| 1. |
- Török, Sandra, et al.
(author)
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Investigation of the absorption Ångström exponent and its relation to physicochemical properties for mini-CAST soot
- 2018
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In: Aerosol Science and Technology. - : Informa UK Limited. - 0278-6826 .- 1521-7388. ; 52:7, s. 757-767
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Journal article (peer-reviewed)abstract
- In this work, a mini-CAST soot generator was used to produce soot with different optical and physicochemical characteristics. Absorption Ångström exponents (AAE) expressing the absorption wavelength dependence were assessed by multiwavelength in-situ and filter-based (aethalometer) laser extinction. The two optical techniques showed good agreement. For the chosen mini-CAST operating conditions, AAEs between 1 and 3.5 were found. Soot with high mass-fractions of organic carbon (OC) and pyrolytic carbon (PC) determined with thermal optical analysis were associated with AAEs significantly higher than 1. Heating to 250 and 500°C removed the majority of polycyclic aromatic hydrocarbons. However, the thermal-optical analysis revealed that OC and PC were abundant in the soot with AAE > 2 also after heating the aerosol. Analysis of mass absorption cross section ratios for elemental carbon and OC indicated that elevated AAEs also after heating to 500°C could be related to persistent OC and PC components and/or the refractory soot. By comparing the mini-CAST soot optical properties with soot properties derived from in-situ extinction measurements in a premixed flame, mini-CAST soot with a higher AAE could be identified as less mature soot.
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| 2. |
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| 3. |
- Eriksson, Axel, et al.
(author)
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Diesel soot aging in urban plumes within hours under cold dark and humid conditions
- 2017
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In: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322.
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Journal article (peer-reviewed)abstract
- Fresh and aged diesel soot particles have different impacts on climate and human health. While fresh diesel soot particles are highly aspherical and non-hygroscopic, aged particles are spherical and hygroscopic. Aging and its effect on water uptake also controls the dispersion of diesel soot in the atmosphere. Understanding the timescales on which diesel soot ages in the atmosphere is thus important, yet knowledge thereof is lacking. We show that under cold, dark and humid conditions the atmospheric transformation from fresh to aged soot occurs on a timescale of less than five hours. Under dry conditions in the laboratory, diesel soot transformation is much less efficient. While photochemistry drives soot aging, our data show it is not always a limiting factor. Field observations together with aerosol process model simulations show that the rapid ambient diesel soot aging in urban plumes is caused by coupled ammonium nitrate formation and water uptake.
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| 7. |
- Malmborg, Vilhelm, et al.
(author)
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Evolution of In-Cylinder Diesel Engine Soot and Emission Characteristics Investigated with Online Aerosol Mass Spectrometry
- 2017
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 1520-5851 .- 0013-936X. ; 51:3, s. 1876-1885
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Journal article (peer-reviewed)abstract
- To design diesel engines with low environmental impact, it is important to link health and climate-relevant soot (black carbon) emission characteristics to specific combustion conditions. The in-cylinder evolution of soot properties over the combustion cycle and as a function of exhaust gas recirculation (EGR) was investigated in a modern heavy-duty diesel engine. A novel combination of a fast gas-sampling valve and a soot particle aerosol mass spectrometer (SP-AMS) enabled online measurements of the in-cylinder soot chemistry. The results show that EGR reduced the soot formation rate. However, the late cycle soot oxidation rate (soot removal) was reduced even more, and the net effect was increased soot emissions. EGR resulted in an accumulation of polycyclic aromatic hydrocarbons (PAHs) during combustion, and led to increased PAH emissions. We show that mass spectral and optical signatures of the in-cylinder soot and associated low volatility organics change dramatically from the soot formation dominated phase to the soot oxidation dominated phase. These signatures include a class of fullerene carbon clusters that we hypothesize represent less graphitized, C5-containing fullerenic (high tortuosity or curved) soot nanostructures arising from decreased combustion temperatures and increased premixing of air and fuel with EGR. Altered soot properties are of key importance when designing emission control strategies such as diesel particulate filters and when introducing novel biofuels.
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| 8. |
- Malmborg, Vilhelm, et al.
(author)
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Relating aerosol mass spectra to composition and nanostructure of soot particles
- 2019
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In: Carbon. - : Elsevier BV. - 0008-6223. ; 142, s. 535-546
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Journal article (peer-reviewed)abstract
- The composition and carbon nanostructure of soot are important parameters influencing health and climate effects, and the efficacy of soot mitigation technologies. We used laser-vaporization, electron-ionization aerosol mass spectrometry (or SP-AMS) to systematically investigate relationships between aerosol mass spectra, carbon nanostructure (HRTEM), and composition (thermal-optical carbon analysis) for soot with varying physicochemical properties. SP-AMS refractory black carbon concentrations (based on C≤5+ clusters) were correlated to elemental carbon (r = 0.98, p < 10−8) and equivalent black carbon (aethalometer) concentrations. The SP-AMS large carbon (C≥6+, midcarbons and fullerene carbons) fraction was inversely correlated to fringe length (r = −0.97, p = 0.028) and linearly correlated to the fraction of refractory organic carbon that partially pyrolize during heating (r = 0.89, p < 10−4). This refractory organic carbon material was incompletely detected with conventional aerosol mass spectrometry (flash vaporization at 600 °C). This suggests that (SP-AMS) refractory carbon cluster analysis provides insight to chemical bonding and nanostructures in refractory carbon materials, lowcarbons (C≤5+) indicate mature soot and large carbons indicate refractory organic carbon and amorphous nanostructures related to C5-components. These results have implications for assessments of soot particle mixing state and brown carbon absorption in the atmosphere and enable novel, on-line analysis of engineered carbon nanomaterials and soot characteristics relevant for climate and health.
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| 9. |
- Martinsson, Johan, et al.
(author)
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Impacts of Combustion Conditions and Photochemical Processing on the Light Absorption of Biomass Combustion Aerosol
- 2015
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 49:24, s. 14663-14671
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Journal article (peer-reviewed)abstract
- The aim was to identify relationships between combustion conditions, particle characteristics, and optical properties of fresh and photochemically processed emissions from biomass combustion. The combustion conditions included nominal and high burn rate operation and individual combustion phases from a conventional wood stove. Low temperature pyrolysis upon fuel addition resulted in "tar-ball" type particles dominated by organic aerosol with an absorption Angstrom exponent (AAE) of 2.5-2.7 and estimated Brown Carbon contributions of 50-70% to absorption at the climate relevant aethalometer-wavelength (520 nm). High temperature combustion during the intermediate (flaming) phase was dominated by soot agglomerates with AAE 1.0-1.2 and 85-100% of absorption at 520 nm attributed to Black Carbon. Intense photochemical processing of high burn rate flaming combustion emissions in an oxidation flow reactor led to strong formation of Secondary Organic Aerosol, with no or weak absorption. PM1 mass emission factors (mg/kg) of fresh emissions were about an order of magnitude higher for low temperature pyrolysis compared to high temperature combustion. However, emission factors describing the absorption cross section emitted per kg of fuel consumed (m(2)/kg) were of similar magnitude at 520 nm for the diverse combustion conditions investigated in this study. These results provide a link between biomass combustion conditions, emitted particle types, and their optical properties in fresh and processed plumes which can be of value for source apportionment and balanced mitigation of biomass combustion emissions from a climate and health perspective.
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