Abstract
In this study, we investigated the contribution of various source categories and regions to the secondary inorganic aerosol (SIA) in Europe with CAMx and its source apportionment tool PSAT during two measurement periods, representing cold and warm seasons. The results suggested that the main source for particulate nitrate was road transport, whereas energy industries were the most important contributor to sulfate particles. Emissions from international shipping were also found to be very important for both nitrate and sulfate particle formation. We found a large increase in secondary organic aerosol (SOA) concentrations when we doubled the biogenic volatile organic compound (BVOC) emissions during the warm season, as expected. We also found, however, a decrease in particulate inorganic nitrate and sulfate concentrations by about −35% and −12%, respectively, at different locations. The negative correlation between BVOCs and SIA indicates the importance of precursor gases and biogenic emission types. The results of further tests suggested that terpene reactions with nitrate radicals at night led to a decline in inorganic nitrate formation. Sulfate concentrations, on the other hand, decreased due to the reactions of BVOCs with OH radicals.
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Acknowledgements
Various input data were provided by INERIS, TNO, ECMWF within the EURODELTA III exercise. We thank G. Yarwood for his valuable comments. This work was funded by the Swiss Federal Office of Environment (FOEN).
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Questioner’s Name: Jerzy Bartnicki
Question: What method have you used for calculating contributions from individual sources and how did you take care of non-linear effects?
Answer: We used the PSAT (Particle Source Apportionment Technology) tool of CAMx model. PSAT is a reactive tracer method where a single tracer tracks the primary PM species, on the other hand, several tracers are required to track the relationships between the gaseous precursors and the resulting secondary PM species, i.e. in case of nitrogen, PSAT uses tracers such as NOx, NO3 radical, HONO, N2O5, PAN, PNA, HNO3, organic nitrates, particulate nitrate. This method has been compared with other methods such as brute-force and zero-out by the developers and shown to be more efficient and better able to deal with the non-linear chemistry than the other methods (Yarwood et al. 2007; Koo et al. 2009).
Questioner’s Name: Rohit Mathur
Question: In the 2xBVOC experiment, did you examine the possible role of increased organic nitrate formation on reducing HNO3 and consequently reduced PNO3 levels?
Answer: Yes, we also investigated the organic nitrate formation in our sensitivity calculations with doubled BVOC emissions. In CB05 mechanism, organic nitrates are produced by reactions of isoprene and its oxidation products with NO2 and NO3 as well as from reactions of monoterpenes with NO3. Increasing BVOC emissions led to an increase in organic nitrates and when the BVOC reactions with NO3 radical were turned off, organic nitrate production decreased significantly at night (opposite to HNO3 formation). These results suggest that monoterpene reactions with nitrate radicals at night are reducing the nighttime formation of HNO3 and consequently formation of PNO3.
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Aksoyoglu, S., Ciarelli, G., El-Haddad, I., Baltensperger, U., Prévôt, A.S.H. (2018). Source Apportionment of Inorganic Aerosols in Europe and Role of Biogenic VOC Emissions. In: Mensink, C., Kallos, G. (eds) Air Pollution Modeling and its Application XXV. ITM 2016. Springer Proceedings in Complexity. Springer, Cham. https://doi.org/10.1007/978-3-319-57645-9_59
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DOI: https://doi.org/10.1007/978-3-319-57645-9_59
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