博碩士論文 102326014 詳細資訊




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姓名 許家綺(Chia-chi Hsu)  查詢紙本館藏   畢業系所 環境工程研究所
論文名稱 2011-2015年台灣都會區細懸浮微粒(PM2.5)成分濃度變化、污染來源推估及對能見度影響
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摘要(中) 大氣細懸浮微粒(氣動粒徑小於2.5μg m-3, PM2.5)會對民眾健康造成影響並導致大氣環境的變遷,檢測各地PM2.5化學特性,有助於瞭解PM2.5環境效應及污染來源。本文彙整2011年至2015年在台灣北(新莊、板橋)、中(忠明)、南(前鎮、前金、小港) 都會區環保署空氣品質監測站手動採集的PM2.5質量及化學成分濃度數據,探討台灣北、中、南部PM2.5的變化趨勢。在PM2.5採集過程,微粒半揮發性成分的揮發以及石英濾紙的吸附有機氣體會影響成分量測的正確性,本文藉由連續三張濾紙裝置進行干擾修正並探討揮發性成分特性以及影響因子。對於PM2.5污染來源,本文以受體模式PMF (Positive Matrix Factorization)進行推估,並以CPF (Conditional Probability Function)輔助判別本地污染源影響,最後探討影響大氣能見度的PM2.5化學成分、氣象因子及污染來源。

研究結果顯示北部地區PM2.5質量濃度以春季最高,且在三月有高濃度發生,四個季節PM2.5化學成分都以SO42-為優勢物種,但夏季SO42-與修正OC濃度濃度差異不大,顯示夏季有機物影響相對重要;中部地區PM2.5質量濃度以秋季最高,SO42-在四個季節都是最主要成分濃度;南部地區PM2.5質量濃度以冬季最高,PM2.5化學成分濃度在四個季節也都以SO42-為主要成分。

PM2.5水溶性無機離子NO3-及Cl-為半揮發性成分,在北部、中部及南部測站NO3-揮發/未修正濃度比值除了冬季以外,其他三個季節都大於100%,且以夏季比值最大;Cl-揮發/ 未修正濃度比值則在四個季節都大於100%,如果不進行修正,會造成PM2.5揮發成分低估。比較PM2.5在低濃度(<35μg m-3)和高濃度(>35μg m-3)各成分占比,SO42-、OC、EC占比下降、NH4+維持不變、NO3-從6%增加到13%,Cl-從1%增加到2%,NO3-增加的幅度最為明顯,顯示降低NO3-和Cl-前驅產生源排放,有助於降低高濃度事件的發生。本文以濾紙採集揮發NH4+,發現揮發NH4+當量數通常大於揮發(NO3-+Cl-)當量數,推測可能有空氣中NH3(g)穿透denuder的現象。

PM2.5碳成分採集過程會發生有機碳揮發以及石英濾紙吸附有機氣體的現象,北、中、南部揮發性有機碳占有機碳的比例平均分別為9%、11、8%,北、中、南部石英濾紙吸附有機氣體的占有機碳比例平均為18、16、14%,代表如果不進行修正,會造成北、中、南有機碳成分平均高估9%、5%、6%。討論揮發離子濃度與環境最高溫度(Tmax)及修正後的PM2.5質量濃度的關係指出揮發NO3- 和NH4+與環境最高溫度及PM2.5濃度有關,揮發Cl-與環境最高溫相關性則不顯著。

利用PMF推估並以CPF輔助判別污染來源,北部、中部、南部測站都以二次硫酸鹽和二次硝酸鹽及氯鹽污染源類別貢獻最大,顯示台灣都市地區PM2.5空氣品質受到化石燃料燃燒排放的影響為最主要。大氣能見度的衰減以南部最為嚴重,整個採樣期間能見度平均為7.5±3.16 km,北部和中部能見度較南部好,採樣期間能見度平均分別為12.57±4.13 km、12.72±3.4 km,能見度以中部>北部>南部。將PM2.5化學成分、污染來源和氣象因子對大氣能見度進行多元迴歸分析,北、中、南能見度主要受水溶性無機離子和氣象因子的影響。

摘要(英) Atmospheric fine particulate matter (aerodynamic diameter less than or equal to PM2.5) will pose human health risk and cause atmospheric environmental change. In order to understand PM2.5 variation trends in Northern, Middle, and Southern Taiwan, this study summarized the results of PM2.5 mass and chemical components manually collected at Xinzhuang, Banqiao, Chungming, Qianzhen, Qianjin, and Siaogang, respectively from 2011 to 2015. The correctness of aerosol components is affected by volatilization of semi-volatile species and the adsorption of volatile organic gases during PM2.5 collection. In this study, a three-filter series was adopted to correct the interference of volatile species and affecting factors. Source apportionment of PM2.5 was conducted by using Positive Matrix Factorization (PMF) with the assistance of Conditional Probability Function (CPF) for local source evaluations. In the final step, the effects of meteorological factors and polluted sources were regressed on ambient visibility.

The results show that PM2.5 mass level was highest in March and SO42- was a predominant species in all seasons in Northern Taiwan. However, the corrected organic carbon (OC) competed with SO42- as the predominant component in summer which indicated organic compounds were important in summer. PM2.5 mass level is highest in autumn and SO42- is a predominant species in all seasons in Middle Taiwan. In addition, PM2.5 mass level is highest in winter and SO42- is a predominant species in all seasons in Southern Taiwan.

The volatilization of NO3- and Cl- are significant as the volatile ratio is greater than one in most occasions. The fraction of NO3- to PM2.5 mass level increased from 6% to 13% when PM2.5 mass level was low (<35μg m-3) as compared to high (>35μg m-3). In implies that the reduction of NO3- and Cl- precursor sources will help reduce high pollution events. Meanwhile, NH3(g) was found to penetrate from denuder adsorption as the equivalence of volatile NH4+ was greater than the equivalence of volatile (NO3-+Cl-) most of the time.

The fractions of volatile OC to retained OC level in the first filter were 9%, 11, and 8% in Northern, Middle, and Southern Taiwan, respectively. Moreover, the fractions of adsorbed volatile organic gases to retained OC level were 18, 16%, and 14% in Northern, Middle, and Southern Taiwan, respectively. If no correction was made, the OC fractions in retained OC mass level would overestimate 9%, 5%, and 6%, respectively. The volatilized NO3- and NH4+ are related to maximum ambient temperature and corrected PM2.5 mass level; however, the volatilized Cl- is not significantly affected by maximum ambient temperature.

The source apportionment using PMF and aided by using CPF showed that sources of secondary sulfate, nitrate, and chloride contributed greatly in Northern, Middle, and Southern Taiwan. It indicates fossil fuel combustion is the most significant source in affecting urban PM2.5 air quality. The degradation of atmospheric visibility is most serious in Southern Taiwan with visibility averaged at 7.5±3.16 km. In contrast, the visibilities in Northern and Middle Taiwan are better with values at 12.57±4.13 km and 12.72±3.4 km, respectively. From multiple regression analysis on ambient visibility by using PM2.5 chemical components, pollution sources, and meteorological factors, water-soluble inorganic ions and meteorological factors are found significant in affecting the visibility in Northern, Middle, and Southern Taiwan.

關鍵字(中) ★ 細懸浮微粒(PM2.5)
★ PM2.5化學成分
★ PM2.5化學成分揮發評估
★ PMF來源解析
★ 大氣能見度
關鍵字(英) ★ Fine particulate matter (PM2.5)
★ PM2.5 chemical components
★ Volatilization assessment of PM2.5 chemical components
★ PMF source apportionment
★ Ambient visibility
論文目次 摘要 III

Abstract III

目錄 VIII

表目錄 X

圖目錄 XII

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細懸浮微粒(PM2.5)重要性之文獻 4

2.1.1 PM2.5對人體的危害 4

2.1.2台灣都會區PM2.5時間與空間濃度分布特性 5

2.1.3大氣中能見度與PM2.5的關係 8

2.2細懸浮微粒(PM2.5)形成來源 10

2.3氣膠化學組成 11

2.3.1 PM2.5氣膠水溶性離子組成 11

2.3.2 PM2.5氣膠碳成分組成 12

2.4受體模式正矩陣因子法PMF(Positive Matrix Factorization)應用 13

第三章 研究方法 15

3.1研究架構 15

3.2採樣地點與時間 16

3.2.1採樣地點 17

3.2.2採樣時間 19

3.3 R&P 2300氣膠成分分析採樣器 20

3.4 PM2.5質量和成分分析方法 24

3.4.1濾紙採樣前準備 24

3.4.2質量濃度秤重分析 25

3.4.3氣膠水溶性離子分析方法 26

3.4.4氣膠碳成分分析方法 27

3.4.5微粒揮發NO3-、NH4+、Cl-及OC補償方法 29

3.5正矩陣因子法PMF (Positive Matrix Factorization)操作 32

3.5.1輸入資料處理 33

3.5.2模式操作 34

3.6條件機率函數CPF (Conditional probability function)推估方法 38

第四章 結果與討論 39

4.1台灣北中南都會區PM2.5手動成分採樣濃度變化趨勢 39

4.1.1北部測站PM2.5成分濃度隨季節及時間的變化 40

4.1.2中部測站PM2.5成分濃度隨季節及時間的變化 44

4.1.3 南部測站PM2.5成分濃度隨季節及時間的變化 48

4.1.4 PM2.5成分占比與PM2.5質量濃度的關係 52

4.2 PM2.5半揮發成分揮發和影響因素 58

4.2.1揮發NH4+探討 58

4.2.2揮發性有機碳及吸附有機氣體Retained有機碳的關係 61

4.2.3 熱光學反射法(TOR)及熱光學透射(TOT)分析裂解碳的差異 64

4.3揮發離子濃度推估 69

4.3.1環境最高溫度(TMax)及修正後PM2.5質量濃度關係推估揮發NO3-濃度 69

4.3.2環境最高溫度(TMax)及修正後PM2.5質量濃度關係推估揮發Cl-濃度 73

4.3.3環境最高溫度(TMax)及修正後PM2.5質量濃度關係推估揮發NH4+濃度 77

4.4受體模式PMF推估北、中、南都會區PM2.5污染來源 81

4.4.1 北部測站PMF推估PM2.5污染來源 81

4.4.2 中部測站PMF推估 PM2.5污染來源 91

4.4.3 南部測站PMF推估 PM2.5污染來源 100

4.5台灣北、中、南都會區PM2.5濃度及氣象因子對大氣能見度影響 112

4.5.1 修正後PM2.5成分及天氣因子與能見度的擬合方程式 117

4.5.2 PM2.5污染因子對大氣能見度影響 123

第五章 結論與建議 128

5.1結論 128

5.2 建議 130

第六章 參考文獻 131

附錄1 各監測站周邊建設及四周環境位置 140

附錄2 北部測站PMF Bootstrap model結果 142

附錄3 中部測站PMF Bootstrap model結果 144

附錄4 南部測站PMF Bootstrap model結果 146

附錄5 CPF篩選因子貢獻濃度前15%日期 148

附錄6 口試委員意見答覆 151

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指導教授 李崇德 審核日期 2015-8-27
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