New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling
-
Published:2023-06-17
Issue:1
Volume:6
Page:
-
ISSN:2397-3722
-
Container-title:npj Climate and Atmospheric Science
-
language:en
-
Short-container-title:npj Clim Atmos Sci
Author:
Zhang Jie, Liu Junyi, Ding Xiang, He Xiao, Zhang TianleORCID, Zheng Mei, Choi Minsu, Isaacman-VanWertz Gabriel, Yee LindsayORCID, Zhang Haofei, Misztal Pawel, Goldstein Allen H.ORCID, Guenther Alex B.ORCID, Budisulistiorini Sri Hapsari, Surratt Jason D.ORCID, Stone Elizabeth A., Shrivastava ManishORCID, Wu Dui, Yu Jian ZhenORCID, Ying Qi
Abstract
AbstractParticulate 2-methyltetrols (2-MT) and 2-methylglyceric acid (2-MG) are typically used to indicate the abundance of isoprene-derived secondary organic aerosols (SOA). However, their formation and fate are not fully understood. In this study, we showed that particulate 2-MT and 2-MG collected at multiple monitoring sites under a wide range of atmospheric and emission conditions, with concentrations spanning six orders of magnitudes, are well reproduced with an expanded isoprene-SOA scheme implemented into the Community Multiscale Air Quality (CMAQ) model. The scheme considers their three-phase (gas-aqueous-organic phase) partitioning, formation from acid-driven multiphase reactions, and degradation by OH radicals in the gas and aqueous phases. The model results reveal that a non-aqueous formation pathway or direct biogenic emission is needed to supplement the commonly assumed acid-driven multiphase reaction process to explain the observed 2-MT concentrations. This missing pathway contributes to 20–40% of 2-MT in areas with aerosol pH<2 and more than 70% under less acidic conditions (pH~2–5), such as those encountered in the western US and China. The typical summertime gas-phase photochemical lifetimes of 2-MT and 2-MG are estimated to be 4–6 and 20–30 h, respectively, and their aqueous lifetimes are approximately 20–40 h. Our simulations show that predicted 2-MT is mainly influenced by its aqueous phase loss to OH, but 2-MG is more sensitive to gas phase OH loss due to the preferential partitioning of the two tracers in the aqueous and gas phases, respectively.
Funder
Partly supported by M. Shrivastava’s DOE Biological and Environmental Research (BER) Early Career Project at the Pacific Northwest National Laboratory National Natural Science Foundation of China
Publisher
Springer Science and Business Media LLC
Subject
Atmospheric Science,Environmental Chemistry,Global and Planetary Change
Reference63 articles.
1. Guenther, A. et al. Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature). Atmos. Chem. Phys. 6, 3181–3210 (2006). 2. Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C. & Seinfeld, J. H. Secondary organic aerosol formation from isoprene photooxidation. Environ. Sci. Technol. 40, 1869–1877 (2006). 3. Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C. & Seinfeld, J. H. Secondary organic aerosol formation from isoprene photooxidation under high-NOx conditions. Geophys. Res. Lett. 32, L18808 (2005). 4. Kleindienst, T. E., Lewandowski, M., Offenberg, J. H., Jaoui, M. & Edney, E. O. Ozone-isoprene reaction: Re-examination of the formation of secondary organic aerosol. Geophys. Res. Lett. 34, L01805 (2007). 5. Ng, N. et al. Secondary organic aerosol (SOA) formation from reaction of isoprene with nitrate radicals (NO 3). Atmos. Chem. Phys. 8, 4117–4140 (2008).
Cited by
2 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|