臺灣博碩士論文加值系統

本研究針對台南都會及沿海地區2002年1月及4月代表冬春兩季之PM2.5氣膠微粒水溶性離
子組成、含水率及酸鹼性，進行兩地冬春季氣膠不同特性、組成及其時空變異探討。
氣膠樣品在相對濕度40±5 %的調理下，台南都會與沿海地區冬春兩季PM2.5氣膠微粒水溶
性離子主要成份均為SO42-、NO3-、NH4+，在冬春兩季三物種合佔都會地區PM2.5質量濃度
的44.6 %及36.1 %，沿海地區則分別為44.6 %、38.0 %，顯示兩地之冬季二次氣膠組成對
PM2.5的貢獻均較春季為高。以PM2.5NR(Neutralization ratio)值計算，在都會地區冬季
之PM2.5氣膠呈中性；而春季之PM2.5氣膠呈鹼性。沿海地區酸鹼特性與都會地區氣膠相似
，冬季PM2.5 氣膠呈中性，而春季呈鹼性。其主因乃由於台南沿海地區以養殖漁業為主，
魚池內因高密度的養殖及大量曝氣，氨氮濃度及總氮量會隨魚體排泄物增加而增高。由都
會及沿海兩地之SOR(硫氧化比率)及NOR(氮氧化比率)發現，SOR高於0.4及NOR高於0.15時，
所代表光化反應相對強烈，其天氣狀態為相對溼度低且當時之O3濃度較SOR及NOR低時為高
。此外，SOR高時風速強烈，但NOR高時其風速較低，顯示硫物種藉較遠處傳輸氧化轉化成
氣膠硫酸鹽，但氮物種由氣態NO2轉化成氣膠NO3-，多為當地之交通污染滯留轉化。
此外，本研究成市堨窞RIFT光譜之氣膠微粒官能基負荷濃度校正，開發一套氣膠SO42-
、NO3-、NH4+含量快速且不具有破壞性之分析方法。由DRIFT光譜顯示SO42-吸收波數隨著
SO32-增減而改變，間接證實SO42-由SO2變成SO32-後再轉化為SO42-，此外，由DRIFT的快
速量測顯示南台灣二次氣膠其結合形態以(NH4)2SO4、NH4NO3、NH4HSO4為主。
台南都會及沿海之PM2.5氣膠含水率，在相對濕度60±2 % 控制下，其沿海地區日夜PM2.5
氣膠平均含水率分別為31.3±8.4 %、38.0±7.2 %，都會地區日夜PM2.5氣膠平均含水率分
別為25.7±16.9 %、24.3±21.5 %，顯示冬春兩季沿海地區PM2.5氣膠含水率均明顯高於都
會地區。而以日夜PM2.5氣膠含水率比較，除冬季日間都會氣膠含水率略高於夜間外，其沿
海冬春兩季及都會春季都會之氣膠含水率均以夜晚較高。以控制於相對濕度60±2 %之調理
環境測得氣膠含水量，其結果與Lee et al. (1998)的降濕模式所計算之含水量值尚有明顯
差異，應與未量測之水溶性有機碳的吸濕特性未能加以計算有關。

The chemical composition, water content, and acidity of atmospheric PM2.5
aerosols in a Tainan urban and coastal area were evaluated in January (winter)
and April (spring) of 2002.
Controlling relative humidity (RH) at 40±5 %, it was found that NH4+, SO4-2
and NO3- were the dominant water-soluble ionic species in both winter and
spring. These accounted for an average 44.6% and 36.1% of PM2.5 mass at the
urban site in winter and spring, respectively, and 44.6% and 38% at the
coastal site, demonstrating that secondary aerosols were a larger part of the
PM2.5 mass in winter at both sites. The average neutralization ratio (NR)
value of PM2.5 in the Tainan urban area was neutral (NR is 1.0±0.2) in
winter, and alkaline (NR is 2.5±0.4) in spring. The average value in the
Tainan coastal area was likewise neutral in winter and alkaline in spring. The
reason for this is that Tainan coastal areas are primarily agricultural and
aquafarm areas with high-density cultivation and high aeration, and hence high
levels of ammonium nitrate and total nitrogen, and aquatic animal wastes. It
was found that a SOR (sulfur oxidation ratio) value of >0.4 and a NOR (
nitrogen oxidation ratio) value of >0.15 represented a relatively strong
photochemical reaction, low relative humidity, and high O3 concentration.
Additionally, strong wind speeds led to a high SOR value, but weak wind speeds
led to a high NOR value. This demonstrates that the gaseous S species (SO2)
that form sulfate aerosols are transported from far away, whereas the N
species that form gaseous NO2 and subsequently NO3- are of local origin (due
to local traffic pollution emissions).
This study also succeeded in establishing DRIFT spectra for calibration of
aerosol functional group loading and a quick, nondestructive method to
determine NH4+, SO4-2 and NO3- content in PM2.5 aerosols. The DRIFT spectrum
showed SO4-2 absorptive wavelength changes followed by SO3-2 changes, and
indirectly proves that SO2 converts to SO3-2, which then converts to SO4-2. It
also shows that the main associated types of secondary aerosols in southern
Taiwan are (NH4)2SO4, NH4NO3 and NH4Cl.
The water content (mass concentration) of atmospheric PM2.5 aerosols
controlled at RH 60±2% was 31.3±8.4% and 38.0±7.2% at the coastal site in
the daytime and nighttime, respectively, and 25.76±16.9% and 24.3±21.5% at
the urban site. The water content was clearly higher in the coastal area in
both winter and spring. Apart from urban winter, when daytime water content
was slightly higher than nighttime, nighttime values were higher than daytime.
Controlling RH at 60±2%, the measured water content was clearly higher than
and different from values calculated using the water ascending model (Lee et
al., 1998). It may be that the water absorptive properties of soluble organic
carbons in aerosols are not taken into consideration in this model.

摘要 ………………………………………………………………　　　Ⅰ
Abstract ……………………………………………………………… Ⅲ
誌謝 ……………………………………………………………… Ⅴ
目錄 ………………………………………………………………. Ⅶ
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 大氣氣膠微粒之成份……………………………….…. 3
2-2 氣膠微粒之酸鹼性……………………………….……. 5
2-3 大氣氣膠水溶性無機鹽類之FTIR量測…………….…… 5
2-4 氣膠含水量……………………………………….…... 7
第三章 實驗與研究方法………………………………….….... 10
3-1 PM2.5氣膠之採樣規劃與測站之選擇…………….….…. 10
3-2 採樣量測方法…………………………………….…... 12
3-2-1 採樣原理及設備………………………………….….... 12
3-2-2 氣象資料之建立………………………………….….... 14
3-3 樣品分析方法………………………………….…..….. 15
3-3-1 採樣前樣品之調理…………………………….…..…... 16
3-3-2 PM2.5微粒氣膠化學成分及酸鹼度之測定…….…..….……. 16
3-3-3 PM2.5微粒氣膠的散射反射式傅立葉轉換紅外線光譜測定. 18
3-3-4 PM2.5氣膠含水率分析……………………….…..….…. 20
3-4 單一鹽類硫酸銨潮解及再結晶特性……….…..….……. 30
第四章 大氣氣膠酸鹼特性及時空變異…………………………….. 35
4-1 都會地區和沿海地區PM2.5氣膠之特性……….….………..　35
4-1-1 都會地區PM2.5氣膠之特性..….….………………………… 35
4-1-2 沿海地區PM2.5氣膠之特性..….….………………………… 38
4-1-3 都會及沿海大氣氣膠離子組成之差異…………………….. 41
4-2 大氣氣膠之日夜特性差異..….….………………………….. 42
4-2-1 都會地區之大氣氣膠日夜特性……..….…………….…….. 42
4-2-2 沿海地區之大氣氣膠日夜特性……..….…………….…….. 44
4-2-3 兩地氣膠日夜變化特性比較….……………………………. 46
4-3 大氣氣膠微粒之酸鹼性….…………………………………. 47
4-3-1 都會地區大氣氣膠微粒之酸鹼性………………………….. 47
4-3-2 沿海地區大氣氣膠微粒之酸鹼性………………………….. 47
4-4 台南都會及沿海地區硫轉化率和氮轉化率之比較….……. 50
4-5 兩地氣膠微粒酸鹼特性之比較.……………………………. 56
第五章 大氣氣膠離子組成的DRIFTS測定……………………….. 62
5-1 氣膠微粒不同粒徑之化學組成在紅外線光譜上之表現….. 62
5-2 DRIFTS檢量線之建立……………………………………… 74
5-3 氣膠微粒之衰變…………………………………………….. 76
5-4 大氣氣膠之結合形態……………………………………….. 77
第六章 PM2.5氣膠含水量分析……..……..…………………………. 80
6-1 GC-TCD和Karl Fischer 電位儀測定之比較……………… 80
6-2 硫酸銨的潮解再結晶……………………………………….. 81
6-3 台南都會及沿海氣膠含水量之量測分析………………….. 83
6-3-1 冬季都會和沿海PM2.5氣膠含水量之變異………………… 87
6-3-2 春季都會和沿海PM2.5氣膠含水量之變異………………… 88
6-4 在相對濕度60 %時之PM2.5氣膠組成……………………... 89
第七章 結論………………………………………………………….. 92
第八章 參考文獻…………………………………………………….. 95
Table List
Table 4.1 Mean(±SD)chemical composition(mg m-3)of PM2.5aerosols for Tainan
urban area, January and April 2002.(number of samples = 59)……………..…………
………………………….……………..36
Table 4.2 Correlation matrix of chemical composition in PM2.5 aerosols for
Tainan urban area, January 2002. (number of samples = 29)….…..37
Table 4.3 Correlation matrix of chemical composition in PM2.5 aerosols for
Tainan urban area, April 2002. (number of samples = 30)…….…..38
Table 4.4 Mean (±SD) chemical composition (mg m-3) of PM2.5 aerosols and
meteorological parameters for Tainan coastal area, January and April 2002. (
number of samples = 59)………………………….………..39
Table 4.5 Correlation matrix of chemical composition in PM2.5 aerosols for
Tainan coastal area, January 2002. (number of samples = 30)….….40
Table 4.6 Correlation matrix of chemical composition in PM2.5 aerosols for
Tainan coastal areas, April 2002. (number of samples = 29)…...…41
Table 4.7 Comparison of SOR values which is more than 0.4 or less than 0.15 in
various meteorological condition, O3 concentration, and NSS-SO42-/ PM2.5 mass
ratio in Tainan urban and coastal areas in January and April, 2002………………
…………………………….54
Table 4.8 Comparison of　NOR values which is more than 0.4 or less than 0.15
in various meteorological condition, O3 concentration, and NO3-/ PM2.5 mass
ratio in Tainan urban and coastal areas in January and April, 2002………………
………………….………...…………….55
Table 4.9 Comparison of dominant species for aerosol in various areas……..59
Table 4.10 Comparison of acidity particulate aerosol in various areas………...
60
Table 4.11 Comparison of sulfur and nitrogen oxidation ratios in various
areas, Taiwan………………………………………………………………61
Table 5.1 Inorganic and organic absorbances observed in spectra of ambient
aerosol…………..…………………………………………………..64
Table 6.1 Comparison of water measured by GC-TCD and Karl Fischer methods………
……………………………………………………..80
Table 6.2 Comparison of measured PM2.5 aerosol water at Tainan and by Lee et
al.(1998) aerosol water of descending RH process.……………….84
Table 6.3 Correlation matrix of measured H2O, theoretical H2O, PM2.5 mass, and
measured chemical compositions in PM2.5 aerosols for Tainan urban and coastal
area, January 2002. (number of samples = 59 )……………………………………………
…………………….85
Table 6.4 Correlation matrix of measured H2O, theoretical H2O, PM2.5 mass, and
measured chemical compositions in PM2.5 aerosols for Tainan urban and coastal
area, April 2002. (number of samples =59)…..…86
Figure List
Fig. 3.1 Relative position of air quality monitoring stations at urban and
coastal area in Tainan………………………………………………………….11
Fig. 3.2 MSP, micro-orifice uniform deposit impactor, MOUDITM model 110..13
Fig. 3.3 Measuremental program for chemical compositions and water contents of
ambient PM2.5………………………………………………………15
Fig. 3.4 Diffuse reflectance set on FTIR apparatus……………………………19
Fig. 3.5 Schematic diagram of the experimental setup for aerosol water mass
measurement…………………………………………………………..25
Fig. 3.6 Tests for water adsorpted on glass vessels at RH of 60±2 % during
various exposed duration……………………………………………...26
Fig. 3.7 Tests for water adsorpted on filters……………………...…………….27
Fig. 3.8 Comparison of extraction water amount for various shaking and non-
shaking time……………………………………………………...28
Fig. 3.9 Comparison of extracted water amount by various methanol amount,
extraction type and duration.…………………………………………….29
Fig. 4.1 Mean (±SD) chemical composition (%) of PM2.5 aerosols in Tainan
urban area, January and April 2002 (number of samples = 59 ). (a) Daytime in
winter; (b) Nighttime in winter; (c) Daytime in spring; (d) Nighttime in spring
……………………………………………………43
Fig. 4.2 Mean (±SD) chemical composition (%) of PM2.5 aerosols in Tainan
coastal area, January and April 2002 (number of samples = 59). (a) Daytime in
winter; (b) Nighttime in winter; (c) Daytime in spring; (d) Nighttime in
spring …………………………………………………...45
Fig. 4.3 Concentration equivalent ratio of NH4+ to sum of excess SO42- and
NO3- for Tainan urban PM2.5 aerosols. (a) Daytime in winter; (b) Nighttime in
winter; (c) Daytime in spring; (d) Nighttime in spring……………….48
Fig. 4.4 Concentration equivalent ratio of NH4+ to sum of excess SO42- and
NO3- for Tainan cosastal PM2.5 aerosols (a) Daytime in winter; (b) Nighttime
in winter; (c) Daytime in spring; (d) Nighttime in spring……..……...49
Fig. 4.5 Various sulfur oxidation and nitrogen oxidation ratio in Tainan urban
area(a) Daytime in winter; (b) Nighttime in winter; (c) Daytime in spring; (d)
Nighttime in spring…….,.………………………………...51
Fig. 4.6 Various sulfur oxidation and nitrogen oxidation ratio in Tainan
coastal area(a) Daytime in winter; (b) Nighttime in winter; (c) Daytime in
spring; (d) Nighttime in spring…………...…………………………...52
Fig. 5.1 Typical FTIR spectra of ambient Tainan aerosol taken at chungsan high
school. (1/23/2002)……………………………………………………63
Fig. 5.2 FTIR spectra of ambient aerosol of 0.056 mm in Tainan urban area. (
taken on 1/23/2002)…………………………………………………..65
Fig. 5.3 FTIR spectra of ambient aerosol of 10 mm in Tainan urban area. (taken
on 1/23/2002)………………………………………………………….66
Fig. 5.4 FTIR spectra of ambient aerosol of 0.32 mm in Tainan urban area. (
taken on 1/23/2002)…………………………………………………..67
Fig. 5.5 FTIR spectra of ambient aerosol of 0.56 mm in Tainan urban area. (
taken on 1/23/2002)…………………………………………………..68
Fig. 5.6 FTIR spectra of ambient aerosol of 1.8 mm in Tainan urban area. (
taken on 1/23/2002)………………………………………………………….69
Fig. 5.7 FTIR spectra of chemical species in different diameters in Tainan
urban area. (a)diameter : 0.56 mm; (B)diameter : 1.0 mm; (C)diameter : 1.8 mm (
taken on 1/23/2002)…………………………………………………..72
Fig. 5.8 FTIR spectra of chemical species in different diameters in Tainan
urban area. (a)diameter : 0.056 mm; (b) diameter : 0.1 mm; (c) diameter : 0.18
mm; (d) diameter : 0.32 mm. (taken on 1/23/2002)……………………73
Fig. 5.9 Absorption intensity of aerosol SO42- and SO32-in different diameter
ranges………………………………………………………………….74
Fig. 5.10 Linear relationship between species concentration measured by IC and
absorption intensity measured by FTIR……………………………….75
Fig. 5.11 Ammonium and Sulfate decay in aerosol measured by FTIR………...77
Fig. 5.12 Size distributions of major chemical species in Tainan urban aerosol
in January and April 2002………………………………………………..79
Fig. 6.1 Humidograph of (NH4)2SO4 measured by GC-TCD in the ascending RH and
descending RH cycles at 25±1°C…………………………….…...82
Fig. 6.2 Humidograph of (NH4)2SO4 measured by Karl Fischer in the ascending RH
and descending RH cycles at 25±1°C…………….………………82
Fig. 6.3 Aerosol water in Taiwan urban and coastal areas, variations of
January 2002…………………………………………………………………...88
Fig. 6.4 Aerosol water in Taiwan urban and coastal areas, variations of April
2002…………………………………………………………………...89
Fig. 6.5 Mean chemical composition of PM2.5, Which was conditioned at 60±2%
relative humidity, in Tainan urban and coastal areas during January and April
2002………………………………………………..91

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