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Epoxide as a precursor to secondary organic aerosol formation from isoprene photooxidation in the presence of nitrogen oxides.
Proc Natl Acad Sci U S A. 2013 Apr 23; 110(17):6718-23.PN

Abstract

Isoprene is a substantial contributor to the global secondary organic aerosol (SOA) burden, with implications for public health and the climate system. The mechanism by which isoprene-derived SOA is formed and the influence of environmental conditions, however, remain unclear. We present evidence from controlled smog chamber experiments and field measurements that in the presence of high levels of nitrogen oxides (NO(x) = NO + NO2) typical of urban atmospheres, 2-methyloxirane-2-carboxylic acid (methacrylic acid epoxide, MAE) is a precursor to known isoprene-derived SOA tracers, and ultimately to SOA. We propose that MAE arises from decomposition of the OH adduct of methacryloylperoxynitrate (MPAN). This hypothesis is supported by the similarity of SOA constituents derived from MAE to those from photooxidation of isoprene, methacrolein, and MPAN under high-NOx conditions. Strong support is further derived from computational chemistry calculations and Community Multiscale Air Quality model simulations, yielding predictions consistent with field observations. Field measurements taken in Chapel Hill, North Carolina, considered along with the modeling results indicate the atmospheric significance and relevance of MAE chemistry across the United States, especially in urban areas heavily impacted by isoprene emissions. Identification of MAE implies a major role of atmospheric epoxides in forming SOA from isoprene photooxidation. Updating current atmospheric modeling frameworks with MAE chemistry could improve the way that SOA has been attributed to isoprene based on ambient tracer measurements, and lead to SOA parameterizations that better capture the dependency of yield on NO(x).

Authors+Show Affiliations

Department of Environmental Sciences and Engineering, Gillings School of Global Public Health, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599, USA.No affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info availableNo affiliation info available

Pub Type(s)

Journal Article
Research Support, N.I.H., Extramural
Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.

Language

eng

PubMed ID

23553832

Citation

Lin, Ying-Hsuan, et al. "Epoxide as a Precursor to Secondary Organic Aerosol Formation From Isoprene Photooxidation in the Presence of Nitrogen Oxides." Proceedings of the National Academy of Sciences of the United States of America, vol. 110, no. 17, 2013, pp. 6718-23.
Lin YH, Zhang H, Pye HO, et al. Epoxide as a precursor to secondary organic aerosol formation from isoprene photooxidation in the presence of nitrogen oxides. Proc Natl Acad Sci U S A. 2013;110(17):6718-23.
Lin, Y. H., Zhang, H., Pye, H. O., Zhang, Z., Marth, W. J., Park, S., Arashiro, M., Cui, T., Budisulistiorini, S. H., Sexton, K. G., Vizuete, W., Xie, Y., Luecken, D. J., Piletic, I. R., Edney, E. O., Bartolotti, L. J., Gold, A., & Surratt, J. D. (2013). Epoxide as a precursor to secondary organic aerosol formation from isoprene photooxidation in the presence of nitrogen oxides. Proceedings of the National Academy of Sciences of the United States of America, 110(17), 6718-23. https://doi.org/10.1073/pnas.1221150110
Lin YH, et al. Epoxide as a Precursor to Secondary Organic Aerosol Formation From Isoprene Photooxidation in the Presence of Nitrogen Oxides. Proc Natl Acad Sci U S A. 2013 Apr 23;110(17):6718-23. PubMed PMID: 23553832.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Epoxide as a precursor to secondary organic aerosol formation from isoprene photooxidation in the presence of nitrogen oxides. AU - Lin,Ying-Hsuan, AU - Zhang,Haofei, AU - Pye,Havala O T, AU - Zhang,Zhenfa, AU - Marth,Wendy J, AU - Park,Sarah, AU - Arashiro,Maiko, AU - Cui,Tianqu, AU - Budisulistiorini,Sri Hapsari, AU - Sexton,Kenneth G, AU - Vizuete,William, AU - Xie,Ying, AU - Luecken,Deborah J, AU - Piletic,Ivan R, AU - Edney,Edward O, AU - Bartolotti,Libero J, AU - Gold,Avram, AU - Surratt,Jason D, Y1 - 2013/04/03/ PY - 2013/4/5/entrez PY - 2013/4/5/pubmed PY - 2013/6/29/medline SP - 6718 EP - 23 JF - Proceedings of the National Academy of Sciences of the United States of America JO - Proc Natl Acad Sci U S A VL - 110 IS - 17 N2 - Isoprene is a substantial contributor to the global secondary organic aerosol (SOA) burden, with implications for public health and the climate system. The mechanism by which isoprene-derived SOA is formed and the influence of environmental conditions, however, remain unclear. We present evidence from controlled smog chamber experiments and field measurements that in the presence of high levels of nitrogen oxides (NO(x) = NO + NO2) typical of urban atmospheres, 2-methyloxirane-2-carboxylic acid (methacrylic acid epoxide, MAE) is a precursor to known isoprene-derived SOA tracers, and ultimately to SOA. We propose that MAE arises from decomposition of the OH adduct of methacryloylperoxynitrate (MPAN). This hypothesis is supported by the similarity of SOA constituents derived from MAE to those from photooxidation of isoprene, methacrolein, and MPAN under high-NOx conditions. Strong support is further derived from computational chemistry calculations and Community Multiscale Air Quality model simulations, yielding predictions consistent with field observations. Field measurements taken in Chapel Hill, North Carolina, considered along with the modeling results indicate the atmospheric significance and relevance of MAE chemistry across the United States, especially in urban areas heavily impacted by isoprene emissions. Identification of MAE implies a major role of atmospheric epoxides in forming SOA from isoprene photooxidation. Updating current atmospheric modeling frameworks with MAE chemistry could improve the way that SOA has been attributed to isoprene based on ambient tracer measurements, and lead to SOA parameterizations that better capture the dependency of yield on NO(x). SN - 1091-6490 UR - https://www.unboundmedicine.com/medline/citation/23553832/Epoxide_as_a_precursor_to_secondary_organic_aerosol_formation_from_isoprene_photooxidation_in_the_presence_of_nitrogen_oxides_ L2 - http://www.pnas.org/lookup/pmidlookup?view=long&pmid=23553832 DB - PRIME DP - Unbound Medicine ER -