Parameterized Yields of Semivolatile Products from Isoprene Oxidation under Different NOx Levels: Impacts of Chemical Aging and Wall-Loss of Reactive Gases

TitleParameterized Yields of Semivolatile Products from Isoprene Oxidation under Different NOx Levels: Impacts of Chemical Aging and Wall-Loss of Reactive Gases
Publication TypeJournal Article
Year of Publication2018
AuthorsXing, Li, Shrivastava Manish, Fu Tzung-May, Roldin Pontus, Qian Yun, Xu Lu, Ng Nga L., Shilling John, Zelenyuk Alla, and Cappa Christopher D.
JournalEnvironmental Science & Technology
Volume52
Number16
Pages9225-9234
Date Published08/2018
Abstract

We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas-phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NOx levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NOx-sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NOx levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box model can be expanded to include more explicit chemical aging processes and help ultimately bridge the gap between the process-based understanding of SOA formation from VOC oxidation and the bulk-yield parametrizations used in chemical transport models.

URLhttp://dx.doi.org/10.1021/acs.est.8b00373
DOI10.1021/acs.est.8b00373
Journal: Environmental Science & Technology
Number: 16
Volume: 52

We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas-phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NOx levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NOx-sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NOx levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box model can be expanded to include more explicit chemical aging processes and help ultimately bridge the gap between the process-based understanding of SOA formation from VOC oxidation and the bulk-yield parametrizations used in chemical transport models.

DOI: 10.1021/acs.est.8b00373
Year of Publication: 2018
Citation:
Xing, L, M Shrivastava, T Fu, P Roldin, Y Qian, L Xu, NL Ng, J Shilling, A Zelenyuk, and CD Cappa.  2018.  "Parameterized Yields of Semivolatile Products from Isoprene Oxidation under Different NOx Levels: Impacts of Chemical Aging and Wall-Loss of Reactive Gases."  Environmental Science & Technology 52(16): 9225-9234, doi:10.1021/acs.est.8b00373.