博碩士論文 953206020 詳細資訊




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姓名 陳永盛(Yung-sheng Chen)  查詢紙本館藏   畢業系所 環境工程研究所
論文名稱 大氣氣膠碳成分量測方法比較及干擾因子的探討
(On the study of measuring methods and interfering factors in the determination of atmospheric aerosol carbons)
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摘要(中) 以熱-光學法分析大氣氣膠碳成分,是廣泛被使用的量測方法,這種方法對於分析過程產生裂解碳的矯正程序,可分成熱-光學反射(TOR)和熱-光學透射(TOT)兩種。本文比較不同溫度協定與裂解碳校正方法的差異,並探討濾紙採樣受到揮發性有機化合物(VOCs, Volatile Organic Compounds)干擾的影響。此外,本文也在海岸地區採樣,進行NaCl對於EC成分解析干擾的評估。最後再以北部新莊微粒超級測站的BC (black carbon)與EC (elemental carbon)監測數據進行線性迴歸分析,以斜率得到BC吸光截面積(σ)的修正數值,訂定大台北都會區合適的σ數值,以及探討σ的影響因子。
研究結果顯示,當大氣氣膠碳成分濃度增加,微粒在濾紙沉積厚度變大,TOR比TOT方式所估算的裂解碳濃度將較低。都市地區由於受到車輛排放與溫度的影響,當進行碳成分採樣時,石英濾紙吸附VOCs的濃度將會提升,且微粒有機碳揮發情形較為顯著。經由北縣石門海岸測站觀測結果顯示,當Na+濃度達3 ~ 6 μg m-3之間時,Na+對於EC成分解析的干擾情形顯著。
本文以2006 ~ 2007兩年環保署北部微粒超級測站逐時數據共約17,000筆,得到σ的修正數值,在這段期間σ數值變動範圍約在20 ~ 40 m2 g-1,當硝酸鹽濃度增加、臭氧發生高濃度、大氣相對濕度達90%以上、以及降雨事件時段,都將造成σ數值上升。本文在評估σ數值日變化時,發現上下班尖峰時段σ數值跟著增加。σ的日變化也與PM2.5、PAH(總多環芳香烴)、OC(有機碳)日變化三者具有良好的相關,顯示當大氣氣膠濃度與有機成分增多將對σ數值造成影響。對於大台北都會區合適的σ數值,本文建議應該從製造商提供的16.6 m2 g-1改為24.5 m2 g-1,此數值適用於AE 31吸光儀量測BC的880 nm波段。
摘要(英) The thermal-optical method is widely used for measuring atmospheric aerosol carbons. In this method, pyrolyzed carbon correction can be split into thermal optical reflectance (TOR) and thermal optical transmittance (TOT). This study compares the differences due to different temperature protocols and pyrolyzed carbon corrections. Meanwhile, the interferences of volatile organic carbons (VOCs) on aerosol carbon analysis for filter samples are also studied. Moreover, the effects of NaCl on EC fractionization in the coastal area are evaluated. Finally, the monitoring data of aerosol black carbon (BC) and elemental carbon (EC) from North aerosol supersite are adopted to conduct a linear regression analysis. The slope resulted from this analysis is considered to be the best BC absorption cross section (σ) and the influencing factors of σ values are also disussed.
The results show that TOR tends to underestimate pyrolyzed carbon correction when atmospheric carbon concentration is increased and thus the depth of particle deposition on a filter. Under the influence of vehicle exhausts and ambient temperature, VOCs adsorption by quartz fiber filter will be increased when using the filter in aerosol collection. Meanwhile, organic carbon evaporation from deposited particles is severer. The interference of Na+ on EC fractionization is significant when Na+ concentration reaches 3 - 6 μg m-3 based on the observation at the Shimen site on the coastline of Taipei County.
In this study, 17,000 hourly data from North aerosol supersite were used to obtain the correction value of σ. The variation of σ is within the range of 20 - 40 m2 g-1 during this time period. Meanwhile, the value of σ is found to increase with higher aerosol nitrate, higher ozone concentration, higher atmospheric relative humidity above 90%, and the duration of raining event. In the diurnal variation of σ, σ value is found to enhance in the traffic peak hours. The diurnal variations of σ value are also agreed well with that of PM2.5, PAH, and OC. It indicates that the increase of atmospheric aerosols and aerosol organic fractions will affect σ values. The best σ value in the greater Taipei metropolis is recommended to change from the manufacturer’s 16.6 to 24.5 m2 g-1 for AE31 Aethalometer in measuring BC at 880 nm wavelength.
關鍵字(中) ★ 氣膠碳成分
★ 碳成分量測方法比較
★ NaCl干擾
★ 黑碳吸光截面積σ
★ VOCs
關鍵字(英) ★ Aerosol carbon fractions
★ comparison of aerosol carbon measurements
★ NaCl interference
★ absorption cross section of black carbon (σ)
★ Volatile organic carbons (VOCs)
論文目次 摘要 I
Abstract III
致謝 V
圖目錄 IX
表目錄 XII
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大氣氣膠的來源及特性 3
2.1.1 氣膠的來源與及分類 3
2.1.2 氣膠的化學特性與粒徑分布 3
2.2氣膠碳成分特性 8
2.2.1 碳成分來源與組成 9
2.2.2 碳成分分布 10
2.3 氣膠碳成分的量測方法 12
2.3.1 IMPROVE (TOR)碳分析法 12
2.3.2 NIOSH (TOT)碳分析法 14
2.3.3 Aethalometer (AE31)氣膠吸光儀 15
2.4氣膠碳成分量測方法比較 16
2.5 微粒有機碳受VOCs影響推估 22
2.6 化學水溶性離子對於元素碳的干擾 24
2.7 黑碳吸光截面積的變化 26
第三章 研究方法 35
3.1 監測及採樣位址選定 38
3.1.1監測及採樣地點 38
3.1.2 監測及採樣時間 40
3.2 氣膠特性監測及採樣儀器 41
3.2.1 連續自動監測儀器 41
3.2.2連續自動監測儀器數據分析處理 42
3.2.3 人工採樣器 44
3.3 人工採樣分析方法 46
3.3.1 氣膠質量濃度秤重分析 46
3.3.2 氣膠水溶性離子分析 47
3.3.3 氣膠碳成分分析 48
3.4 碳成分監測及分析儀器 49
3.4.1 DRI 2001氣膠碳成分分析儀 49
3.4.2 Sunset 5040半自動氣膠碳成分監測儀 52
3.4.3 AE 31氣膠吸光儀(黑碳濃度監測儀) 54
3.5 碳成分量測方法比較 57
3.5.1 IMPROVE與NIOSH分析方法比較 57
3.5.2 調整溫度協定造成的分析差異 57
3.5.3 TOT與TOR裂解碳校正差異 59
3.5.4 VOCs的影響及氣膠有機碳推估 60
3.5.5 石英濾紙吸附VOCs的飽和試驗 61
3.6 NaCl對於元素碳的干擾評估 62
3.7 黑碳吸光截面積的建立 63
第四章 結果與討論 67
4.1 碳分析儀測試及校正 67
4.1.1 DRI 2001碳分析儀測試及校正 67
4.1.2 Sunset 5040 碳分析儀測試及校正 72
4.1.3 AE 31 吸光儀測試及校正 74
4.1.4 濾紙樣本重複試驗精確性評估 75
4.2 碳成分量測方法比較 77
4.2.1 IMPROVE與NIOSH分析方法比較 77
4.2.2 調整溫度協定造成的分析差異 81
4.2.3 TOT與TOR校正方法差異 86
4.2.4 微粒沉積厚度對於TOT與TOR方法的估算差異 91
4.2.5微粒有機碳(POC)的誤差推估 96
4.2.6 石英濾紙吸附VOCs的飽和試驗 102
4.3 黑碳及元素碳的量測方法比較 104
4.4 化學水溶性離子對於EC的干擾評估 107
4.4.1 NaCl對EC干擾試驗 108
4.4.2 海岸背景測站的EC受NaCl的干擾影響 112
4.5 黑碳吸光截面積的碳討 120
4.5.1 黑碳吸光截面積的建立 120
4.5.2 造成黑碳吸光截面積變化的影響因子 122
4.5.3 影響黑碳吸光截面積變化的事件日評估 126
4.5.4 黑碳吸光截面積的日變化 135
4.5.5 黑碳吸光截面積的季節性變化 142
4.5.6 台北都會區合適的黑碳吸光截面積數值 144
第五章 結論與建議 148
5.1 結論 148
5.2 建議 150
參考文獻 152
附錄一 口試委員意見答覆 166
附錄二 臭氧高濃度事件日的黑碳吸光截面積逐時變化 171
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指導教授 李崇德(Chung-Te Lee) 審核日期 2008-7-28
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