GSTDTAP  > 地球科学
DOI10.5194/acp-19-9641-2019
Seasonal differences in formation processes of oxidized organic aerosol near Houston, TX
Dai, Qili1,2; Schulze, Benjamin C.2,5; Bi, Xiaohui1,2; Bui, Alexander A. T.2; Guo, Fangzhou2; Wallace, Henry W.2,6; Sanchez, Nancy P.2; Flynn, James H.3; Lefer, Barry L.3,7; Feng, Yinchang1; Griffin, Robert J.2,4
2019-07-31
发表期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN1680-7316
EISSN1680-7324
出版年2019
卷号19期号:14页码:9641-9661
文章类型Article
语种英语
国家Peoples R China; USA
英文摘要

Submicron aerosol was measured to the southwest of Houston, Texas, during winter and summer 2014 to investigate its seasonal variability. Data from a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) indicated that organic aerosol (OA) was the largest component of nonrefractory submicron particulate matter (NR-PM1) (on average, 38 % +/- 13 % and 47 % +/- 18 % of the NR-PM1 mass loading in winter and summer, respectively). Positive matrix factorization (PMF) analysis of the OA mass spectra demonstrated that two classes of oxygenated OA (less- and more-oxidized OOA, LO and MO) together dominated OA mass in summer (77 %) and accounted for 39 % of OA mass in winter. The fraction of LO-OOA (out of total OOA) is higher in summer (70 %) than in winter (44 %). Secondary aerosols (sulfate + nitrate + ammonium + OOA) accounted for similar to 76 % and 88 % of NR-PM1 mass in winter and summer, respectively, indicating NR-PM1 mass was driven mostly by secondary aerosol formation regardless of the season. The mass loadings and diurnal patterns of these secondary aerosols show a clear winter-summer contrast. Organic nitrate (ON) concentrations were estimated using the NOx+ ratio method, with contributions of 31 %-66 % and 9 %-17 % to OA during winter and summer, respectively. The estimated ON in summer strongly correlated with LO-OOA (r = 0.73) and was enhanced at nighttime.


The relative importance of aqueous-phase chemistry and photochemistry in processing OOA was investigated by examining the relationship of aerosol liquid water content (LWC) and the sum of ozone (O-3) and nitrogen dioxide (NO2) (O-x = O-3 + NO2) with LO-OOA and MO-OOA. The processing mechanism of LO-OOA apparently was related to relative humidity (RH). In periods of RH < 80 %, aqueous-phase chemistry likely played an important role in the formation of wintertime LO-OOA, whereas photochemistry promoted the formation of summertime LO-OOA. For periods of high RH > 80 %, these effects were opposite those of low-RH periods. Both photochemistry and aqueous-phase processing appear to facilitate increases in MO-OOA concentration except during periods of high LWC, which is likely a result of wet removal during periods of light rain or a negative impact on its formation rate.


The nighttime increases in MO-OOA during winter and summer were 0.013 and 0.01 mu g MO-OOA per mu g of LWC, respectively. The increase in LO-OOA was larger than that for MO-OOA, with increase rates of 0.033 and 0.055 mu g LO-OOA per mu g of LWC at night during winter and summer, respectively. On average, the mass concentration of LO-OOA in summer was elevated by nearly 1.20 mu g m(-3) for a similar to 20 mu g change in LWC, which was accompanied by a 40 ppb change in O-x.


领域地球科学
收录类别SCI-E
WOS记录号WOS:000477971700003
WOS关键词POSITIVE MATRIX FACTORIZATION ; HIGH-RESOLUTION ; MASS-SPECTROMETRY ; PARTICULATE MATTER ; HYGROSCOPIC GROWTH ; SUBMICRON AEROSOLS ; BOUNDARY-LAYER ; IN-SITU ; SECONDARY ; FIELD
WOS类目Environmental Sciences ; Meteorology & Atmospheric Sciences
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/185359
专题地球科学
作者单位1.Nankai Univ, Coll Environm Sci & Engn, State Environm Protect Key Lab Urban Ambient Air, Tianjin 300350, Peoples R China;
2.Rice Univ, Dept Civil & Environm Engn, Houston, TX 77005 USA;
3.Univ Houston, Dept Earth & Atmospher Sci, Houston, TX 77004 USA;
4.Rice Univ, Dept Chem & Biomol Engn, Houston, TX 77005 USA;
5.CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91125 USA;
6.Washington State Dept Ecol, Lacey, WA 98503 USA;
7.NASA, Div Tropospher Composit, Washington, DC 20024 USA
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Dai, Qili,Schulze, Benjamin C.,Bi, Xiaohui,et al. Seasonal differences in formation processes of oxidized organic aerosol near Houston, TX[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(14):9641-9661.
APA Dai, Qili.,Schulze, Benjamin C..,Bi, Xiaohui.,Bui, Alexander A. T..,Guo, Fangzhou.,...&Griffin, Robert J..(2019).Seasonal differences in formation processes of oxidized organic aerosol near Houston, TX.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(14),9641-9661.
MLA Dai, Qili,et al."Seasonal differences in formation processes of oxidized organic aerosol near Houston, TX".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.14(2019):9641-9661.
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