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研究生:溫志雄
研究生(外文):Jyh-Shyong Wen
論文名稱:台灣一般大氣氣膠化學成份之連續監測及含水量之量測
論文名稱(外文):Continuous monitoring of major chemical components of aerosols in Taiwan and Measurement of liquid water content.
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:2002
畢業學年度:90
語文別:中文
論文頁數:200
中文關鍵詞:超級測站質量濃度有機碳元素碳黑碳硫酸鹽硝酸鹽氣膠含水量ISORROPIA模式
外文關鍵詞:liquid water contentISORROPIAmass concentrationSupersitenitratesulfateorganic carbonelemental carbonblack carbon
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大氣氣膠對環境的衝擊及人體健康的效應,已經引起重視,並投入大量的經費與人力進行研究。但對於氣膠特性的解析仍然多憑藉人工採樣,使用濾紙採樣然後分析氣膠特性,僅可提供較粗略的時間與空間的解析度,而且對於採樣誤差不容易量化,因此提供精確且能避免採樣運送及儲存誤差的即時(Real-Time)自動連續量測是很重要的,台灣超級測站的建置即是希望能提供達到上述目的所需的監測結果。在台灣地區由於大氣溼度較高,考量大氣氣膠在高濕環境朝解其含水量對於質量濃度量測、酸性沉降、光學性質、全球氣候變遷與人體健康皆具有顯著的影響,因此估算大氣氣膠含水量有其必要性,目前含水量推估模式雖然已經發展出來,但都是以實驗室產生的氣膠為基礎,對於大氣氣膠含水量的估算仍然有待評估,而且目前對於大氣氣膠含水量直接量測得數據仍然相當有限,有鑑於此,本文使用一套能量測收集在濾紙上氣膠含水量量測系統 (Chang and Lee, 2002; Lee and Chang, 2002),進行量測與模式模擬的比較,期望能初步探窺大氣氣膠含水量的面貌。
研究結果顯示出台北地區2002年春季PM2.5的平均濃度為37.2mg/m3,PM10的平均濃度為54.9mg/m3。有機碳成份的平均濃度為7.6mg/m3,元素碳成份的平均濃度為2.6mg/m3,黑碳的平均濃度為3.7mg/m3。硫酸鹽的平均濃度為7.1mg/m3,硝酸鹽的平均濃度為3.6mg/m3,若不考量黃沙時期的影響,3到5月各月月平均濃度變化不大。
在量測期間氣膠特性的變動顯示:氣膠質量濃度及主要化學物種濃度的隨時間變化濃度受上下班(學)的影響大,工作日及假日型態有明顯差異。 風速影響污染物的稀釋與擴散,本文發現:除了PM2.5-10濃度與風速成正比外,其他監測項目皆成反比。在高相對濕度,PM10由粗細粒徑氣膠共存,轉變為以細粒徑氣膠為主。從二次有機碳估算結果顯示細粒徑氣膠碳成份主要為二次有機碳,約佔總碳的56%,其次為元素碳佔25%,一次有機碳佔19%。本文以「近污染源氣膠化學性質」推估PM2.5污染來源 (Lee and Hsu, 1996),結果顯示二次反應所佔百分比高於交通活動,二種來源加總可佔細粒徑氣膠約35%至95%不等。
對於氣膠含水量特性的探討,本文獲得具體成果如下:從含水量與各監測項目相關係數矩陣來看,含水量主要受相對濕度及氣膠成份的影響。從大氣氣膠含水量歷程分析來看,若將乾微粒直接增濕到當時大氣相對溼度,所量測到的含水量是低估的,因為沒有考慮到氣膠在大氣中的歷程。但若從最高溼度降濕到當時大氣相對溼度,所測得的微粒含水量,則有高估的可能。因此,必須考量微粒在增濕前的大氣相對溼度所保有的含水量,才能量測到正確的含水量。若氣膠已經增濕到比較屬於高濕度的階段,則三種方式量測到的水量彼此相當接近。 本文量測的氣膠含水量與模式推估值有良好的相關性,判定係數R2高達0.86,但模式值低估許多,造成差異的原因主要有:模式值未納入吸濕性有機物、使用水溶性離子未涵蓋大氣中易吸濕的所有無機性鹽類。當秤重溫度維持在22∼27℃間,濕度控制在26∼34%之間,乾氣膠成份中仍帶有3%至29%的水量。在回復採樣時大氣相對溼度氣膠含水量顯示,氣膠含水量佔細粒徑氣膠百分比平均為64%,最大為86%,最低也有30%。
The environmental impact and health effects of atmospheric aerosols have drawn much attention. From time to time, people invest a great deal of money and efforts to understand the role of aerosols. Until recently, filter based sampling and laboratory analysis is still the mainstream to resolve aerosol properties. This could only provide a rough temporal and spatial resolution of aerosol chemical contents and is hard for quantification of sampling artifacts. The real-time continuous measurement for aerosol properties could provide the solution of acquiring precise results without incurring transportation and storge errors like filter samples. The installation of Taiwan supersite is to achieve the aforementioned objectives. Owing to the high atmospheric RH, it is necessary to assess liquid water content (LWC) of aerosols for their effects on mass measurement, acid deposition, light attenuation, global change, and health effects. Although there are several thermal equilibrium models to estimate aerosol LWC, however, they are all built by the LWC of laboratory generated known aerosols. These models need more data from aerosols in real atmosphere to test. To date, the data of aerosol LWC are scarce; this study adopted a developed measurement system to detect LWC from collected filters (Chang and Lee, 2002; Lee and Chang, 2002). Measurement results and model estimates are compared in this study to understand more on aerosol LWC in the real atmosphere.
The results of aerosol properties from continuous monitoring in the springtime of urban Taipei show as follows. PM2.5 and PM10 is with an average of 37.2mg/m3 and 54.9mg/m3, respectively. The average of organic carbon is higher at 7.6mg/m3 compared with 2.6mg/m3 for elemental carbon and 3.7mg/m3 for black carbon. The measured average for sulfates is 7.1mg/m3 and that of 3.6mg/m3 is for nitrates. For all these aerosol properties, excluding the data during yellow sand periods, the monthly averages vary very little from March to May.
The time history of aerosol mass and major chemical species are influenced by the time shift of on and off duty. Concentration pattern in working days and holidays is deviated from each other significantly. Wind speed has been expected to influence the dilution and dispersion of pollutants. This study agrees with the above inference by showing a linear relationship between PM2.5-10 and wind speed and a reverse relationship between wind speed and other measurements. At high relative humidity (RH), the predominant size fraction changed from equal weight of fine and coarse particles into fine particles. An apportionment of carbonaceous materials shows secondary organic carbon is predominant in occupying 56%, followed by elemental carbon with 25%, and primary organic carbon with 19%. By applying a “near-source aerosol chemical properties” source apportionment to PM2.5, the contributions from secondary reaction is found higher than that from mobile vehicles. The contributions from the two sources could be summed up to 35-95% of fine mass.
For the assessment of LWC of aerosol, aerosol LWC is found mainly determined by atmospheric RH and its chemical compositions. From the humidographs of aerosol LWC, the results will tend to underestimate if the measurement system is operated from dry state of arosol to the reconstructed RH. However, starting from a very high RH to the reconstructed RH will induce an overestimate in measuring aerosol LWC. The right procedure is to include aerosol LWC retained in the previous RH cycle. Meanwhile, for aerosol in the high RH stage, the measurements of aerosol LWC are close to each other. The aerosol LWC measured in this study is agreed well with ISORROPIA model estimate with a R2 at 0.86. However, the model underestimates aerosol LWC, which is probably due to not incorporating hygroscopic organics and all hygroscopic inorganic salts into the model. It is noteworthy to reveal that for temperature controlled in the range of 22-270C and RH within 26-34%, the conditioned particles before weighing still carry 3-29% LWC. The measurement of aerosol LWC at the RH when it was collected shows an average of 64% in the range of 86-30% of the fine mass.
摘要
Abstract
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……………………………………5
2.1 氣膠量測目的及遭遇問題………………………………………….5
2.1.1氣膠量測目的……………………………………………………5
2.1.2氣膠量測的問題…………………………………………….…..6.
2.2 氣膠對環境的衝擊與健康上的危害………………………...……11
2.3 氣膠物理化學特性及質量濃度量測……………………………..13
2.4 氣膠碳成份來源及量測…………………………………………..18
2.4.1 元素碳的組成………………………………………………..18
2.4.2元素碳的來源…………………………………………………20
2.4.3 有機碳的組成…………………………………………………21
2.4.4 有機碳的來源…………………………………………………22
2.4.5 氣膠碳成份的量測……………………………………………23
2.5 氣膠硫╱硝酸鹽來源及量測……………………………………...34
2.5.1氣膠硫╱硝酸鹽來源……………………………..………….34
2.5.2 氣膠硫╱硝酸鹽來源的量測……………..…………………35
2.6 氣膠含水量量測………………………………………………….37
2.6.1氣膠含水量特性……………………………………………..37
2.6.2 氣膠含水量的量測方法…………………..…………………39
2.7 氣膠特性連續監測(超級測站)……………………………….53
2.7.1美國超級測站簡介……………………………………….…..53
2.7.2台灣超級測站簡介…………………………………………56
第三章、研究方法…………………………………70
3.1 採樣及監測地點環境說明………………………………………70
3.2 實驗方法及流程…………………………………………………70
3.3 連續自動監測設備…………………………………………..…..71
3.3.1氣膠質量濃度連續監測…………………………………….72
3.3.2 氣膠碳成份連續監測………………………………………76
3.2.3氣膠硫酸鹽連續監測………………………………………79
3.3.4 氣膠硝酸鹽連續監測………………………………………83
3.3.5氣膠黑碳濃度連續監測……………………………………87
3.4 採樣設備及含水量分析儀………………………………………91
3.4.1 濾紙重量分析……………………………………………….91
3.4.2 水溶性離子成份分析…..…………………………………..92
3.4.3 含水量分析儀……..…………………………………….….93
3.5 ISORROPIA模式………………………………………………104
第四章、結果與討論……………………………….116
4.1 大氣氣膠即時監測結果基本描述………………….……….….116
4.1.1 氣膠質量濃度………………………………………………117
4.1.2 氣膠碳成份濃度……………………………………………119
4.1.3 氣膠硫酸鹽濃度……………………………………………121
4.1.4氣膠硝酸鹽濃度…………………………………………….122
4.1.5 氣膠黑碳濃度……………………………………………….122
4.1.6 氣象因子……………………………………………………123
4.2 大氣氣膠變動特性及污染來源分析………………………..…..124
4.2.1 一日間24小時變化及假日╱工作日的差異………………124
4.2.2 氣象因子與氣膠質量濃度及化學成份的關係…………….128
4.2.3 二次有機氣膠的估算………………………………………132
4.2.4 近污染源氣膠化學性質推估PM2.5污染來源……………..134
4.3 大氣氣膠含水量特性探討………………………………………135
4.3.1 大氣氣膠濃度及成份…….…………………………………135
4.3.2 大氣氣膠含水量歷程分析………………………………….138
4.3.3 大氣氣膠含水量實測值與模式推估值差異比較………….140
4.3.4 大氣氣膠吸濕潮解影響因子探討…………………………142
4.3.5大氣氣膠含水量對質量濃度的影響………………………144
4.4 不同監測方法結果比較…………………………………………146
4.4.1 黑碳與元素碳的比較………………………………………146
4.4.2 不同去除水氣方法對PM2.5質量濃度的影響……………147
第五章、結論與建議……………………………….187
5.1 結論……………………………………………………………….187
5.2建議………………………………………………………………..189
參考文獻……………………………………………190
圖 目 錄
圖2.1、PM2.5氣膠中非揮發和半揮發性物質示意圖…………………64
圖2.2、氣膠的三種模態……………………………………………….64
圖2.3、理想大氣氣膠的粒徑分布…………………………………….65
圖2.4、DRI TOR碳分析儀區塊圖……………………………..……..66
圖2.5、DRI TOR 碳分析結果溫度記錄曲線(thermogram)範例….67.
圖2.6、次微米石墨中OC與EC經由MnO2氧化的時間與溫度關係……………………………………………………………..…..…….68
圖2.7、次微米石墨經由MnO2氧化的Arrhenius plot………………68
圖2.8、美國PM2.5細粒徑氣膠監測網絡示意圖…………………….69
圖2.9、美國超級測站分布位置………………………………..…….69
圖3.1、超級測站置放地點:新莊運動公園附近地圖………….….105
圖3.2、本研究的實驗方法及流程圖………………………………..106
圖3.3、R&P 1400a氣膠質量濃度監測系統……………………….107
圖3.4、漸縮元件示意圖…………………………………………….108
圖3.5、自動採樣盒收集單元……………………………………….108
圖3.6、R&P 5400碳成份連續監測儀(外觀;硬體設置盤)………109
圖3.7、收集器/燃燒器………………………………………………109
圖3.8、氣膠碳成份連續監測儀採樣階段氣流流程………………109
圖3.9、氣膠碳成份連續監測儀分析階段氣流流程……………….110
圖3.10、C3脈衝產生器…………………………………………….110
圖3.11、SO2脈衝分析儀……………………………………………110
圖3.12、大氣氣膠硫酸鹽成份監測儀採樣分析流程…………..…111
圖3.13、C3脈衝產生器…………………………………………….111
圖3.14、NOX脈衝分析儀…………………………………………..111
圖3.15、大氣氣膠硫酸鹽成份監測儀採樣分析流程……………..112
圖3.16、吸光儀外觀………………………………………………..112
圖3.17、吸光儀剖面圖………………………………………………113
圖3.18、吸光儀運轉示意圖…………………………………………113
圖3.19、在相對溼度為20%、50%與85%時,比較NaCl氣膠系統背景水量與總系統水量的量測訊號圖譜……………………………114
圖3.20、GC-TCD氣膠含水量量測系統設備……………………..115
圖4.1、各監測項目直方圖…………………………………………156
圖4.2、PM2.5及PM10質量濃度每日平均值變化趨勢……………158
圖4.3、PM2.5總碳及有機碳濃度每日平均值變化趨勢……………158
圖4.4、PM2.5元素碳及黑碳濃度每日平均值變化趨勢……………159
圖4.5、PM2.5硫酸鹽及硝酸鹽濃度每日平均值變化趨勢………….159
圖4.6、盒型圖圖例符號說明………………………………………160
圖4.7、工作日PM2.5質量濃度一日24小時變化趨勢……….…..161
圖4.8、例假日PM2.5質量濃度一日24小時變化趨勢……………161
圖4.9、工作日PM10質量濃度一日24小時變化趨勢……………162
圖4.10、例假日PM10質量濃度一日24小時變化趨勢……………162
圖4.11、工作日TC濃度一日24小時變化趨勢…………………..163
圖4.12、例假日TC濃度一日24小時變化趨勢………………….163
圖4.13、工作日OC濃度一日24小時變化趨勢…………………..164
圖4.14、例假日OC濃度一日24小時變化趨勢…………………..164
圖4.15、工作日EC濃度一日24小時變化趨勢…………………..165
圖4.16、例假日EC濃度一日24小時變化趨勢…………………..165
圖4.17、工作日Sulfate濃度一日24小時變化趨勢……………….166
圖4.18、例假日Sulfate濃度一日24小時變化趨勢……………….166
圖4.19、工作日Nitrate濃度一日24小時變化趨勢………………167
圖4.20、例假日Nitrate濃度一日24小時變化趨勢………………167
圖4.21、風速與氣膠質量濃度及化學成份的關係…………………168
圖4.22、降雨與氣膠質量濃度的變化………………………………169
圖4.23、相對濕度與氣膠質量濃度的關係………………………….170
圖4.24、相對濕度與PM2.5氣膠化學成份的關係…………………..171
圖4.25、不同濕度下PM2.5與PM10質量濃度的關係…………….172
圖4.26、台北地區春季一次及二次有機碳日平均變化…………..173
圖4.27、台北地區春季氣膠污染來源推估………………………..174
圖4.28、TEOM與短時程(6小時)濾紙採樣PM2.5質量濃度比較.175
圖4.29、大氣氣膠含水量與溫濕度變化趨勢………………………176
圖4.30、氣膠質量濃度及吸濕物種連續監測結果…………………177
圖4.31、大氣氣膠實際含水量比較…………………………….178
圖4.32、大氣氣膠實測含水量與ISORROPIA模式估算值關係….181
圖4.33、連續監測硫酸鹽平均值與IC分析量測值比較………….181
圖4.34、連續監測硝酸鹽平均值與IC分析量測值比較…………..182
圖4.35、實測含水量與ISORROPIA模式估算值(4月19日)….183
圖4.36、實測含水量與ISORROPIA模式估算值(4月20日)…..184
圖4.37、實測含水量與ISORROPIA模式估算值(4月21日)…..185
圖4.38、BC與EC的關係…………………………………………..186
圖4.39、不同去除水氣方法PM2.5質量濃度的關係……………….186
表 目 錄
表2.1、主要空氣污染物及污染來源…………………………………57
表2.2、空氣污染物質的影響.………………………………………...58
表2.3、細粒(包含成核態和累積態)及粗粒氣膠物理及化學性質.59
表2.4、燃料燃燒所產生氣膠碳排放率推估…………………………60
表2.5、不同來源元素碳與有機碳佔氣膠總質量比率……………...61
表2.6、部份都會區的大氣氣膠中經證實的二次有機化合物………62
表4.1、台北地區春季氣膠監測結果基本統計結果………………..150
表4.2、台北地區春季氣膠化學成份各月平均值…………………..151
表4.3、台北地區春季氣膠化學成份各月所佔比例……………….151
表4.4、台北地區春季不同時段OC與EC迴歸式………………..152
表4.5、短時程採樣IC分析水溶性離子濃度………………………153
表4.6、含水量與各監測項目相關係數矩陣……………………….154
表4.7、於後秤重時溫濕度狀態下的氣膠含水量佔PM2.5質量濃度百分比………………………………………………………………….….155
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