低分子量二元有機酸氣膠分析方法及
含水特性之研究

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許惠敏(Hui-Min Hsu) 查詢紙本館藏

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環境工程研究所

論文名稱

低分子量二元有機酸氣膠分析方法及含水特性之研究
(Analysis Method and hygroscopicity of Low Molecular Weight Dicarboxylic acids on Aerosols )

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摘要(中)

在許多探討大氣基本物理特性、輻射作用、雲霧形成機制、區域性能見度、全球氣候變遷、氣膠化學組成與人體健康風險評估等研究中，發現大氣氣膠的含水量皆佔有不可忽略的影響程度。氣膠含水量在大氣氣膠的物理與化學特性研究領域中佔有相當重要的地位。近年來已有許多學者對無機氣膠的吸濕成長進行相當多研究，但在有機氣膠方面則是剛剛起步，再加上有機物質對於氣膠吸濕特性又有許多不確定的影響，所以在有機氣膠的吸濕特性方面仍需更多的研究及數據來說明其對氣膠含水量的影響。
本研究主要是以GC-TCD氣膠含水量分析儀（Lee and Chang, 2002; Chang and Lee, 2002）量測收集在濾紙上大氣常見有機四種二元酸（Oxalic acid、Succinic acid、Malonic acid及Glutaric acid）的含水量，且將量測的數據與文獻量測單顆粒氣膠含水量相比較。此外，亦藉由GC/MS分析技術，分析大氣中常見的有機二元酸的成分與含量。
就有機酸成分分析結果顯示：以新莊超級測站這個採樣點來說，大氣氣膠中有機酸的平均濃度：Oxalic acid=167±36ng/M3、Malonic acid=15±4ng/M3、Succinic acid=14±4ng/M3、Glutaric acid=4±1ng/M3，總二元有機酸佔質量濃度的百分比為0.56%±0.13%，佔總碳濃度的4.60%±1.23%，佔有機碳濃度的7.55%±1.84%。
就GC-TCD量測有機氣膠含水量來說：GC-TCD法顯示Oxalic acid及Succinic acid氣膠並無DRH與CRH，其AMC分別為1.26及1.00；Malonic acid氣膠DRH=70-75%，在潮解點相對濕度後，氣膠仍會隨著相對濕度再升高持續吸水；無CRH；Glutaric acid氣膠的DRH＝90％。
就溫度對有機氣膠含水量的影響來說：在增濕過程中，當溫度越高時，氣膠大量吸水點會發生在較低的相對濕度環境下；而在降濕過程中，氣膠的含水量在同一相對濕度環境下，卻會隨溫度增加而增加。

摘要(英)

Water content of atmospheric aerosols is related to atmospheric radiation, cloud and mist formation, visibility, local climate change, chemical and physical properties of aerosols, and human health assessment. As the results, the measurements of water content of aerosols become increasingly important in aerosol science research. Resently, many scholars have invested the hygroscopic characteristic of inorganic aerosols. However, few researches focused on similar topics of the organic aerosols. Because the hygroscopicity of organic aerosols is uncertain for now, it needs more scientific datas to realize the relationship between atmospheric moisture and hygroscopicity of organic aerosols related to water content within them.
In this research, a thermal conductivity detector (GC-TCD, Lee and Chang, 2002; Chang and Lee, 2002) was used to measure water content of four organic acids (Oxalic acid, Succinic acid, Malonic acid and Glutaric acid). The results of oxalic acid and succinic acid showed no DRH(Deliquescence Relative Humidity) and CRH(Crystallization Relative Humidity). AMC(Aerosol Mass Change) of oxalic acid and succinic acid indicated 1.26 and 1.00, respectively. The DRH of Malonic acid is at 70-75%. Water content of malonic acid increased with increasing relative humidity above DRH. However, malonic acid shows that CRH doesn’t exist. Glutaric acid reveals its DRH at 90%.
Applying GC/MS, the quantities of dicarboxylic acids were measured in associated with atmospheric aerosols. Air-borne particulate samples at Hsin-Chuang supersite from 19th September to 28th September. The average concentrations of oxalic acid, malonic acid, succnic acid and glutaric acid were 167±36 ng/M3, 15±4 ng/M3, 14±4 ng/M3, 4±1 ng/M3, respectively. The average percentage to four dicarboxylic acids was about 0.56%±0.13%. That total dicarboxylic acid mass concentration occupied 4.60%±1.23% and 7.55%±1.84% of total carbon and organic carbon concentrations.
The sensitivity of water content of organic aerosols was also influenced by temperature. During the experiments of increasing humidity, DRH of organic aerosols occurred at lower RH for higher temperatures. Contrastly, water content of organic aerosols increased with increasing temperature under the same humidity during the process of decreasing humidity.

關鍵字(中)

★ 二元酸
★ 潮解點相對濕度
★ 再結晶點相對濕度

關鍵字(英)

★ dicarboxylic acid
★ DRH
★ CRH

論文目次

目錄
表目錄 V
圖目錄 VI
第一章前言 1
1.1研究動機 1
1.2研究目的 3
第二章文獻回顧 4
2.1氣膠含水特性 4
2.2氣膠含水特性對環境之衝擊 4
2.2.1氣膠質量濃度量測 4
2.2.2 酸性沉降 5
2.2.3 氣膠光學性質 6
2.2.4 氣候變遷 8
2.2.5 人體健康 10
2.3影響氣膠含水特性的因子 12
2.3.1 溫度 12
2.3.2 大氣濕度 14
2.3.3 氣膠物種組成 15
2.3.4 氣膠混合方式 16
2.3.5 氣膠亞穩定特性（Metastability） 17
2.4氣膠含水特性的量測方法與研究成果 19
2.4.1目前所採用的氣膠含水特性量測方法 19
2.4.2有機純氣膠含水特性的量測方法 19
2.5大氣常見的有機氣膠 24
2.5.1大氣有機氣膠種類與含量 24
2.5.2大氣中有機酸的來源與特性 29
2.5.3大氣中常見有機酸的含水特性 32
第三章研究方法 37
3.1 有機氣膠吸濕特性研究架構 37
3.2 GC-TCD氣膠含水量量測系統 37
3.2.1量測原理 38
3.2.2 GC-TCD氣膠含水量量測系統 41
3.2.3量測步驟 45
3.2.4偵測極限 46
3.2.5萃取時間與調理時間 47
3.3大氣氣膠的組成分析 48
3.3.1 量測規劃與步驟 49
3.3.2大氣氣膠採樣設備 52
3.3.3採樣濾紙的前處理 55
3.3.4質量濃度分析方法 55
3.3.5碳成份分析方法 55
3.3.6水溶性離子分析方法 57
3.3.7二元有機酸的分析方法 57
3.3.7.1樣本萃取方法（分析water soluble dicarboxylic acids） 57
3.3.7.2分析儀器設備及分析條件的設定 58
第四章結果與討論 61
4.1有機二元酸氣膠分析方法的探討 61
4.1.1有機二元酸的定性與檢量線的製作 61
4.1.2有機二元酸的萃取方法的探討 66
4.1.2.1 Hexane的萃取效率 66
4.1.2.2高濃度樣本全程分析程序測試 68
4.1.2.3大氣氣膠樣本全程分析程序測試 71
4.1.3大氣氣膠中二元有機酸的含量 74
4.1.3.1採樣地點 74
4.1.3.2大氣中二元有機酸的含量分析 75
4.2純有機氣膠含水特性 77
4.2.1 Oxalic acid氣膠含水特性 78
4.2.2 Malonic acid氣膠含水特性 80
4.2.3 Succinic acid氣膠含水特性 82
4.2.4 Glutaric acid氣膠含水特性 83
4.2.5 四種低分子量二元有機酸氣膠吸水能力之比較 84
4.3溫度對於有機氣膠含水量的影響 86
4.3.1溫度對Malonic acid氣膠含水特性的影響 86
4.3.2溫度對Succinic acid氣膠含水特性的影響 87
4.3.3溫度對Glutaric acid氣膠含水特性的影響 88
第五章結論與建議 90
5.1結論 90
5.2建議 91
第六章參考文獻 92
表目錄
表2.1. 以多元迴歸法展現相關研究結果的係數（張士昱，2002） 18
表2.2 文獻中有關氣膠含水量量測方法彙整表 22
表2.2 文獻中有關氣膠含水量量測方法彙整表（續） 23
表2.3 Rogge et al.（1993b）洛杉磯都市地區微粒中有機物種佔碳質量濃度的百分比結果 25
表2.4大氣氣膠中脂肪族二元羧酸含量彙整表 26
表2.4大氣氣膠中脂肪族二元羧酸含量彙整（續） 27
表2.4大氣氣膠中脂肪族二元羧酸含量彙整（續） 28
表2.5 大氣中常見二元酸含水特性一覽表（Peng et al., 2001） 33
表2.6二元酸鹽類含水特性一覽表（Chan et al., 2001） 35
表3.1GC/MS操作條件設定列表 60
表4.1 有機二元酸丁酯化標準品滯留時間彙整表 63
表4.2 有機二元酸丁酯化標準品SIM的設定參數 66
表4.3 有機二元酸丁酯化標準品檢量線範圍與RRF值 66
表4.4 Hexane萃取效率穩定性一覽表 68
表4.5使用15cm無水硫酸鈉管柱除水後，樣本全程萃取分析回收率 71
表4.6模擬大氣氣膠有機酸含量較低之樣本全程萃取分析回收率 72
表4.7大氣樣本分析總表 76
表4.8四種低分子量二元有機酸氣膠吸水特性彙整表 85
圖目錄
圖2.1 dicarboxylic acids、ketocarboxylic acids、α-dicarbonyls化學結構式（Kawamura et al., 1995） 31
圖2.2大氣中二元酸的來源與變化途徑（Kawamura et al., 1995） 32
圖3.1 研究架構圖 37
圖3.2 GC-TCD氣膠含水量量測系統設備（Lee and Chang, 2002）…42
圖3.3 氣膠再懸浮系統 44
圖3.4 有機氣膠含水量的量測步驟 45
圖3.5 大氣氣膠採樣及成分量測步驟 50
圖3.6 採樣時的濾紙配置 51
圖3.7 R＆P Model 2300採樣器的設備圖 54
圖3.8 PM2.5蜂巢式套管採樣器的構造 54
圖4.1 GC/MS中有機二元酸丁酯化標準品的分析圖譜 62
圖4.2 GC/MS中標準品Di-butyl oxalate的分析圖譜 63
圖4.3 GC/MS中標準品Di-butyl malonate的分析圖譜 64
圖4.4 GC/MS中標準品Di-butyl succinate的分析圖譜 64
圖4.5 GC/MS中標準品Di-butyl glutarate的分析圖譜 65
圖4.6 GC/MS中內標2-Bromododecanoic acid甲酯化的分析圖譜 65
圖4.7 Hexane的萃取二丁酯標準品的回收效率 67
圖4.8 無水硫酸鈉吸水與不吸水狀態下的情形 69
圖4.9 無水硫酸鈉管柱裝置圖 70
圖4.10 二元有機酸氣膠的萃取分析標準作業流程 73
圖4.11台北縣新莊運動公園採樣點周遭地理環境 74
圖4.12 25℃環境下Oxalic acid的含水特性 79
圖4.13 25℃環境下Malonic acid的含水特性 81
圖4.14 25℃環境下Succinic acid的含水特性 82
圖4.15 25℃環境下Glutaric acid的含水特性 84
圖4.16 不同溫度下Malonic acid含水特性的改變 87
圖4.17 不同溫度下Succinic acid含水特性的改變 88
圖4.18 不同溫度下Glutaric acid含水特性的改變 89

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指導教授

李崇德(C-T Lee)

審核日期

2003-12-23

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