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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
Research article
08 Feb 2017
Review status
A revision of this discussion paper was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.
Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics
Jenni Alanen1, Pauli Simonen1, Sanna Saarikoski2, Hilkka Timonen2, Oskari Kangasniemi1, Erkka Saukko1, Risto Hillamo2, Kati Lehtoranta3, Timo Murtonen3, Hannu Vesala3, Jorma Keskinen1, and Topi Rönkkö1 1Aerosol Physics, Faculty of Natural Sciences, Tampere University of Technology, P.O. Box 692, 33101 Tampere, Finland
2Atmospheric Composition Research, Finnish Meteorological Institute, P.O. Box 503, 00101 Helsinki, Finland
3VTT Technical Research Centre of Finland Ltd., P.O. Box 1000, 02044 VTT, Espoo, Finland
Abstract. Natural gas usage in traffic and energy production sector is a growing trend worldwide, thus an assessment of its effects on air quality, human health and climate is required. Engine exhaust is a source of primary particulate emissions and secondary aerosol precursors that both contribute to air quality and can cause adverse health effects. Technologies, such as cleaner engines or fuels, that produce less primary and secondary aerosol could potentially significantly decrease the atmospheric particle concentrations and their adverse effects. In this study, we used a potential aerosol mass (PAM) chamber to investigate the secondary aerosol formation potential of natural gas engine exhaust. The PAM chamber was used with a constant UV-light voltage that resulted in an equivalent atmospheric age of 11 days at a maximum. The studied passenger car engine, retrofitted to run with natural gas, was observed to have a low or moderate secondary particle formation potential, although the simulated atmospheric ages were relatively long. The secondary organic aerosol (SOA) formation potential was measured to be 8–18 mg kgfuel−1. However, the mass of total aged particles, i.e. particle mass measured downstream the PAM chamber, was 6–184 times as high as the mass of the emitted primary exhaust particles. The total aged particles consisted mainly of nitrate, organic matter, sulfate and ammonium, the fractions depending on exhaust after-treatment and used engine parameters. Also the volatility, composition and concentration of the total aged particles were found to depend on the engine operating mode, catalyst temperature and catalyst type. For example, a high catalyst temperature promoted the formation of sulfate particles, whereas a low catalyst temperature promoted nitrate formation. However, especially the concentration of nitrate needed a long time, more than half an hour, to stabilize, which complicated the conclusions but also indicates the sensitivity of nitrate measurements on experimental parameters such as emission source and system temperatures. Sulfate was measured to have the highest evaporation temperature and nitrate the lowest. The evaporation temperature of ammonium depended on the fractions of nitrate and sulfate in the particles. The average volatility of the total aged particles was measured to be lower than that of primary particles, indicating better stability of the aged natural gas engine emitted aerosol in the atmosphere. According to the results of this study, the shift from traditional liquid fuels to natural gas can have a decreasing effect on total particle pollution in the atmosphere; in addition to the very low primary particle emissions, also the secondary organic aerosol formation potential of natural gas exhaust is lower or on the same level as the SOA formation potential measured on liquid fuels in previous studies.

Citation: Alanen, J., Simonen, P., Saarikoski, S., Timonen, H., Kangasniemi, O., Saukko, E., Hillamo, R., Lehtoranta, K., Murtonen, T., Vesala, H., Keskinen, J., and Rönkkö, T.: Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics, Atmos. Chem. Phys. Discuss.,, in review, 2017.
Jenni Alanen et al.
Jenni Alanen et al.


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Short summary
Secondary organic and inorganic aerosols deteriorate air quality. Their formation from a natural gas engine was studied and compared with the emitted primary particulate emission. The volatility of the formed particles was defined as a function of temperature. Photochemical ages 4–11 days, mimicked by a potential aerosol mass chamber, produced 8–18 mg/kg_fuel SOA, respectively. Aged emission particles were found to be less volatile than the fresh, implicating longer stability in the atmosphere.
Secondary organic and inorganic aerosols deteriorate air quality. Their formation from a natural...