Photochemical aging and secondary organic aerosols generated from limonene in an oxidation flow reactor
- 57 Downloads
Oxidation flow reactors (OFRs) are increasingly used to study the formation and evolution of secondary organic aerosols (SOA) in the atmosphere. The OH/HO2 and OH/O3 ratios in OFRs are similar to tropospheric ratios. In the present work, we investigated the production of SOA generated by OH oxydation and ozonolysis of limonene in OFR as a function of OH exposure and O3 exposure. The results are compared with those obtained from the simulation chambers. The precursor gas is exposed to OH concentrations ranging from 2.11 × 108 to 1.91 × 109 molec cm−3, with an estimated exposure time in the OFR of 137 s. In the environmental chambers, the precursor was oxidized using OH concentrations between 2.10 × 106 and 2.12 × 107 molec cm−3 over exposure times of several hours. In the overlapping OH exposure region, the highest SOA yields are obtained in the OFR, which is explained by the ozonolysis of limonene in the OFR. However, the yields decrease with the increase of OHexp in both systems.
KeywordsPhotochemistry Aging Particles OFR Atmosphere Environmental chambers
The authors thank the University Claude Bernard for the technical and financial support provided by the Institute for Research on catalysis and the environment of Lyon (IRCELYON). We thank Mr. Christian George who participated in all the steps of preparation of this paper except in the redaction.
This study was supported by the European Research Council under the Horizon 2020 Research and Innovation Program Project of the European Union under Convention N° 690958 (MARSU).
Compliance with ethical standards
Conflict of interest
The authors declare that they have no conflict of interest.
- Atkinson R (1997) Gas-phase tropospheric chemistry of volatile organic compounds alkanes and alkenes. J Phys Chem 26:215–290Google Scholar
- Fang W, Gong L, Shengn L (2017) Online analysis of secondary organic aerosols from OH-initiated photooxidation and ozonolysis of α-pinene, β-pinene, Δ3-carene and d-limonene by thermal desorption–photoionisation aerosol mass spectrometry. Environ Chem 14:75–90. https://doi.org/10.1071/EN16128 CrossRefGoogle Scholar
- Lambe AT, Onasch TB, Massoli P, Croasdale DR, Wright JP, Ahern AT, Davidovits P (2011) Laboratory studies of the chemical composition and cloud condensation nuclei (CCN) activity of secondary organic aerosol (SOA) and oxidized primary organic aerosol (OPOA). Atmos Chem Phys 11:8913–8928. https://doi.org/10.5194/acp-11-8913-2011 CrossRefGoogle Scholar
- Lambe AT, Onasch TB, Croasdale DR, Wright JP, Martin AT, Franklin JP, Davidovits P (2012) Transitions from functionalization to fragmentation reactions of laboratory secondary organic aerosol (SOA) generated from the OH oxidation of alkane precursors. Environ Sci Technol 46:5430–5437. https://doi.org/10.1021/es300274t CrossRefGoogle Scholar
- Peng Z, Palm BB, Day DA, Talukdar RK, Hu W, Lambe AT et al (2018) Model evaluation of new techniques for maintaining high-NO conditions in oxidation flow reactors for the study of OH initiated atmospheric chemistry. ACS Earth Space Chem 2:72 86. https://doi.org/10.1021/acsearthspacechem.7b00070 CrossRefGoogle Scholar
- Riipinen I, Pierce JR, Yli-Juuti T, Nieminen T, Häkkinen S, Ehn M, Junninen H, Lehtipalo K, Petäjä T, Slowik J, Chang R, Shantz NC, Abbatt J, Leaitch W, Kerminen VM, Worsnop D, Pandis SN, Donahue NM, Kulmala M (2011) Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentration. Atmos Chem Phys 11:3865–3878. https://doi.org/10.5194/acp-11-3865-2011 CrossRefGoogle Scholar
- Perraud V, Bruns EA, Ezell MJ, Johnson SN, Yu Y, Alexander ML, Zelenyuk A, Imre D, Chang WL, Dabdub D, Pankow JF, Finlayson-Pitts BJ (2012) Nonequilibrium atmospheric secondary organic aerosol formation and growth. Proc Natl Acad Sci USA 109:2836–2841. https://doi.org/10.1073/pnas.1119909109 CrossRefGoogle Scholar
- Simonen P, Saukko E, Karjalainen P, Timonen H, Bloss M, Aakko-Saksa P, Dal Maso M (2016) A new oxidation flow reactor for measuring secondary aerosol formation of rapidly changing emission sources. Atmos Meas Tech Discuss:1–27. https://doi.org/10.5194/amt-2016-300
- Zhang X, Azhar G, Rogers SC, Foster SR, Luo S, We JY (2014) Overexpression of p49/STRAP alters cellular cytoskeletal structure and gross anatomy in mice. BMC Cell Biol:15–32. https://doi.org/10.1186/1471-2121-15-32
- Zhao D, Schmitt SH, Wang M, Acir IH, Tillmann R, Tan Z, Mentel TF (2018b) Effects of effects of NOx and SO2 on the secondary organic aerosol formation from photooxidation of α-pinene and limonene. Atmos Chem Phys 18:1611–1628. https://doi.org/10.5194/acp-18-1611-2018
- Zhao Y, Lambe AT, Saleh R, Saliba G, Robinson AL (2018a) Secondary organic aerosol production from gasoline vehicle exhaust: effects of engine technology, cold start, and emission certification standard. Environ Sci Technol 52:1253–1261. https://doi.org/10.1021/acs.est.7b05045 CrossRefGoogle Scholar