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1 理 逸 1 易 異 逸 參 來 料 量 不 類 度 異 SO42->NO3 SO42->NH4+ NO3- 度 量 PM2.5 PM10 量 粒 量 度 0.8 1% 量 量 oxalic acid 量 PM2.5 PM10 oxalic acid 例 69 % % 數 裂 (C2) oxalic acid 參 料 度 Abstract Dicarboxylic acids are ubiquitous in the troposphere and one of important organic matters, resulting from marine pathway, fossil fuel burning, biomass burning, cooking, forest biosource and anthropogenic emissions. This study focused on the concentration variations of water-soluble inorganic species and dicarboxylic acids in aerosol during different air quality -periods. The results reveal the concentration of SO42-always exceeded contents of NO3 and NH4+ within both fine and coarse fractions. However, the increase of NO3-, presenting the traffic emission, was significant during the period of episode. The percentage contribution of dicarboxylic acids in both PM2.5 and PM10 was % by mass. Oxalic acid was the biggest single dicarboxylic acids. During the episode, the transformation percentage of dicarboxylic acids in

2 both PM2.5 and PM10 increased significantly. The percent of oxalic acid in measured dicarboxylic acids raised from 69 % during non-episode to be % during episode, indicating the more carbon-bonding dicarboxylic acids decomposed to be 2 carbon-bonding products, oxalic acid during the period of episode. These results can offer the estimation for air quality model application. Keywords: fossil fuel burning, oxalic acid, malonic acid, succinic acids, diurnal variations. (Chebbi and Carlier, 1996) 來 料 量 類 (Kalberer et al., 2000) 料 succinic(c4) malonic(c3) oxalic(c2) 不 數 (Hatakeyama et al., 1987) 來 不 O3 2 9 不 (Kawamura et al., 1996) 都 都 量 1-3 % 10 % 不 量 異 (Khwaja,1995 Kawamura and Sakaguchi, 1999) 量 3-8 % (Wang et al., 2002) (oxalate) (malonate) succinate) (Kawamura et al., 1996) 度 ng m-3 都 900 ng m-3 度 (Kawamura and Sakaguchi, 1999) PM2.5 PM 類 度 都 理 樓 離 度 15 離 1 省 500 度 / 離 (Versatile Air Pollutant Sampler, VAPS, URG-3000K) PM PM2.5 粒 流量 2.0 Lpm (PM2.5-10) 15.0 Lpm (PM2.5) 理

3 粒濾 量 Metler AT261 Delta 5 數 Sartorius CP2P 6 數 量 粒濾 4 oc 冷 粒 易 離 漏 離 粒 濾 PE 10.0 ml (Yihder TS-500) m 濾 濾 立 濾 gradient pump (Dionex GP50) IC (Dionex DX-600) 行 AS mm ID anion suppression system (ASRS-ultra) 流 NaOH MeOH 量 1000 L succinic acid malic acid malonic acid tartric acid maleic acid oxalic acid 六 量 Tabe 1 流 濾 離 F-, Br-, NO2-, NO3-, SO42-, Cl-, Na+, NH4+, K+, Ca2+, Mg2+ (Tsai and Kuo, 2005) 濾 利 Ion Pac CS12A CG12A ( 4 mm) 流 20 mm MSA 流 0.5 ml/min 離 論 3.1 PM2.5 PM10 量 度 1 2 PM10 粒 ( 1) 量 類 例 SO42- NO3- NH4+ 類 PM2.5 粒 量 3.2 量 度 1% 量 oxalic acid 量 succinic acid malonic acid PM10 粒 ( 2) 類 (SO42- NO3- NH4+) 度 PM10 NO3- 度 PM2.5 NO3- 度 PM10 PM2.5 SO42 度 例 降 度 量 3.3 論 PM10 PM2.5 Mg2+ Ca2+ 例 降 異 Mg2+ Ca2+ 來 量 度 Mg2+ Ca2+ 量 度

4 例 降 Cl- K+ NH4+ PM10 量 度 例 例 度 數 0.8 來 露 粒 3.4 PM10 量 略 PM2.5 粒 六 量 PM2.5 量 度 例 ( %) 略 六 量 PM10 粒 量 例 ( %) oxalic acid 例 69 % oxalic acid 量 降 量 PM10 量 度 例 ( %) 略 降 量 例 malic acid maleic acid oxalic acid 例都 oxalic acid 73 % 69% PM2.5 oxalic acid 例 69 % 80% Oxalic acid 來 了 都 量 oxalic acid PM2.5 量 oxalic acid succinic acid malonic acid 11 % 兩 22 % 例 異 量 裂 oxalic acid 度 m 度 m 累 論 PM2.5 PM 類 論 SO42->NO3- SO42->NH4+ PM10 NO3- 度 PM2.5 NO3- 度 度 量 PM2.5 PM10 量 粒 量 度 0.8 1% 量 量 oxalic acid 量 succinic acid malonic acid oxalic acid succinic acid malonic acid 裂 歷 (C4) (C3) (C2) oxalic acid 度 異

5 參 參 1. Chebbi, A., Carlier, P., Carboxylic acids in the troposphere, occurrence, sources, and sinks: a review. Atmospheric Environment 30, Hatakeyama, S., Ohno, M., Weng, J., Takagi, H., Akimoto, H., Identification of C2 C10 ω-oxocarboxylic acids, pyruvic acid and C2 C3 α -dicarbonyls. Environmental Science and Technology 21, alberer, M., Yu, J., Cocker, R.G., Flagan, R.C., Seinfeld, J.H., Aerosol formation in the cyclohexene-ozone system. Environmental Science and Technology 34, Kawamura, K., Kasukabe, H., Barrie, L.A., Source and reaction pathways of dicarboxylic acids, ketoacids and dicarbonyls in Arctic aerosols: one year of observations. Atmospheric Environment 30, Kawamura, K., Sakaguchi, F., Molecular distributions of water soluble dicarboxylic acids in marine aerosols over the Pacific Ocean including tropics. Journal of Geophysical Research 104, Khwaja, H.A., Atmospheric Concentrations of Carboxylic Acids and Related Compounds at a Semiurban Site. Atmospheric Environment 29, Wang, G., Niu, S., Liu, C., Wang, L., Identification of dicarboxylic acids and aldehydes of PM10 and PM2.5 aerosols in Nanjing, China. Atmospheric Environment 36, PM10 mass concentration: 95.2±26.9 µg m-3 1. PM10 PM10 mass concentration: 110.8±24.9 µg m-3 2. PM10 Sodium (4.40±3.22)% Others (40.95±16.48)%Sulfate (16.67±9.33)% Dicarboxylic acid (0.86±0.42)% Nitrate (10.29±5.36)% Bromine (0.92±1.03)% Nitrite (2.16±3.51)% Chloride (4.42±1.83)% Fluorine (1.30±1.26)% Calcium (3.01±0.80)% Ammonium (9.42±3.18)% Potassium (3.25±1.26)% Magnesium (2.37±0.83)% Oxalic acid (69.21±39.60)% Maleic acid (2.23±1.97)% Tartaric acid (0.76±0.81)% Malonic acid (10.03±5.39)% Malic acid (5.95±3.32)% Succinic acid (11.81±6.77)% Oxalic acid (72.66±26.18)% Maleic acid (4.56±3.33)% Tartaric acid (0.541±0.66)% Malonic acid (8.69±3.39)% Malic acid (6.18±2.46)% Succinic acid (7.373±2.98)% Sodium

6 (4.73±1.08)% Others (42.62±14.75)% Sulfate (13.55±4.39)% Dicarboxylic acid (0.82±0.27)% Nitrate (12.09±8.04)% Bromine (0.68±0.84)% Nitrite (1.14±0.75)% Chloride (5.84±1.25)% Fluorine (0.93±1.08)% Calcium (2.47±0.83)% Ammonium (9.56±3.37)% Potassium (3.28±0.99)%Magnesium (2.29±0.27)% PM2.5 mass concentration: 56.2±16.2 µg m-3 3. PM2.5 PM2.5 mass concentration: 72.9±15.5 µg m-3 4. PM2.5 Sodium (2.68±3.87)% Others (49.16±20.27)% Sulfate (18.33±11.30)% Dicarboxylic acid (1.00±0.48)% Nitrate (9.96±6.41)% Bromine (0.15±0.21)% Nitrite (1.62±4.22)% Chloride (3.00±2.09)% Fluorine (0.09±0.12)% Calcium (1.16±0.30)% Ammonium (10.14±3.81)% Potassium (2.45±1.53)% Magnesium (0.28±0.10)% Succinic acid (11.80±6.85)% Malic acid (5.90±3.35)% Malonic acid (9.92±5.45)% Tartaric acid (0.70±0.81)% Maleic acid (2.15±2.03)% Oxalic acid (69.53±39.84)% Sodium (2.18±0.68)% Others 4.75±13.60)% Sulfate (15.44±6.34)% Dicarboxylic acid (1.01±0.59)% Nitrate (11.55±6.43)% Bromine (0.04±0.08)% Nitrite (0.24±0.17)% Chloride (3.20±1.45)% Fluorine (0.05±0.09)% Calcium (0.54±0.15)% Ammonium (9.17±3.12)% Potassium 1.33±0.90)% Magnesium (0.17±0.07)% Succinic acid (6.78±2.78)% Malic acid (4.69±2.64)% Malonic acid (5.44±1.86)%Tartaric acid (0.52±0.64)% Maleic acid (2.91±2.92)% Oxalic acid (79.66±54.27)%