Johan Martinsson

Evolution of In-Cylinder Diesel Engine Soot and Emission Characteristics Investigated with Online Aerosol Mass Spectrometry

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.

Investigation of the absorption Ångström exponent and its relation to physicochemical properties for mini-CAST soot

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. Copyright

Diesel soot aging in urban plumes within hours under cold dark and humid conditions

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.