Sources and characteristics of summertime organic aerosol in the Colorado Front Range: perspective from measurements and WRF-Chem modeling

被引：12

作者：

Bahreini, Roya ^{[1
,2
]}

Ahmadov, Ravan ^{[3
,4
]}

McKeen, Stu A. ^{[3
,4
]}

Vu, Kennedy T. ^{[2
]}

Dingle, Justin H. ^{[2
]}

Apel, Eric C. ^{[5
]}

Blake, Donald R. ^{[6
]}

Blake, Nicola ^{[6
]}

Campos, Teresa L. ^{[5
]}

Cantrell, Chris ^{[7
]}

Flocke, Frank ^{[5
]}

Fried, Alan ^{[8
]}

Gilman, Jessica B. ^{[3
]}

Hills, Alan J. ^{[5
]}

Hornbrook, Rebecca S. ^{[5
]}

Huey, Greg ^{[9
]}

Kaser, Lisa ^{[5
]}

Lerner, Brian M. ^{[3
,4
,10
]}

Mauldin, Roy L. ^{[7
]}

Meinardi, Simone ^{[6
]}

Montzka, Denise D. ^{[5
]}

Richter, Dirk ^{[8
]}

Schroeder, Jason R. ^{[6
,11
]}

Stell, Meghan ^{[5
]}

Tanner, David ^{[9
]}

Walega, James ^{[8
]}

Weibring, Peter ^{[8
]}

Weinheimer, Andrew ^{[5
]}

机构：

[1] Univ Calif Riverside, Dept Environm Sci, Riverside, CA 92521 USA

[2] Univ Calif Riverside, Environm Toxicol Grad Program, Riverside, CA 92521 USA

[3] NOAA, Earth Syst Res Lab, Boulder, CO 80305 USA

[4] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80301 USA

[5] Natl Ctr Atmospher Res, Atmospher Chem Observat & Modeling Lab, Boulder, CO 80301 USA

[6] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA

[7] Univ Colorado, Dept Atmospher & Ocean Sci, Boulder, CO 80303 USA

[8] Univ Colorado, Inst Arctic & Alpine Res, Boulder, CO 80303 USA

[9] Georgia Inst Technol, Dept Earth & Atmospher Sci, Atlanta, GA 30033 USA

[10] Aerodyne Res Inc, Billerica, MA 01821 USA

[11] NASA, Langley Res Ctr, Newport News, VA 23666 USA

来源：

ATMOSPHERIC CHEMISTRY AND PHYSICS | 2018年 / 18卷 / 11期

关键词：

POSITIVE MATRIX FACTORIZATION; MASS-SPECTROMETER; AIR-QUALITY; UINTAH BASIN; COMPOUND EMISSIONS; OZONE POLLUTION; LOS-ANGELES; US OIL; GAS; PHOTOOXIDATION;

D O I：

10.5194/acp-18-8293-2018

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

The evolution of organic aerosols (OAs) and their precursors in the boundary layer (BL) of the Colorado Front Range during the Front Range Air Pollution and Photochemistry Experiment (FRAPPE, July-August 2014) was analyzed by in situ measurements and chemical transport modeling. Measurements indicated significant production of secondary OA (SOA), with enhancement ratio of OA with respect to carbon monoxide (CO) reaching 0.085 +/- 0.003 mu gm(-3) ppbv(-1). At background mixing ratios of CO, up to similar to 1.8 mu gm(-3) background OA was observed, suggesting significant non-combustion contribution to OA in the Front Range. The mean concentration of OA in plumes with a high influence of oil and natural gas (O&G) emissions was similar to 40% higher than in urban-influenced plumes. Positive matrix factorization (PMF) confirmed a dominant contribution of secondary, oxygenated OA (OOA) in the boundary layer instead of fresh, hydrocarbon-like OA (HOA). Combinations of primary OA (POA) volatility assumptions, aging of semi-volatile species, and different emission estimates from the O&G sector were used in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) simulation scenarios. The assumption of semi-volatile POA resulted in greater than a factor of 10 lower POA concentrations compared to PMF-resolved HOA. Including top-down modified O&G emissions resulted in substantially better agreements in modeled ethane, toluene, hydroxyl radical, and ozone compared to measurements in the high-O&G-influenced plumes. By including emissions from the O&G sector using the top-down approach, it was estimated that the O&G sector contributed to < 5% of total OA, but up to 38% of anthropogenic SOA (aSOA) in the region. The best agreement between the measured and simulated median OA was achieved by limiting the extent of biogenic hydrocarbon aging and consequently biogenic SOA (bSOA) production. Despite a lower production of bSOA in this scenario, contribution of bSOA to total SOA remained high at 40-54 %. Future studies aiming at a better emissions characterization of POA and intermediate-volatility organic compounds (IVOCs) from the O&G sector are valuable.

引用

页码：8293 / 8312

页数：20

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