臺灣博碩士論文加值系統

摘 要
本研究於2002年配合環保署監資處大陸沙塵暴密集觀測計畫，利用環型擴散採樣器在台中市中興大學測站進行酸性空氣污染物的密集採樣，採樣時間分別為2002年1/29-2/1、2/11-2/13、3/5-3/11及3/17-3/24。採樣時同時收集大氣的溫度、濕度及風速資料，以瞭解大陸沙塵暴對中部地區酸性空氣污染物之影響。
採樣期間氣狀污染物HCl、HNO2、HNO3、NH3及SO2的平均濃度分別為0.74、2.81、1.35、6.30及8.36 g / m3，統計分析結果顯示沙塵暴及非沙塵暴期間上述氣體並無顯著差異。沙塵暴過境期間PM10、PM2.5-10及PM2.5之平均濃度為87 ± 31、 45 ± 19及42 ± 17 g / m3，而非沙塵暴期間PM10、PM2.5-10及PM2.5平均濃度則為71 ± 28g 、32 ± 17及40 ± 16 g / m3 ，在沙塵暴過境期間PM2.5-10之質量濃度有顯著增加（p＜0.05）。此外，在非沙塵暴期間，台中都會區PM2.5-10 佔 PM10之質量比例約為43 %， 而沙塵暴過境期間其質量比例高達52 %（p＝0.0502）。
氣膠中水溶性離子成分的分析結果顯示，沙塵暴過境期間PM2.5中之化學組成濃度並無增加之現象，而PM2.5-10氣膠中的Cl-、Na+、Mg2+及Ca2+則在沙塵暴期間濃度明顯增加1.6 ~21倍之間（p＜0.05），PM10氣膠中亦是以這四種離子增加最明顯，而NH4+則是唯一在PM2.5及PM2.5-10氣膠中濃度均減少的物種。在粗細粒比方面，NO3-及SO4=在沙塵暴期間粗粒濃度有明顯的增加，其餘的離子則不明顯。
分析PM10之[NH4+] / （[nss-SO4=] + [NO3-]），沙塵暴期間比值為0.72而非沙塵期間為0.81，兩者間有顯著的差異，另外計算（[NH4+] + [ Ca+]）/（[nss-SO4=] + [NO3-]），發現不論在沙塵暴及非沙塵暴期間均趨近於1，表示沙塵暴期間的高污染是粗粒中的nss-SO4=及NO3-濃度增加所導致，且Ca2+在NH4+濃度相對減少時是另一個重要之氣膠中和物種。
沙塵暴及非沙塵暴期間的PM2.5-10氣膠中氯損失分別為52及68 ％，沙塵暴過境氯損失約減少23％（p＜0.05），氯損失百分比與[Ca2+] / [Na+]比值呈現負相關，原因是沙塵暴期間Ca2+取代部分的Na+與酸性氣體反應所致，該線性回歸式為：
氯損失(％)＝ - 0.25（[Ca2+] / [Na+]）＋0.85 （R2＝0.51）
氣膠的污染來源推估結果，中部地區的PM10氣膠中是以二次氣膠的含量最多。沙塵暴帶來大量粗粒及部分細粒的塵土顆粒，造成PM10氣膠質量增加主要是來自粗粒的塵土顆粒（2倍）及海水飛沫（1.4倍），粗粒中的Ca2+與nss-SO4=呈現中度相關，而與NO3-的相關性則較差，推測應該是沙塵暴傳輸過程中經過較多SOx排放的地區所致。

Abstract
This study used Annular Denuder System (ADS) to collect acidic air pollutants ( PM10 and PM2.5 particles and acidic gases ) at Chung-Hsing university in Taichung city from January to March in 2002. In the sampling period, China dust storms effected Taiwan in 2/11-2/12D、3/6-3/9、3/18-3/19 and 3/23-3/24.
The mean concentrations of HCl(g)、HNO2(g)、HNO3(g)、SO2(g) and NH3(g) were 0.74、2.81、1.35、6.30 and 8.36 g / m3 , respectively. These concentrations are not remarkably different between the dust storm and the non-dust storm periods. In the dust storm periods the mean concentrations of PM10、PM2.5 and PM2.5-10 were 87±31、45±19 and 42±17 g / m3, respectively. The concentrations of PM2.5-10 are remarkably higher in the dust storm periods. The average ratios of PM2.5-10 / PM10 were 43％ and 52％ in the non-dust storm and the dust storm periods, respectively.
The mean concentrations of Cl-、Na+、Mg2+ and Ca2+ in the PM2.5-10 and PM10 particles in the dust storm periods are 1.6 to 2.1 times higher than these in the non-dust storm periods(p＜0.05). NO3- and SO4= species in the PM2.5-10 particles increased remarkable in the dust storm periods. However, NH4+ specie in the PM2.5 and PM2.5-10 were found significantly lower in the dust storm periods.
The average ratio of [NH4+] / （[nss-SO4=] + [NO3-]）in PM10 particles in the dust storm periods and in the non-dust storm periods were 0.72 and 0.81, respectively(p＜0.05). But（[NH4+] + [ Ca+]）/（[nss-SO4=] + [NO3-]）in PM10 particles were closed to 1.0 either in the dust storm periods or in the non-dust storm periods. These results indicate that the concentrations of nss-SO4= and NO3- in PM2.5-10 particles increase in the dust storm periods, and Ca2+ is an important neutralizing agent.
There were 52％ and 68％ chlorine loss in the dust storm periods and in the non-dust storm periods, respectively. In the dust storm periods, chlorine loss decreased about 23％(p＜0.05). Chlorine loss (％) was negatively correlated with the ratio of [Ca2+] / [Na+], since Ca2+ might replace Na+ to react with acidic gases. The relationship between Chlorine loss (％) and the ratio of [Ca2+] / [Na+] was
Chlorine loss (％) ＝ - 0.25×( [Ca2+] / [Na+] )＋0.85 R2＝0.51
Secondary aerosols (nss-NO3- and nss-SO4= ) were the major species in PM10 aerosols in central Taiwan. During the dust storm periods, most of coarse particles and a few fine particles were brought along with the China dust storms. There are about 2 times PM2.5-10 and 1.4 times ocean salts contributed by the dust storms. Ca2+ in coarse particles correlated better with nss-SO4= ias compared with NO3- in coarse particles. This result indicated that the dust storms may have passed through the area with higher SO2(g) concentrations.

目 錄
第一章 前言…...……..…...................................................1-1
1.1 研究緣起..................................................................1-1
1.2 研究目的..................................................................1-3
第二章 文獻回顧.................................................................2-1
2.1 氣膠的來源及物理化學組成特性..........................2-1
2.1.1 氣膠來源及粒徑分佈.....................................................2-1
2.1.2 氣膠水溶性離子之形成.................................................2-3
2.1.3 氣膠水溶性離子之粒徑分佈.........................................2-5
2.1.3 水溶性離子物種之特性.................................................2-7
2.2 氣膠與氣象及地形因子的關係.............................2-10
2.2.1 氣象因子的影響..........................................................2-10
2.2.2 地形因子的影響..........................................................2-11
2.3 氣膠對環境及人體健康的影響.............................2-11
2.4 台中都會區氣膠特性.............................................2-13
2.5 大陸沙塵暴特性.....................................................2-14
2.5.1 大陸沙塵暴發生原因..................................................2-14
2.5.2 大陸沙塵暴對環境及人體健康的影響......................2-15
2.5.3 台灣地區受大陸沙塵暴影響的情況..........................2-16
2.5.4 國內對於大陸沙塵暴的研究成果..............................2-16
2.6 國內外酸性空氣污染物的分析結果.....................2-19
第三章 研究方法.................................................................3-1
3.1 採樣規劃...................................................................3-1
3.1.1 採樣時間...................................................................... ..3-1
3.1.2 採樣測站之環境描述.....................................................3-1
3.1.3 採樣濾紙處理程序.........................................................3-2
3.1.4 採樣儀器設備.................................................................3-2
3.2 分析項目...................................................................3-3
3.2.1 氣膠水溶性離子分析....................................................3-3
3.2.2 氣狀污染物分析............................................................3-4
3.3 分析方法...................................................................3-5
3.3.1 氣膠酸鹼性分析.............................................................3-5
3.3.2 海水加強因子分析.........................................................3-6
3.3.3 主成分因子分析.............................................................3-6
3.3.4 氯離子損失法分析…………………………………….3-8
第四章 結果與討論..............................................................4-1
4.1 觀測值與環保署空品測站監測值之比較...............4-1
4.2 大氣氣膠質量濃度變化分析...................................4-4
4.2.1 採樣期間之空氣品質狀態及氣象因子特性..............4-10
4.2.2 氣膠質量濃度變化及粗細粒比..................................4-13
4.2.3 氣膠日夜濃度變化......................................................4-15
4.3 氣膠水溶性陰陽離子特性分析.............................4-17
4.3.1 氣膠水溶性陰陽離子濃度...........................................4-17
4.3.2 氣膠水溶性陰陽離子濃度百分比及粒徑分佈...........4-24
4.3.3 氣膠水溶性陰陽離子當量濃度平衡及酸鹼性分析...4-35
4.3.4 氣膠水溶性陰陽離子相關性分析...............................4-41
4.4 氣膠污染來源推估.................................................4-50
4.4.1 海水加強因子分析.......................................................4-50
4.4.2 主成分因子分析.............................................................4-57
4.4.3 氯離子損失法分析…………………………………….4-58
4.5 採樣期間氣狀污染物特性.....................................4-99
4.5.1 沙塵暴及非沙塵暴期間比較.......................................4-99
4.5.2 與國內外文獻比較.......................................................4-99
第五章 結論..........................................................................5-1
第六章 建議
參考文獻
附錄
附錄一 環形擴散採樣器實驗步驟
附錄二 粒狀污染物採樣結果
附錄三 氣狀污染物採樣結果
附錄四 氯鹽及硝酸鹽微粒的揮發量
附錄五 1994-2002年大陸沙塵暴影響台灣的日數統計
附錄六 沙塵暴事件日統計（PM2.5-10 / PM10）
附錄七 2000年3月中部地區沙塵暴事件日統計分析
表 目 錄
表2.1 典型大氣氣膠的三尖峰粒徑分佈...........................................2-2
表4.2.1 a 採樣紀錄（1/29-2/1及2/11-2/13）........................................4-5
表4.2.1 b 採樣紀錄（3/5-3/11）............................................................4-6
表4.2.1 c 採樣紀錄（3/17-3/24）..........................................................4-7
表4.2.2 a 採樣期間天氣型態及中部監測站PSI值（1/29-2/1及2/11-2/13）..............................................................................4-11
表4.2.2 b 採樣期間天氣型態及中部監測站PSI值（3/5-3/11及3/17-3/24）.............................................................................4-12
表4.2.3 沙塵暴與非沙塵暴採樣期間氣膠平均質量濃度與粗細粒比...........................................................................................4-15
表4.2.4 採樣期間日間及夜間大氣氣膠質量濃度比較..................4-16
表4.3.1 a 沙塵暴及非沙塵暴期間氣膠水溶性離子平均質量濃度...........................................................................................4-22
表4.3.1 b 沙塵暴及非沙塵暴期間氣膠水溶性離子平均質量百分比...........................................................................................4-23
表4.3.2 沙塵暴及非沙塵暴期間PM10、PM2.5及PM2.5-10氣膠水溶性離子含量百分比排序...........................................................4-26
表4.3.3 沙塵暴及非沙塵暴期間氣膠水溶性陰陽離子PM2.5 / PM10比值...........................................................................................4-34
表4.3.4 沙塵暴及非沙塵暴期間PM10、PM2.5 及PM2.5-10氣膠水溶性陰陽離子平衡及NR值計算結果........................................4-40
表4.3.5 a 沙塵暴期間PM10氣膠質量濃度與水溶性離子成分相關性...........................................................................................4-44
表4.3.5 b 非沙塵暴期間PM10氣膠質量濃度與水溶性離子成分相關性...........................................................................................4-45
表4.3.6 a 沙塵暴期間PM2.5氣膠質量濃度與水溶性離子成分相關性...........................................................................................4-46
表4.3.6 b 非沙塵暴期間PM2.5氣膠質量濃度與水溶性離子成分相關性...........................................................................................4-47
表4.3.7 a 沙塵暴期間PM2.5-10氣膠質量濃度與水溶性離子成分相關性...........................................................................................4-48
表4.3.7 b 非沙塵暴期間PM2.5-10氣膠質量濃度與水溶性離子成分相關性.......................................................................................4-49
表4.4.1 海水來源離子的比值..........................................................4-50
表4.4.2 a PM10氣膠氣膠中Cl-、SO4=、K+、Mg2+及Ca2+對Na+的質量比值...................................................................................4-52
表4.4.2 b PM2.5氣膠氣膠中Cl-、SO4=、K+、Mg2+及Ca2+對Na+的質量比值...................................................................................4-53
表4.4.2 c PM2.5-10氣膠氣膠中Cl-、SO4=、K+、Mg2+及Ca2+對Na+的質量比值...............................................................................4-54
表4.4.3 a PM10氣膠海水加強因子分析法結果（應用Wilson, 1975）.....................................................................................4-55
表4.4.3 b PM10氣膠海水加強因子分析法結果（應用Cheng et al., 2000）.....................................................................................4-55
表4.4.4 a PM2.5氣膠海水加強因子分析法結果（應用Wilson, 1975）.....................................................................................4-55
表4.4.4 b PM2.5氣膠海水加強因子分析法結果（應用Cheng et al., 2000）.....................................................................................4-55
表4.4.5 a PM2.5-10氣膠海水加強因子分析法結果（應用Wilson, 1975）.....................................................................................4-56
表4.4.5 b PM2.5-10氣膠海水加強因子分析法結果（應用Cheng et al., 2000）.....................................................................................4-56
表4.4.6 a 沙塵暴期間PM10氣膠化學組成、氣態空氣污染物及氣象資料之VARIMAX轉換因子分析結果總表（樣本數為18筆）.........................................................................................4-61
表4.4.6 b 非沙塵暴期間PM10氣膠化學組成、氣態空氣污染物及氣象資料之VARIMAX轉換因子分析結果總表（樣本數為20筆）.........................................................................................4-62
表4.4.7 a 沙塵暴期間PM2.5氣膠化學組成、氣態空氣污染物及氣象資料之VARIMAX轉換因子分析結果總表（樣本數為18筆）.........................................................................................4-63
表4.4.7 b 非沙塵暴期間PM2.5氣膠化學組成、氣態空氣污染物及氣象資料之VARIMAX轉換因子分析結果總表（樣本數為20筆）.........................................................................................4-64
表4.4.8 a 沙塵暴期間PM2.5-10氣膠化學組成、氣態空氣污染物及氣象資料之VARIMAX轉換因子分析結果總表（樣本數為18筆）.........................................................................................4-65
表4.4.8 b 非沙塵暴期間PM2.5-10氣膠化學組成、氣態空氣污染物及氣象資料之VARIMAX轉換因子分析結果總表（樣本數為20筆）....................................................................................4-66
表4.4.9 利用主成分因子分析法推估沙塵暴及非沙塵暴期間PM10、PM2.5及PM2.5-10氣膠之污染貢獻因子................................4-67
表4.4.10 a 氯離子損失法推估PM10氣膠海鹽成分計算過程……4-70
表4.4.10 b 氯離子損失法推估PM2.5氣膠海鹽成分計算過程……4-72
表4.4.10 c 氯離子損失法推估PM2.5-10氣膠海鹽成分計算過程…4-74
表4.4.11 a 氯離子損失法推估PM10氣膠中海鹽相關離子濃度……………………………………………………......….4-76
表4.4.11 b 氯離子損失法推估PM2.5氣膠中海鹽相關離子濃度………………………………………………………...…4-79
表4.4.11 c 氯離子損失法推估PM2.5-10氣膠中海鹽相關離子濃度…………………………………………………………...4-82
表4.4.12 a 利用氯損失法推估PM10氣膠的污染來源……………4-85
表4.4.12 b 利用氯損失法推估PM2.5氣膠的污染來源……………4-87
表4.4.12 c 利用氯損失法推估PM2.5-10氣膠的污染來源…………4-89
表4.4.13 a 2002年1/29-3/24中興大學測站PM10氣膠中氯損失百分比與[Ca2+]/[Na+]比值……………………………………...4-92
表4.4.13 b 2002年1/29-3/24中興大學測站PM2.5氣膠中氯損失百分比與[Ca2+]/[Na+]比值……………………………………...4-94
表4.4.13 c 2002年1/29-3/24中興大學測站PM2.5-10氣膠中氯損失百分比與[Ca2+]/[Na+]比值…………………………………...4-96
表4.5.1 沙塵暴及非沙塵暴期間酸性空氣污染物平均質量濃度………………………………………………………….4-101
表4.5.2 本研究酸性氣體採樣結果與國內量測結果比較............4-102
表4.5.3 本研究酸性氣體採樣結果與國外量測結果比較............4-103
圖 目 錄
圖3.1.1 環形擴散採樣器裝置..........................................................3-11
圖3.1.2 採樣點位置及其鄰近環境..................................................3-12
圖3.1.3 石英濾紙處理流程圖..........................................................3-13
圖3.1.4 水溶性陰陽離子分析流程圖..............................................3-14
圖4.1.1 中興大學測站（1）PM10氣膠質量濃度及（2）SO2氣體濃度觀測值與大里測站監測值比較圖.....................................4-2
圖4.1.2 中興大學測站（1）PM10氣膠質量濃度及（2）SO2氣體濃度觀測值與大里測站監測值之相關性.................................4-3
圖4.2.1 a 採樣期間環保署陽明及大里監測站PM10氣膠質量濃度逐時變化圖.................................................................................4-8
圖4.2.1 b 採樣期間環保署陽明及大里監測站CO氣體濃度逐時變化圖.............................................................................................4-9
圖4.2.2 採樣期間PM10、PM2.5及PM2.5-10氣膠質量濃度與粗細粒比逐日變化圖...........................................................................4-14
圖4.3.1 a 沙塵暴及非沙塵暴期間（1）PM10、（2）PM2.5及（3）PM2.5-10氣膠水溶性離子平均質量濃度比較...................................4-20
圖4.3.1 b 沙塵暴及非沙塵暴期間PM10、PM2.5及PM2.5-10氣膠水溶性離子平均質量百分比比較...............................................4-21
圖4.3.2 a 沙塵暴及非沙塵暴期間PM10氣膠水溶性離子含量圓餅圖...........................................................................................4-27
圖4.3.2 b 沙塵暴及非沙塵暴期間PM2.5氣膠水溶性離子含量圓餅圖...........................................................................................4-28
圖4.3.2 c沙塵暴及非沙塵暴期間PM2.5-10氣膠水溶性離子含量圓餅圖...........................................................................................4-29
圖4.3.3 a 採樣期間硝酸鹽微粒質量濃度與粗細粒比逐日變化圖...........................................................................................4-30
圖4.3.3 b 採樣期間硫酸鹽微粒質量濃度與粗細粒比逐日變化圖...........................................................................................4-30
圖4.3.3 c 採樣期間氯鹽微粒質量濃度與粗細粒比逐日變化圖....4-31
圖4.3.3 d 採樣期間鈉鹽微粒質量濃度與粗細粒比逐日變化圖...4-31
圖4.3.3 e 採樣期間銨鹽微粒質量濃度與粗細粒比逐日變化圖....4-32
圖4.3.3 f 採樣期間鉀鹽微粒質量濃度與粗細粒比逐日變化圖....4-32
圖4.3.3 g 採樣期間鎂鹽微粒質量濃度與粗細粒比逐日變化圖...4-33
圖4.3.3 h 採樣期間鈣鹽微粒質量濃度與粗細粒比逐日變化圖...4-33
圖4.3.4 (1)PM10、(2)PM2.5及(3)PM2.5-10氣膠中水溶性陰陽離子當量濃度平衡關係.......................................................................4-37
圖4.3.5 a 採樣期間PM10氣膠NR值及Ca2+微粒質量濃度逐日變化圖...........................................................................................4-38
圖4.3.5 b 採樣期間PM2.5氣膠NR值及Ca2+微粒質量濃度逐日變化圖...........................................................................................4-39
圖4.4.1 (a)PM10(b)PM2.5及(c)PM2.5-10氣膠中氯損失百分比與[Ca2+]/[Na+]比值之比較…………………………………...4-98
圖4.5.1 沙塵暴及非沙塵暴期間氣狀空氣污染物平均質量濃度比較.........................................................................................4-101

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