemical properties and AOD correlated moderately with each other under a non-calm wind environment (R2=0.5, p< 0.05). The application of the ISORROPIA II model for aerosol acidity simulation indicated that mountain aerosol was acidic, and the aerosol in the ground level was more toward acidic or neutral. The computations of molar concentrations of the correlated WSIIs to infer aerosol compound form resulting in more potassium sulfate and potassium nitrate in BB events at LABS and ammonium nitrate in high particulate events in the plain area

關鍵字(中)

★ 氣膠水溶性無機離子短時間變化
★ 生質燃燒煙團
★ 山谷風
★ 氣膠光學厚度
★ PM2.5，NO2-與NO2

關鍵字(英)

★ High time-resolved water-soluble inorganic ions
★ biomass burning smoke
★ mountain-valley wind
★ Aerosol optical depth
★ PM2.5 NO2- and NO2.

論文目次

摘要 I
Abstract III
致謝 V
目錄 VI
圖目錄 IX
表目錄 XX
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 生質燃燒 4
2.1.1 生質燃燒氣膠長程傳輸 4
2.1.2 生質燃燒氣膠化學成分特性 5
2.1.3 生質燃燒氣膠粒徑變化 6
2.1.4 生質燃燒氣膠光學特性 7
2.2 氣膠光學厚度(Aerosol Optical Depth, AOD) 7
2.3 氣膠水溶性無機離子 8
2.3.1 氣膠中和狀況與結合型態 9
2.4 高山地區氣膠與氣體 11
2.4.1 雲霧動態變化 12
2.4.2 山谷風循環 14
2.5平地地區氣膠與氣體 15
2.5.1 NO2-離子形成條件 16
2.5.2 PM10 與PM2.5水溶性離子 18
2.6 氣膠水溶性離子連續監測儀器 19
2.6.1 即時氣膠水溶性離子監測儀器 20
2.7 模擬氣膠含水量與pH值 22
2.7.1 氣膠pH值 22
2.7.2 氣膠含水量模擬 24
第三章研究方法 27
3. 1研究架構 27
3.2 監測地點與監測週期 28
3.3 監測設備與方法 29
3.3.1 短時間氣膠水溶性無機離子監測 30
3.3.2 品保品管方法以及MDL的作法 33
3.4 大氣氣膠連續監測系統 34
3.4.1 自動監測儀器 34
3.4.2 NOAA氣膠觀測系統 36
3.4.3 積分式散光儀(Integrating Nephelometer) 37
3.4.4 微粒碳吸收光度計(PSAP) 40
3.4.5 粒徑分布監測系統 44
3.4.6 PWD22即時天氣探測儀 47
3.4.7 其他連續監測儀器 49
3.5 氣流軌跡模式(NOAA HYSPLIT) 51
3.6 ISORROPIAⅡ 模式分析 53
第四章結果與討論 54
4.1 鹿林山氣膠水溶性無機離子短時間變化 54
4.1.1 短時間自動監測與手動監測水溶性無機離子比對 55
4.1.2 春季鹿林山氣象資料、氣體、水溶性無機離子動態變化 56
4.1.3 雲霧、山谷風及生質燃燒事件辨識方法 60
4.1.4 鹿林山氣膠水溶性離子不同軌跡來源短時間變化 61
4.2 鹿林山春季生質燃燒及山谷風事件氣膠、氣體及氣象參數動態變化 63
4.2.1 生質燃燒事件(3月16日至3月20日) 63
4.2.2 春季中國傳輸及山谷風事件(3月25日、27日、28日、29日) 78
4.3 平地氣膠水溶性無機離子短時間變化 94
4.3.1 平地地區監測氣象資料、氣體、氣膠水溶性無機離子動態變化 95
4.3.2 中央大學與豐原高中測站不同軌跡來源短時間變化 101
4.4 中央大學與豐原高中測站高濃度氣膠、氣體及氣象參數動態 103
4.4.1 豐原高濃度事件 103
4.4.2 四月高濃度事件 120
4.4.3 五月高濃度事件 161
4.5 平地地區NO2-離子形成與變化 192
4.5.1 中央大學與豐原高中測站NO2-離子短時間變化 192
4.5.2 平地地區中NH4NO2結合型態 197
4.5.3 NO2-離子與NO2氣體異質反應關係 203
4.6 探討高山與平地短時間氣膠化學成分與氣膠光學厚度關係 206
4.6.1鹿林山短時間氣膠化學成分與AOD關係 206
4.6.2平地短時間氣膠化學成分與AOD關係 210
4.7 平地與高山地區高濃度事件發生的原因和污染途徑或來源 217
第五章結論與建議 225
5.1 結論 225
5.2 建議 228
第六章參考文獻 229
附錄一、2018年春季鹿林山觀測間逆推軌跡圖 238
附錄二、2018年春季鹿林山觀測期間火點圖 245
附錄三、2018年中央大學測站4月PM10觀測期間逆推軌跡圖 249
附錄四、2018年中央大學測站5月PM2.5觀測期間逆推軌跡圖 252
附錄五、2017年豐原高中測站11月觀測期間逆推軌跡圖 255
附錄六、口試委員意見與回覆 258

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指導教授

李崇德

審核日期

2020-3-9

推文