Effects of Gaseous Sulphuric Acid on Diesel Exhaust Nanoparticle Formation and Characteristics

Rönkkö, Topi; Lähde, Tero; Heikkilä, Juha; Pirjola, Liisa; Bauschke, Ulrike; Arnold, Frank; Schläger, Hans; Rothe, Dieter; Yli-Ojanperä, Jaakko; Keskinen, Jorma

doi:10.1021/es402354y

Cited by 77 publications

(33 citation statements)

References 37 publications

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“…It has been also shown in many studies that, by increasing the fuel sulphur content, the primary emissions of ultrafine particles are increased (e.g. Rönkkö et al, 2013). However, the nucleation mode particles formed from sulphur (and other condensable vapours) are often not well represented, in some cases not at all, in the PN emission factors and PSDs in the literature.…”

Section: Effect Of Sulphur On Psds and Emission Factorsmentioning

confidence: 99%

Continental anthropogenic primary particle number emissions

et al. 2016

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Abstract. Atmospheric aerosol particle number concentrations impact our climate and health in ways different from those of aerosol mass concentrations. However, the global, current and future anthropogenic particle number emissions and their size distributions are so far poorly known. In this article, we present the implementation of particle number emission factors and the related size distributions in the GAINS (Greenhouse Gas-Air Pollution Interactions and Synergies) model. This implementation allows for global estimates of particle number emissions under different future scenarios, consistent with emissions of other pollutants and greenhouse gases. In addition to determining the general particulate number emissions, we also describe a method to estimate the number size distributions of the emitted black carbon particles. The first results show that the sources dominating the particle number emissions are different to those dominating the mass emissions. The major global number source is road traffic, followed by residential combustion of biofuels and coal (especially in China, India and Africa), coke production (Russia and China), and industrial combustion and processes. The size distributions of emitted particles differ across the world, depending on the main sources: in regions dominated by traffic and industry, the number size distribution of emissions peaks in diameters range from 20 to 50 nm, whereas in regions with intensive biofuel combustion and/or agricultural waste burning, the emissions of particles with diameters around 100 nm are dominant. In the baseline (current legislation) scenario, the particle number emissions in Europe, Northern and Southern Americas, Australia, and China decrease until 2030, whereas especially for India, a strong increase is estimated. The results of this study provide input for modelling of the future changes in aerosol-cloud interactions as well as particle number related adverse health effects, e.g. in response to tightening emission regulations. However, there are significant uncertainties in these current emission estimates and the key actions for decreasing the uncertainties are pointed out.

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Section: Effect Of Sulphur On Psds and Emission Factorsmentioning

confidence: 99%

Continental anthropogenic primary particle number emissions

et al. 2016

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“…In most cases in our measurements, primary exhaust particle mass concentrations from the natural gas engine were close to the detection limits of the instruments EEPS, HRLPI and SP-AMS (Alanen et al, 2015;Lehtoranta et al, 2017). Exceptions were made by the high temperature catalyst cases (M2, C2, 500 • C and M2, C1, 450 • C) during which more primary particle mass was formed, especially on the size ranges of the HRLPI and EEPS: a high catalyst temperature favors the conversion of SO 2 into SO 3 and further into sulfuric acid, which can nucleate and condense on existing particles in the sampling process or when released into the atmosphere (see, e.g., Arnold et al, 2012;Rönkkö et al, 2013). The primary particle formation phenomena and concentrations have been discussed in more detail in Lehtoranta et al (2017) while this paper focuses on secondary aerosol formation and the total aged particle emissions.…”

Section: Instrumentation and Data Analysismentioning

confidence: 99%

Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics

et al. 2017

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Abstract. Natural gas usage in the traffic and energy production sectors 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, which both contribute to air quality and can cause adverse health effects. Technologies, such as cleaner engines or fuels, that produce less primary and secondary aerosols could potentially significantly decrease 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, which resulted in relatively long equivalent atmospheric ages of 11 days at most. The studied retro-fitted natural gas engine exhaust was observed to form secondary aerosol. The mass of the total aged particles, i.e., particle mass measured downstream of the PAM chamber, was 6-268 times as high as the mass of the emitted primary exhaust particles. The secondary organic aerosol (SOA) formation potential was measured to be 9-20 mg kg −1 fuel . The total aged particles mainly consisted of organic matter, nitrate, sulfate and ammonium, with the fractions depending on exhaust after-treatment and the engine parameters used. 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, in particular, the concentration of nitrate needed a long time to stabilize -more than half an hour -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 had 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 exhaust of a natural gas engine equipped with a catalyst forms secondary aerosol when the atmospheric ages in a PAM chamber are several days long. The secondary aerosol matter has different physical characteristics from those of primary particulate emissions.

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“…The primary particles can be generated directly in the engine during fuel combustion or can be nucleated in the air during dilution and cooling of hot exhaust (Kittelson, 1998;Kittelson et al, 2008;Arnold et al, 2012;Rönkkö et al, 2013;Vu et al, 2015). The former primary particles consist mostly of soot and exist mainly in the Aitken mode and accumulation mode, ranging from 30 to 500 nm, and the freshly nucleated vehicular particles during the initial 1-2 s of exhaust cooling and dilution processes reportedly exhibit a nucleation mode at 10-20 nm (Shi et al, 2000;Zhu et al, 2002aZhu et al, , b, 2006Vu et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

Simultaneous measurements of new particle formation at 1 s time resolution at a street site and a rooftop site

et al. 2017

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Abstract. This study is the first to use two identical Fast Mobility Particle Sizers for simultaneous measurement of particle number size distributions (PNSDs) at a street site and a rooftop site within 500 m distance in wintertime and springtime to investigate new particle formation (NPF) in Beijing. The collected datasets at 1 s time resolution allow deduction of the freshly emitted traffic particle signal from the measurements at the street site and thereby enable the evaluation of the effects on NPF in an urban atmosphere through a site-by-site comparison. The number concentrations of 8 to 20 nm newly formed particles and the apparent formation rate (FR) in the springtime were smaller at the street site than at the rooftop site. In contrast, NPF was enhanced in the wintertime at the street site with FR increased by a factor of 3 to 5, characterized by a shorter NPF time and higher new particle yields than at the rooftop site. Our results imply that the street canyon likely exerts distinct effects on NPF under warm or cold ambient temperature conditions because of on-road vehicle emissions, i.e., stronger condensation sinks that may be responsible for the reduced NPF in the springtime but efficient nucleation and partitioning of gaseous species that contribute to the enhanced NPF in the wintertime. The occurrence or absence of apparent growth for new particles with mobility diameters larger than 10 nm was also analyzed. The oxidization of biogenic organics in the presence of strong photochemical reactions is suggested to play an important role in growing new particles with diameters larger than 10 nm, but sulfuric acid is unlikely to be the main species for the apparent growth. However, the number of datasets used in this study is relatively small, and larger datasets are essential to draw a general conclusion.

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Effects of Gaseous Sulphuric Acid on Diesel Exhaust Nanoparticle Formation and Characteristics

Cited by 77 publications

References 37 publications

Continental anthropogenic primary particle number emissions

Continental anthropogenic primary particle number emissions

Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics

Simultaneous measurements of new particle formation at 1 s time resolution at a street site and a rooftop site

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Effects of Gaseous Sulphuric Acid on Diesel Exhaust Nanoparticle Formation and Characteristics

Cited by 77 publications

References 37 publications

Continental anthropogenic primary particle number emissions

Continental anthropogenic primary particle number emissions

Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics

Simultaneous measurements of new particle formation at 1 s time resolution at a street site and a rooftop site

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Product

Resources

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Simultaneous measurements of new particle formation at 1 s time resolution at a street site and a rooftop site