A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles

被引：6

作者：

Zhu, Qindan ^{[1
,2
,15
]}

Schwantes, Rebecca H. ^{[1
]}

Coggon, Matthew ^{[1
]}

Harkins, Colin ^{[1
,2
]}

Schnell, Jordan ^{[2
]}

He, Jian ^{[1
,2
]}

Pye, Havala O. T. ^{[3
]}

Li, Meng ^{[2
]}

Baker, Barry ^{[13
]}

Moon, Zachary ^{[13
,14
]}

Ahmadov, Ravan ^{[4
]}

Pfannerstill, Eva Y. ^{[5
,18
]}

Place, Bryan ^{[3
]}

Wooldridge, Paul ^{[6
]}

Schulze, Benjamin C. ^{[7
]}

Arata, Caleb ^{[8
]}

Bucholtz, Anthony ^{[9
]}

Seinfeld, John H. ^{[10
]}

Warneke, Carsten ^{[1
]}

Stockwell, Chelsea E. ^{[1
]}

Xu, Lu ^{[1
,2
,17
]}

Zuraski, Kristen ^{[1
,2
]}

Robinson, Michael A. ^{[1
,2
]}

Neuman, J. Andrew ^{[1
]}

Veres, Patrick R. ^{[1
,16
]}

Peischl, Jeff ^{[1
,2
]}

Brown, Steven S. ^{[1
,11
]}

Goldstein, Allen H. ^{[5
,8
]}

Cohen, Ronald C. ^{[6
,12
]}

McDonald, Brian C. ^{[1
]}

机构：

[1] Chem Sci Lab, NOAA, Boulder, CO 80305 USA

[2] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA

[3] US EPA, Off Res & Dev, Res Triangle Pk, NC 27711 USA

[4] Global Syst Lab, NOAA, Boulder, CO 80305 USA

[5] Univ Calif Berkeley, Dept Environm Sci Policy & Management, Berkeley, CA 94720 USA

[6] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[7] CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91125 USA

[8] Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USA

[9] Naval Postgrad Sch, Dept Meteorol, Monterey, CA 93943 USA

[10] CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91125 USA

[11] Univ Colorado, Dept Chem, Boulder, CO 80309 USA

[12] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA

[13] NOAA, Air Resources Lab, College Pk, MD 20740 USA

[14] Earth Resources Technol ERT Inc, Laurel, MD 20707 USA

[15] MIT, Dept Earth Atmospher & Planetary Sci, Cambridge, MA 02319 USA

[16] Natl Ctr Atmospher Res, Res Aviat Facil, Boulder, CO 80301 USA

[17] Washington Univ, Dept Energy Environm & Chem Engn, St Louis, MI 63130 USA

[18] Forschungszentrum Julich, Inst Energy Climate Res 8 Troposphere, D-52425 Julich, Germany

来源：

ATMOSPHERIC CHEMISTRY AND PHYSICS | 2024年 / 24卷 / 09期

关键词：

MONOTERPENE EMISSIONS; NITRATE CHEMISTRY; AIR-QUALITY; ISOPRENE; MODEL; GAS; AEROSOL; MECHANISM; HYDROLYSIS; PRODUCTS;

D O I：

10.5194/acp-24-5265-2024

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

The declining trend in vehicle emissions has underscored the growing significance of volatile organic compound (VOC) emissions from volatile chemical products (VCPs). However, accurately representing VOC chemistry in simplified chemical mechanisms remains challenging due to its chemical complexity including speciation and reactivity. Previous studies have predominantly focused on VOCs from fossil fuel sources, leading to an underrepresentation of VOC chemistry from VCP sources. We developed an integrated chemical mechanism, RACM2B-VCP, that is compatible with WRF-Chem and is aimed at enhancing the representation of VOC chemistry, particularly from VCP sources, within the present urban environment. Evaluation against the Air Quality System (AQS) network data demonstrates that our model configured with RACM2B-VCP reproduces both the magnitude and spatial variability of O 3 and PM 2.5 in Los Angeles. Furthermore, evaluation against comprehensive measurements of O 3 and PM 2.5 precursors from the Reevaluating the Chemistry of Air Pollutants in California (RECAP-CA) airborne campaign and the Southwest Urban NO x and VOC Experiment (SUNVEx) ground site and mobile laboratory campaign confirm the model's accuracy in representing NO x and many VOCs and highlight remaining biases. Although there exists an underprediction in the total VOC reactivity of observed VOC species, our model with RACM2B-VCP exhibits good agreement for VOC markers emitted from different sectors, including biogenic, fossil fuel, and VCP sources. Through sensitivity analyses, we probe the contributions of VCP and fossil fuel emissions to total VOC reactivity and O 3 . Our results reveal that 52 % of the VOC reactivity and 35 % of the local enhancement of MDA8 O 3 arise from anthropogenic VOC emissions in Los Angeles. Significantly, over 50 % of this anthropogenic fraction of either VOC reactivity or O 3 is attributed to VCP emissions. The RACM2B-VCP mechanism created, described, and evaluated in this work is ideally suited for accurately representing ozone for the right reasons in the present urban environment where mobile, biogenic, and VCP VOCs are all important contributors to ozone formation.

引用

页码：5265 / 5286

页数：22

共 93 条

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