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At least 19 recordsLinked to original sources
PubMed2002

Sorption of polycyclic aromatic hydrocarbons and polychlorinated biphenyls to soot and soot-like materials in the aqueous environment: mechanistic considerations.

Recent studies have shown that sorption of polycyclic aromatic hydrocarbons (PAHs) in soot-water systems is exceptionally strong. As a consequence, soot may fully control the actual fate of PAHs in the aquatic environment. However, sorption has only been characterized for a limited number of PAHs to diesel soot, and the mechanism is poorly understood. In this paper, we present an extensive data set of sorbent-water distribution coefficients (K(S), n = 236) for a series of PAHs (both native and added) and polychlorinated biphenyls (PCBs) to five different types of soot and five soot-like materials. Both Ks values and physicochemical properties of the sorbents show large variation. In general, sorption is very strong, with K(S) values up to 10(10), showing the highest distribution coefficients on a mass basis ever reported. Sorption of in particular PAHs is often over 1000 times as strong as sorption to amorphous sedimentary organic carbon. The variation in K(S) values cannot be explained by "soot carbon fractions" or specific surface areas of the sorbents. Instead, values for native PAHs are mostly determined by the sorbates' molar volume, and values for added PAHs and PCBs are determined by the sorbents' average pore diameter. From differences in K(S) values between native and added PAH analogues, it can be deduced that generally more than 50% (with values up to 97%) of the native PAH concentration in soot is not available for distribution to the aqueous phase. We conclude that this is caused by physical entrapment of the chemicals within the solid matrix. Furthermore, most sorbents appear to preferentially sorb PCBs with planar configurations, a phenomenon most likely driven by sorption in molecular-sized pores. Pore sorption is also concluded to be the most important sorption mechanism for added PAHs together with pi-pi interaction processes with flat aromatic sorbent surfaces. Frequently observed, slowly desorbing, resistant contaminant fractions in sediments may very well be explained on the basis of these results.

Adsorption↗
PubMed2004

Modeling maximum adsorption capacities of soot and soot-like materials for PAHs and PCBs.

Recent studies have shown that not partitioning but adsorption is the main mechanism for sorption of hydrophobic organic compounds to soot and soot-like materials. For compounds that adsorb by van derWaals forces only, variation in soot-water distribution coefficients will result from differences in these forces for adsorption, as well as the maximum number of accessible sites. This maximum number of accessible sites may a priori be expected to vary due to differences in both sorbent characteristics and sorbate dimensions. In this modeling study, variation in maximum adsorption capacities is explained from sorbent and sorbate properties. Maximum adsorption capacities were calculated using (a) literature values for soot-water distribution coefficients for polycyclic aromatic hydrocarbons and polychlorobiphenyls on 10 different soot and soot-like materials and (b) Langmuir affinities for adsorption at a carbonaceous surface estimated using a recently reported method. The variation in maximum adsorption capacities could be explained by the variation in sorbent specific surface area, sorbent organic carbon content, and the sorbent-sorbate contact area. Furthermore, increasing sorbate thickness was related to a decrease in maximum adsorption capacities, which points to adsorption in micropores. Maximum adsorption capacities decreased by 1-2 orders of magnitude as the contact area increased by 50%. This points to adsorption sites being hardly larger than sorbates.

Adsorption↗
PubMed2002

Soot-water distribution coefficients for polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans and polybrominated diphenylethers determined with the soot cosolvency-column method.

For many types of hydrophobic compounds, sorption non-linearity and solid-water distributions in the field well above expectations from organic matter partitioning models have lead to the proposition that strong adsorption to soot surfaces may not be limited to polycyclic aromatic hydrocarbons but may extend as a significant process for many aromatic compound classes. Here, the soot-water distribution coefficients (Ksc) were determined with the soot cosolvency-column method for homolog series of five polychlorinated dibenzo-p-dioxins (PCDDs), five polychlorinated dibenzofurans (PCDFs) and for two polybrominated diphenylethers (PBDEs). All compounds exhibited significantly stronger association with soot carbon than expected from estimates of their bulk organic-carbon normalized partition coefficients (Koc). The Ksc/Koc ratios (at aqueous concentrations of around 0.1-1 microg/l) were for PCDDs (up to tetrachlorination) 19-130 (median 25), for PCDFs (also up to tetrachlorination) 150-490 (median 300), and for both the tetra- and pentabrominated PBDEs a factor of 60. The particularly strong soot sorption for the PCDFs is of similar enhancement factors as previously elucidated for polycyclic aromatic hydrocarbons. Compound-class specific correlations between log Ksc and octanol-water partition coefficients (log Kow) were significant for both PCDDs and PCDFs (and with R2 > 98%). These may prove useful for anticipating variable fractions of dissolved exposures between different environmental regimes and putative remediation objects.

Adsorption↗
PubMed2004

Universal occurrence of soot superaggregates with a fractal dimension of 2.6 in heavily sooting laminar diffusion flames.

Using small-angle light scattering we show that a new phase of soot with size ca. 10 microm and a fractal dimension of D approximately equal to 2.6 exists in laminar diffusion flames for a wide range of heavily sooting fuels. This new phase appears to be a supramicrometer extension of the well-known submicrometer, D approximately equal to 1.8 phase of soot formed via diffusion-limited cluster aggregation (DLCA). The occurrence of this new soot phase correlates with an empirical sooting index for fuels. This supports a creation scenario in which these supramicrometer aggregates are created via a percolation of the submicrometer, D approximately equal to 1.8 aggregates.

Journal Article↗
PubMed2004

Mass spectrometry up to 1 million mass units for the simultaneous detection of primary soot and of soot precursors (nanoparticles) in flames.

A hybrid setup consisting of low pressure burner, flow reactor and photo-ionization mass spectrometer was used for the simultaneous detection of primary soot and of flame generated nanoparticles precursing soot. The studied flames were low pressure (120-180 mbar) C2H4/O2 flames surrounded by an N2 shield. The flow reactor was not used in this study. Through variation of the burner conditions (stoichiometry, sampling height) it could be shown that nanoparticles and soot are entirely independent species. The former, in particular, are found very early in the flame and their concentration profiles do not vary very much throughout the flame. This renders the possibility that nanoparticles are emitted together with soot and consequently may constitute an additional environmental hazard. Photo-ionization mass spectrometry is well suited for the detection of these particles.

Carbon↗
PubMed2005

Extremely slowly desorbing polycyclic aromatic hydrocarbons from soot and soot-like materials: evidence by supercritical fluid extraction.

Combustion-derived PAHs are strongly sorbed to their particulate carrier (i.e., soot, charcoal), and therefore, very slow desorption kinetics of the chemicals might be anticipated. Measurements are however lacking, because conventional methods (Tenax, XAD, gas-purging) fail to accurately determine desorption kinetics due to practical problems. In this study, we used a mild supercritical fluid extraction (SFE) method, which mimics desorption into water and circumvents these problems, to quantify desorption kinetics of 13 native PAHs from pure charcoal, coal, and four types of soot. The results show that generally only very small PAH fractions are released. Desorption behavior was, however, not related to common sorbent/sorbate characteristics. Two-site model-derived "fast desorbing fractions" were <0.01 in the majority of cases, and for the dominant "slow sites", the calculated rate constants for desorption into water measured from 10(-7) to 10(-5) h(-1). These data suggest that desorption of coal and combustion-derived PAHs can be even slower than the "very slow" desorption observed in sediments. Estimated time scales required for removal of pyrogenic PAHs from these extremely slow sites into water amount to several millennia. Our results imply reduced chemical risks for soot and soot-like materials, casting doubts on current risk assessment procedures and environmental quality standards of pyrogenic PAHs.

Carbon↗
PubMed2004

Formation of polychlorinated dibenzo-p-dioxins/dibenzofurans from soot of benzene and o-dichlorobenzene combustion.

Soots were prepared from flame combustion of benzene and o-dichlorobenzene (ODCB), creating one soot without carbon-chlorine bonds (benzene soot) and one with such bonds (ODCB soot). ODCB soot was tested for PCDD/F formation between 277 and 600 degrees C without additional chlorine, but levels were very low. Copper and Cu2O were added as potential catalysts for ODCB soot oxidation, but levels of PCDD/F observed were even lower than without these additives. Both benzene soot and ODCB soot produced PCDD/F after adding CuCl2 to the reaction mixtures, suggesting that a (volatile) metal chloride was needed in order for PCDD/F formation to take place. Under the various conditions of [Cu2+], time, and temperature tested, ODCB soot was always more reactive than benzene soot in forming PCDD/F. It seemed plausible that, despite the fact that CuCl2 was very effective in creating C-Cl bonds in benzene soot, the C-Cl bonds created in ODCB soot during preparation were of a reactivity so as to make this soot especially prone to PCDD/F formation. High temperature (gas phase) chlorination of soots by HCI or other chlorinating agents, followed by deposition of these soots and condensed metal chlorides on the ducts and walls of the postcombustion zone, could create an effective mechanism for de novo formation of PCDD/F.

Benzene↗
PubMed1983

Subchronic oral toxicity in guinea pigs of soot from a polychlorinated biphenyl-containing transformer fire.

We have previously described the acute po toxicity in guinea pigs of soot from a transformer fire at the State Office Building in Binghamton, New York. The soot was determined to contain polychlorinated biphenyls, biphenylenes, dibenzodioxins, and dibenzofurans. The present study evaluates soot toxicity in guinea pigs receiving 0, 0.2, 1.9, 9.3, or 46.3 ppm soot in the feed for 90 days or 231.5 ppm for 32 days. At 231.5 ppm, body weight loss, thymic atrophy, bone marrow depletion, skeletal muscle and gastrointestinal tract epithelial degeneration, and fatty infiltration of hepatocytes were observed. Mortality had reached 35% by Day 32 (when survivors were killed), with total soot consumption of approximately 400 mg/kg. At 46.3 or 9.3 ppm soot, a reduced rate of body weight gain was observed, and at 46.3 ppm, the mortality by Day 90 was 30%. Relative (to body) thymus weights were decreased in both groups, while relative spleen weights were increased at 46.3 ppm soot only. Salivary gland interlobular duct squamous metaplasia and focal lacrimal gland adenitis were detected histopathologically, while bone marrow depletion was noted only in females at the higher dose. Diminished serum alanine aminotransferase (ALT) activity in both sexes and decreased serum sodium levels in male and potassium levels in female animals were detected at both dose levels. decreased gamma-glutamyl transferase activity and red blood cell count and elevated serum creatinine and triglycerides were observed only in animals fed 46.3 ppm soot. At 1.9 ppm soot, salivary gland duct metaplasia was observed in both sexes, along with decreased relative thymus weights, ALT activity, and serum sodium levels in male animals only. No effects attributable to soot exposure were noted in animals receiving 0.2 ppm soot for 90 days. Total average soot consumption for male and female animals in the 0.2, 1.9, 9.3, and 46.3 ppm dosage groups was 1.2, 12, 55, and 275 mg/kg, respectively. Although many of the observed effects were typical of acute exposure of guinea pigs to the Binghamton soot or to polychlorinated aromatic hydrocarbons in general, salivary gland duct metaplasia has not been previously reported. Toxic effects of this subchronic exposure were observed at lower total doses than with acute exposure, although variations in absorption due to the effects of different vehicles (aqueous in the acute study versus the feed in this study) could account for some or all of this difference.

Administration, Oral↗
PubMed2006

A morphological investigation of soot produced by the detonation of munitions.

The morphology of three different detonation soot samples along with other common soot materials such as carbon black, diesel soot and chimney soot was studied by elemental and proximate analysis, X-ray diffraction and electron microscopy. The goal of this study was to better define the morphology of the detonation soot in order to better assess the interactions of this type of soot with explosive residues. The detonation soot samples were obtained by the detonation of artillery 155mm projectiles filled with either pure TNT (2,4,6-trinitrotoluene) or composition B, a military explosive based on a mixture of TNT and RDX (trimethylentrinitramine). The carbon content of the soot samples varied considerably depending on the feedstock composition. Detonation soot contains less carbon and more nitrogen than the other carbonaceous samples studied, due to the molecular structure of the energetic materials detonated such as TNT and RDX. The ash concentration was higher for detonation soot samples due to the high metal content coming from the projectiles shell and to the soil contamination which occurred during the detonation. By X-ray diffraction, diamond and graphite were found to be the major crystalline carbon forms in the detonation soot. Two electron microscopy techniques were used in this study to visualise the primary particles and to try to explain the formation mechanism of detonation soot samples.

Carbon↗
PubMed2004

Box model investigation of the effect of soot particles on ozone downwind from an urban area through heterogeneous reactions.

Soot can provide additional surface area where heterogeneous reactions can take place in the atmosphere. These reactions are dependent on the number of reactive sites on the soot surface rather than the soot surface area per se. A box model, MOCCA, is used to investigate the effects of introducing heterogeneous reactions on soot into air parcel passing over an urban area and traveling downwind. The model was run at two soot mass concentrations of 2 microg/m3 and 20 microg/m3 with a surface density of n-hexane and decane. Signifcant change in gasphase concentration was only observed for the higher soot concentration. Due to the noncatalytic nature of the heterogeneous reactions, soot sites are rapidly consumed, and soot site concentrations are greatly reduced shortly after emissions are turned off. Notable changes in gaseous concentrations due to the introduction of heterogeneous reactions are not observed in the urban setting. The impact of heterogeneous reactions is more evident after emissions are turned off (i.e. downwind from the urban center). These changes are minimal for the condition that used n-hexane surface density. For conditions that used decane soot, NOx concentrations showed a slight increase, with NO being higher in the daytime and NO2 at night. The maximum O3 reduction observed when using the higher soot concentration is 7 ppb, downwind of the urban center. Change in O3 concentration was less than 1 ppb when using the lower soot loading. The observed effects of heterogeneous reactions on soot decrease with time.

Air Pollutants↗
PubMed2000

Kerosene soot genotoxicity: enhanced effect upon co-exposure with chrysotile asbestos in Syrian hamster embryo fibroblasts.

Epidemiological and experimental studies have suggested an enhancement of asbestos-induced bronchogenic carcinoma by cigarette smoke. Further, our recent experimental and epidemiological studies have indicated that besides smoking, several other compounds including kerosene soot may accelerate disease processes in asbestos-exposed animals as well as in the humans. Incomplete combustion of kerosene oil generates large volumes of soot, which contains various polycyclic aromatic hydrocarbons and aliphatic compounds. As reported earlier, exposure to kerosene soot is known to cause biochemical and pathological changes in the pulmonary tissue, which may cause cardiopulmonary disorders. In this study we investigated genotoxic effects caused by kerosene soot and chrysotile asbestos as well as co-exposure of kerosene soot and chrysotile using Syrian hamster embryo fibroblasts (SHE). The micronucleus assay revealed a significant increase of induced micronuclei (MN), (P</=0.05) in SHE cells after treatment with kerosene soot (0.5-1.0 microg/cm(2)) for 66 h (36 MN/1000 cells). Combined treatment with chrysotile and soot induced up to 110 MN/1000 cells (chrysotile alone: 80 MN/1000 cells; concentrations: 1 microg/cm(2), exposure times: 66 h). Kinetochore staining revealed mainly clastogenic effects in all cases (soot: 21.3% CRMN(+); chrysotile: 27%; soot+chrysotile: 27.6%; control: 20.8%). This is the first study showing that kerosene soot is not only genotoxic but it can also elevate the genotoxic potential of chrysotile asbestos. This information may be of importance for workers occupationally exposed to asbestos and domestically exposed to kerosene soot.

Animals↗
PubMed2002

Extraction of polycyclic aromatic hydrocarbons from soot and sediment: solvent evaluation and implications for sorption mechanism.

Soot contains high levels of toxic compounds such as polycyclic aromatic hydrocarbons (PAHs). Extraction of PAHs from soot for quantitative analysis is difficult because the compounds are extremely tightly bound to the sorbent matrix. This study was designed to investigate the effect of solvent type on PAH extraction yield, to identify the most optimal solvent for PAH extraction from soot, and to gain insight into the mechanism of PAH sorption to soot in aquatic environments. To that end, different types of soot as well as coal, charcoal, and sediments containing soot-like material were extracted with seven organic solvents. Large differences in extraction recoveries were observed among solvents, with relative values as low as 16% as compared to the best extracting solvent. These differences were much larger for soot than for sediments. Dichloromethane, which to date is the most widely used solvent for soot and sediment extractions, appeared to be the overall worst extractant, whereas toluene/methanol (1:6) gave the best results. Based on extraction yields and solvent properties, extraction of PAHs from soot was explained by a two-step mechanism involving swelling of the sorbent matrix and subsequent displacement of sorbates by solvent molecules. Due to the low displacement capacity of water, desorption of PAHs from soot in the aquatic environment will be strongly limited. Moreover, a certain fraction of the total PAH mass on soot is suggested to be physically entrapped, making it unavailable for partitioning to the aqueous phase.

Carbon↗
PubMed2005

Laboratory investigation of heterogeneous interaction of sulfuric acid with soot.

The internal mixing state of soot with sulfuric acid is believed to significantly impact the optical, cloud-forming, and chemical properties of soot-containing aerosols, but little is known about the interaction between soot and sulfuric acid. We report the first measurements of the uptake of H2SO4 on three types of soot generated from methane, hexane, and kerosene combustion. H2SO4 loss on soot is found to be irreversible. The measured uptake coefficients are 0.018 +/- 0.007 for kerosene soot, 0.012 +/- 0.006 for methane soot, and 0.0076 +/- 0.0016 for hexane soot at a total pressure of 1-2 Torr and 298 K assuming a geometric surface area, likely corresponding to the upper limits. Additional experiments using the differential mobility analysis and Fourier transform infrared spectroscopy techniques are carried out to further characterize the interaction of H2SO4 with soot. The results suggest that uptake of H2SO4 takes place efficiently on soot particles, representing an important route to convert hydrophobic soot to hydrophilic aerosols.

Aerosols↗