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A modeling evaluation of the effect of chlorine on the formation of particulate matter in combustion.

The effect of chlorine on the fuel-rich oxidation of hydrocarbons and on the molecular weight growth of aromatics is analyzed by simulating experiments featuring a model chlorinated additive CH3Cl in a jet-stirred/plug-flow reactor and premixed flames. The kinetic model used in this work emphasizes the role of resonantly stabilized radicals in the formation and growth of aromatics, and considers soot inception as the net effect of molecular weight growth and graphitization of aromatic structures. Chlorinated hydrocarbons decompose at temperatures significantly lower than hydrocarbons, producing reactive Cl-atoms, which have a strong tendency to go to HCl. The HCI, tying up the H-atoms, inhibits hydrocarbon oxidation. The model is able to predict not only the levels but the shape of the experiments quite well and also the surprising finding of an increased soot formation associated with lower PAH levels found in rich flames with significant levels of chlorine. Based on reaction kinetic analysis, chlorine addition to the fuel enhances soot formation by promoting the formation of aromatic-ring compounds and accelerating the abstraction of aromatic H-atoms from stable PAH molecules. This process activates the transformation of aromatics to soot.

Journal Article↗
PubMed2000

Nitro-PAH in ambient particulate matter in the atmosphere of Athens.

Nitrated polynuclear aromatic hydrocarbons (NPAH) with a molecular mass of 247 Daltons were found in soot collected in downtown Athens during a campaign performed in 1996. In particular, 2-nitrofluoranthene (2-NFa) and 2-nitropyrene (2-NPy), which are mainly related to photo-induced chemical processes occurring in the atmosphere, were more abundant than 1-nitropyrene (1-NPy) usually associated to motor vehicle exhaust.

Air Pollutants↗
PubMed1999

Trends in alkanes and PAHs in airborne particulate matter from Oporto and Vienna: identification and comparison.

A total of 56 weekly samples from Oporto and 40 from Vienna were collected and analysed, for 23 n-alkanes and 16 polycyclic aromatic hydrocarbons (PAH), by GC-MS after extraction with a toluene/methanol mixture. Total and elemental carbon were in the same range of values for both sampling sites. Although parts of the spectrum of species in both sampling sites were constant over the sampling period there is no evidence for suggesting a universal tracer for alkanes. For both Oporto and Vienna, Principal Component Analysis (PCA) identified two PCs and in both cases the first PC contained only PAHs while the second contained only alkanes. This separation between alkanes and PAHs and the observation of an alternating pattern with higher concentrations of odd carbon numbered from C27 to C30 (natural emissions from biological origin) is believed to result from a separation between anthropogenic and biological contributions associated with the first and second PC, respectively.

Air Pollutants↗
PubMed1999

Genotoxicity and embryotoxicity of urban air particulate matter collected during winter and summer period in two different districts of the Czech Republic.

This study is the in vitro part of a long-term program to investigate the impact of air pollution on the health of a population in a polluted region of Northern Bohemia. In order to assess the possible health risks associated with a complex mixture of hundreds of organic compounds adsorbed to air particles, we used a biomarker-directed fractionation procedure to evaluate biological activities of different chemical compound classes. The extractable organic compounds from the air particles collected in both the polluted and the control districts during the summers and winters of 1993-1994 were investigated. The principal aim of this study was to compare the DNA binding activities of those compound classes using an in vitro acellular assay coupled with 32P-postlabeling and an embryotoxicity assay using Chick Embryotoxicity Screening Test (CHEST). In both assays, the highest activity was due to the neutral fractions from which the aromatic subfractions containing mainly polycyclic aromatic hydrocarbons (PAHs) and their methyl-derivates were the most active for both localities and seasons. A good correlation between the levels of DNA adduct formation using S9 metabolic activation and the ED50 for all different complex mixtures of organic compounds was observed (r=0.773, p<0.001). DNA adduct maps and high performance liquid chromatography (HPLC) profiles were similar for samples from both districts and seasons. The major DNA adducts resulting from the crude extracts were identical to those derived from aromatic fractions. The DNA adducts tentatively identified constituted about 50% of the total adducts formed by the crude extracts following S9-metabolic activation. Our results confirmed the similarities of the major ubiquitous emission sources of organic compounds in both districts. This is the first report in which the biological activities of complex mixtures in short-term assays with remarkably different endpoints such as DNA adduct formation and embryotoxicity have been compared.

Air Pollutants↗
PubMed2001

Continuous automated measurement of hexavalent chromium in airborne particulate matter.

An automated continuous instrument for the collection and measurement of aerosol Cr(VI) is described. The system alternately collects the sample on one of two glass fiber filters. After 15-min sample collection on one filter, the sampling switches over to the second filter. The freshly sampled filter is washed for 8.5 min, and the washings are preconcentrated on a minicolumn packed with anion exchange resin. The washed filter is dried with filtered hot air for the next 6.5 min so that it is ready for sampling at the end of the 15-min cycle. The preconcentrated Cr(VI) on the column is eluted with 0.1 M sodium perchlorate and then reacted with sym-1,5-diphenylcarbazide prior to absorbance detection with a light emitting diode-based dedicated flow-through absorbance detector. The detection limit (S/N = 3) is 5 ng of Cr(VI)/m3, orders of magnitude lower than current regulatory requirements. The instrument operates unattended over long periods. In continuous round-the-clock operation, filter replacement frequency is every 24-72 h, depending on dust loading. The system is portable for facile field deployment and permits fully automated rapid determinations at a very low analysis cost per sample.

Aerosols↗