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研究生:姜明辰
研究生(外文):Ming-Chen Jiang
論文名稱:2015年春季鹿林山氣膠水溶性無機離子短時間動態變化特性
指導教授:李崇德李崇德引用關係
指導教授(外文):Chung-te Lee
學位類別:碩士
校院名稱:國立中央大學
系所名稱:環境工程研究所
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2016
畢業學年度:104
語文別:中文
論文頁數:285
中文關鍵詞:氣膠水溶性無機離子短時間動態變化傳輸生質燃燒煙團雲霧事件氣膠特性PILS-IC
外文關鍵詞:Short-term dynamic variations of aerosol water-soluble inorganic ionstransported biomass burning smokeaerosol properties in fog eventsPILS-IC
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本文於2015年春季在鹿林山大氣背景觀測站(以下簡稱鹿林山,海拔高度2,862 m)以即時氣膠水溶性離子監測系統(Particle-Into-Liquid-Sampler coupled to an Ion Chromatograph, PILS-IC)監測PM2.5水溶性離子,並結合測站內即時監測儀器監測的PM2.5、PM10大氣質量濃度、PM1、PM10光學吸光及散光係數、氣體污染物濃度、氣膠數目濃度與粒徑分布動態變化等資料進行討論。
在不受生質燃燒、谷風、雲霧事件影響時段,PM2.5大氣質量濃度平均為3.2±0.3 μg m-3,PM2.5水溶性無機離子以陰離子為主,其中SO42-濃度最高,平均為0.7±0.1 μg m-3;陽離子濃度較低,且環境中常呈現NH4+不足以完全中和SO42-和NO3-現象。鹿林山午後易受谷風影響,谷風影響期間CO、O3、RH、PM10、PM2.5數值會上升。三次雲霧事件都發生在午後,CO、O3、PM2.5濃度分別為0.13±0.04 ppm、48.3±9.4 ppbv、16.5±4.1 μg m-3,SO42-、NH4+、NO3-平均濃度分別為3.6±0.8、2.2±1.1、1.5±0.8 μg m-3,顯示受到谷風影響的污染物濃度。計算雲霧期間與大氣SO2平衡而溶解於霧珠的SO42-和PILS-IC量測的SO42-比值(Dissolved Gas over Measured Ions, DIGMI),發現在“雲霧發生”前段DIGMI略大於1情況較多,“雲霧發生”期間和以後則DIGMI數值小於1,代表雲霧事件大多受谷風傳輸帶來SO42-,變低DIGMI數值。
鹿林山四次生質燃燒事件(含谷風及雲霧事件)中, CO、O3、PM2.5和K+平均濃度分別為0.26±0.3 ppm、74.2±7.9 ppbv、28.8±6.7 μg m-3、0.6±0.1 μg m-3,SO42-、NH4+、NO3-濃度分別為4.1±0.8、3.0±1.0、1.9±0.4 μg m-3;生質燃燒期間,大氣環境長時間出現過剩NH4+ (ExNH4+),代表足以中和SO42-,推測環境中SO42-結合型態為(NH4)2SO4和(NH4)2SO4。受生質燃燒影響期間出現雲霧時,觀測較多情況DIGMI數值小於1,平均數值為0.71±0.16,代表環境中傳輸氣膠SO42-濃度大於SO2轉化成SO42-濃度。
以不受生質燃燒、谷風、雲霧影響時段的NH4+、K+、NO3-、SO42-濃度為基本案例,比較他時段前述成分濃度差異百分比,當不受生質燃燒影響但受谷風影響時段分別增加98.7%、57.4%、88.8%、40.8%,不受生質燃燒影響但受雲霧影響時段分別增加100.0%、83.6%、98.6%、68.8%。單純受生質燃燒影響時段NH4+、K+、NO3-、SO42-濃度增加100.0%、96.6%、98.8%、69.2%,受生質燃燒影響且發生谷風前述離子濃度增加100.0%、96.6%、98.8%、77.0%,最後,受生質燃燒影響且發生雲霧濃度前述離子濃度各增加100.0%、96.1%、99.1%、74.6%。

In this study, PM2.5 water-soluble inorganic ions (WSIIs) were monitored using an in-situ Particle-Into-Liquid-Sampler coupled to an Ion Chromatograph (PILS-IC) system at Lulin Atmospheric Background Station (LABS, 2,862 m a.s.l.) in spring 2015. Meanwhile, PM2.5 and PM10 mass concentrations, PM1 and PM10 light-scattering and -absorption coefficients, trace gas concentrations, and dynamic variations of aerosol number concentrations and size spectra monitored at LABS were also adopted for discussion.
PM2.5 mass concentraions were averaged at 3.2±0.3 μg m-3 during the period without been affected by the transported biosmass burning (BB) smoke, upslope wind, and fog event. Among PM2.5 chemical components, anion dominated WSIIs with SO42- averaged at 0.7±0.1 μg m-3 as the predominant component in contrast to relative low concentration of cation with NH4+ incapable of complete neutralizing SO42- and NO3-. Meanwhile, LABS was frequently affected by the upslope wind accompanying with the rises of CO, O3, RH, PM10, and PM2.5. Three cloud events happened in the afternoon to result in the rises of pollutant levels by having the mean values of CO, O3, and PM2.5 at 0.13±0.04 ppm, 48.3±9.4 ppbv, and 16.5±4.1 μg m-3, respectively, and that of SO42-, NH4+, and NO3- at 3.6±0.8, 2.2±1.1, and 1.5±0.8 μg m-3, respectively. The values of Dissolved Gas over Measured Ions (DIGMI) were calculated by dividing the dissolved SO42- concentrations in fog droplets in equilibrium with atmospheric SO2 over SO42- measured by PILS-IC. The DIGMI values were frequently greater than 1 before the occurrence of a cloud event in contrast to less than 1 during and after a cloud event. It indicated that SO42- was transported by the upslope wind from the hill to reduce the DIGMI values in the cloud events.
Durning the four BB events (including upslope and cloud events), mean levels of CO, O3, PM2.5, K+, SO42-, NH4+, and NO3- were 0.26±0.3 ppm, 74.2±7.9 ppbv, 28.8±6.7 μg m-3, 0.6±0.1 μg m-3, 4.1±0.8 μg m-3、3.0±1.0 μg m-3、1.9±0.4 μg m-3, respectively. In most occasions, excess NH4+ (ExNH4+) was found enough to complete neutralizing SO42- to form (NH4)2SO4 and (NH4)2SO4. The DIGMI values were often less than 1 with a mean value of 0.71±0.16 during the fog peroid when influenced by the transported BB smoke. This implied that SO42- in the transported smoke was more than that of the dissolved SO2 in the fog droplets.
Take mean values of NH4+, K+, NO3-, and SO42- during the time period not affected by the transported BB smoke, upslope wind, and fog events as the base case for comparing with that of the other time periods in terms of percentage differences are shown as follows. For the period not affected by the transported BB smoke but under the influence of the upslope wind, the differences for NH4+, K+, NO3-, and SO42- were 98.7%, 57.4%, 88.8%, and 40.8%, respectively. Similarly, the differences for the period not affected by the transported BB smoke but under the influence of fog events were 100.0%, 83.6%, 98.6%, and 68.8%, respectively. Moreover, the differences of NH4+, K+, NO3-, and SO42- for the period affected purely by the transported BB smoke were 100.0%, 96.6%, 98.8%, and 69.2%, respectively. In the case for the period affected by the transported BB smoke and upslope wind, the differences of the aforementioned WSIIs were 100.0%, 96.6%, 98.8%, and 77.0%, respectively. Finally, the differences of the precedent WSIIs were 100.0%, 96.1%, 99.1%, and 74.6%, respectively, for the period affected by the transported BB smoke and fog events.

摘要 I
Abstract III
致謝 V
目錄 VI
圖目錄 VIII
表目錄 XXIII
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氣膠水溶性無機離子監測儀器 3
2.1.1 濕式前驅氣體分離器 3
2.1.2 即時氣膠水溶性監測儀器 3
2.2 生質燃燒 7
2.2.1 生質燃燒氣體和水溶性無機離子特性 7
2.2.2 生質燃燒氣膠光學特性 8
2.2.3 生質燃燒氣膠傳輸 9
2.3 氣膠水溶性無機離子 11
2.3.1 氣膠中和狀況與結合型態 12
2.4 高山地區氣體與氣膠 13
2.4.1 雲霧氣膠特性 15
2.4.2 溶解 16
第三章 研究方法 17
3.1 研究架構 17
3.2採樣地點與採樣週期 19
3.3採樣設備與方法 21
3.3.1手動採樣器 21
3.3.2採樣濾紙前處理與設置 22
3.3.3微粒揮發NO3-、NH4+、Cl-補償方法 25
3.4 大氣氣膠連續監測系統 27
3.4.1 自動監測儀器 27
3.4.2 即時氣膠水溶性無機離子層析儀 28
3.4.3 NOAA氣膠監測系統 31
3.4.4 積分式散光儀(Integrating Nephelometer) 32
3.4.5 微粒碳吸收光度計(PSAP) 34
3.4.6 粒徑分布監測系統 37
3.4.7 其他連續監測儀器 39
3.5 鹿林山不同氣團來源判別分類與逆推軌跡方法 41
3.6 雲霧中可溶性氣體溶解情況 43
第四章 結果與討論 46
4.1 氣膠水溶性無機離子手動與自動量測比對 46
4.1.1水溶性無機離子非揮發成分手動採樣與自動量測比對 46
4.1.2水溶性無機離子揮發修正手動採樣與自動量測比對 47
4.1.3 水溶性離子濃度手動濾紙揮發修正與自動量測線性關係彙整 51
4.2觀測期間氣膠水溶性無機離子動態變化 52
4.2.1氣體、氣象參數和水溶性無機離子濃度動態變化 55
4.3不受生質燃燒煙團傳輸影響氣膠水溶性離子動態變化 59
4.3.1 不受生質燃燒影響氣膠水溶性無機離子動態變化 59
4.3.2 不受生質燃燒傳輸影響時間氣膠動態變化討論 87
4.3.3 不受生質燃燒影響時間內雲霧事件氣膠動態變化 91
4.3.4 不受生質燃燒影響時間內雲霧事件氣膠動態變化彙整 125
4.4 鹿林山受生質燃燒煙團傳輸影響氣膠動態變化 135
4.4.1 生質燃燒事件 135
4.4.2 彙整鹿林山生質燃燒事件氣體資料與氣膠動態特性 196
4.5 探討鹿林山受雲霧和受生質燃燒煙團影響無機水溶性離子比值差異 204
第五章 結論與建議 211
5.1 結論 211
5.2 建議 214
第六章 參考文獻 215
附錄一、2015年3月1日至4月14日鹿林山觀測期間逆推軌跡圖 226
附錄二、2015年3月1日至4月15日鹿林山觀測期間火點圖 238
附錄三、 口試委員意見與答覆 246


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