Polycyclic Aromatic Hydrocarbons Evaluation of Sources and Effects (1983) / Chapter Skim
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2 POLYCYLIC AROMATIC HYDROCARBONS FROM NATURAL AND STATIONARY SOURCES AND THEIR ATMOSPHERIC CONCENTRATIONS
2 POLYCYLIC AROMATIC HYDROCARBONS FROM NATURAL AND STATIONARY SOURCES AND THEIR ATMOSPHERIC CONCENTRATIONS
Pages 53-96
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From page 53... ...
as biologic monitors of aquatic pollution. The 1980 NRC report The International Mussel Watch31 described the program and gave the two general aims of the "watch": to produce information on the contamination of coastal ecosystems and food resources and global data on the abundance of anthropogenic contaminants.
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From page 54... ...
TABLE 2-1 Polycyclic Aromatic Hydrocarbons in Coal, Oil-Shale, and Petroleum Isolatesa Relative Peak Valuesb Coal Coal Petroleum PAHSynthoil C Syncrude D Shale B Mix A Fluorene5.3 9.9 2.2 3.9 9-Methylfluorene2 .0 1.
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From page 55... ...
TABLE 2-2 PAHs Resulting from Gasification of Western Coal, Coal Blend, Wood, and Peata ~Concentration, 1lg/g of feed stock North WyomingMont ana I 11.
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From page 56... ...
TABLE 2-3 Polycyclic Aromatic Hydrocarbons in Used Motor Oil Identified by Gas Chromatography-Mass Spectrometrya Compound Methylbiphenyl Methylbiphenyl Me thy lbiphenyl Fluorene Methylbiphenyl Methylb iphenyl Me thy lbiphenyl Methylf luorene Methylf luorene Me thy 1 f luorene Phenanthrene Deuterated anthraceneC Methyl f luorene D ime thy 1 f 1uorened Anthrac ene Dimethy lf luorened flethylphenan tl:~rene Methyl pl~e nanthrene Me thylphenanthrene Trimethylfluorenee Me thy lphenanthrene Trimethylfluorenee rirnethylf luorenee Phenylnaph thalene Tri~nethylf luorenee Trime thyl f 1uorenee Dimethylphenanthrened D ime t hy lphe nanthrene d D ime thy 1 phenantl~rened Hethylanthracene D ime thy 1 phe nan th r ened D imethylphenanthrened Me thylanthracene D imethy lphenanthrened F luoranthene Methylanthracene Ethylcyclopenta [clef ~ phenanthreneC Ethylcyclopenta [clef ~ phenanthreneC Trime thylphenanthrenee Pyrene l 1 ug/ml oi 1b 0.74 0.36 0.26 1.47 0.42 0.18 0.09 0.10 1.19 0.08 7.80 0.50 0.08 0.58 0.10 0.33 0.61 2.63 3.62 2.95 0.12 2.44 0.29 0.36 0.90 0.15 0.18 0.22 0.16 0.75 0.09 2.45 4.21 0.28 2.80 4.36 0.21 0.08 0.79 0.46 0.10 0.10 .
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From page 57... ...
Table 2-3 (cont. ~ C ompound Ethylcyclopenta [clef ]
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From page 58... ...
pyrene Perylene Hethylbenzofluoranthene MethylbenzopyreneJ Benzo[ghi] perylene gtml oilb 0.36 0.13 0.18 0.41 0.32 1.67 aReprinted with permission from White et al.;49 copyright Ann Arbor Science Publishers, Inc.
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From page 59... ...
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From page 63... ...
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From page 64... ...
TABLE 2-7 Summary of Average PAR Emission from Coal-Stoker-Fired Boilers With and Without Reinjection from the Stoker Dust Collectora Compound Concentrationb . Reinjected _ ~g/dry SCMC Without Reinject~on ~g/dry SCMC /kg of fuel ~g/kg of fuel Phenanthrene 9.60 66.0 9.40 76.0 Anthracene 0.29 2.0 8.50 68.0 Methylanthracenes/ 0.66 -- 0.84 phenanthrenes Fluoranthene 2.50 -- 8.60 Pyrene 0.86 -- 0.37 Methylpyrene/ 0.21 -- 0.12 fluorsnthene Benzo~ciphenan- 0.069 -- 0.093 threne Benz~aJanthracene 0.10 -- 0.07 Chrysene 0.15 ~0.12 Methylchrysenes 0.051 -- 0.059 Dimethylbenz- 0.028 -- -- anthracenes Benzofluoranthenes 0.13 -- 0.09 Benzote~pyrene 0.044 -- 0.047 Benzota~pyrene 0.039 -- 0.043 Perylene 0.036 -- 0.043 Indeno[1,2,3-cd]
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orseth;4 copyright Ann Arbor Sclence Publishers, Inc. hDetectable.
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From page 70... ...
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From page 71... ...
TABLE 2-11 POM Emission Factorsa Emission Factor, mg/k~ 0.12-m Logs, 0.82-kg/h Burn Rate Compounds Phenanthrene/anthracene 0.88 2.30 Cl-Phenanthrenes/anthracenes 0.42 0.18 C2-Phenanthrenes/anthracenes 0.11 0.04 Cyclopentaphenanthrenes/ ND ND anthracenes Pyrenes 0.33 . 1.39 Fluoranthene 0.25 0.10 Benzota~fluorene 0.26 0.26 Unidentified POMs 0.70 1.31 Cl-Fluoranthenes/pyrenes 0.10 ND Benzotghi~fluorene 0.04 0.10 9-Phenylanthracene 0.04 0.20 C3-Phenanthrenes/anthracenes 0.20 0.03 Benzo~ghi~fluoranthene ND ND C2-Pyrenes 0.08 ND Cyclopenta~cdipyrene ND ND Benzotc~phenanthrene ND ND Benz~aJanthracene/chrysene 0.44 1.35 Higher-molecular-weight POMs 0.25 1.26 Total 4.10 8.52 aAdapted from Hubble et al.16 bND = 0.06-m Logs, 7.
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From page 72... ...
TABLE 2-12 Estimation of Annual Emission of POM Contributed by Various Sourcesa Source Residential heating: Wood-fired (total) :b Coal-fired Oil-fired Gas-fired Open burning: Agriculture open burning Prescribed burning Forest wild fires Coal-refuse fires Land-clearing waste burning Structural fires Coke production Mobile sources: Auto -- gasoline Auto -- diesel Trucks -- diesel Industrial boilers: Coal Gas Oil Wood/bark ~agasse Annual Emission of Total POM , Metric tons % 3,837 102 7~4 9~8 1,190 1,071 1,478 28~5 171 86 632 2,160.8 1.2 103.5 69.0 2.1 1.3 1.2 0.3 34.8 0.9 0.1 0.1 10.8 9.7 13.4 0.3 1.6 0.8 5.7 19.6 0.1 0.9 6.3 0.1 0.1 0.1 0.1 aTabulated from Peters36 for the early to middle 1970s.
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From page 73... ...
TABLE 2-13 Emission of PAHs in Wood Smokea Emission, mg/kg of wood burned Fireplace Baffled Stove ~ ~ ~ Seasoned Seasoned Seasoned Nonbaffled Stove Seasoned Green PAR Oak Oak Pine Oak Pine Anthracene/ 8 75 146 62 103 phenanthrene Methyl~anthracenes/ 3 21 51 17 51 phenanthrenes) Fluoranthene <1 18 32 21 19 Pyrene <1 16 24 17 19 Methyl~fluoranthenes/ |
From page 74... ...
TABLE 2- 14 Emission Factors for PAHs from Residential Combustion Sources as a Function of Thermal Efficiencya Combustion Source Wood-burning stove 17 ,000 Wood-burning f ireplace 2,000 Automatic coal furnace 1,900 Oil furnace Gas furnace aData from Peters 36 . Approximate POM Emission Fac tor ~ pg/J ( fuel input)
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From page 76... ...
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From page 77... ...
TABLE 2-17 PAN Emission from a Secondary Lead Smelter Processing Batteriesa Emission Concentration,b ng/Nm] Compound 1A 1B 2A 2B Anthracene/phenanthrene 600 740 770 940 Methylanthracenes 25 34 41 33 Fluoranthene 160 170 330 310 Pyrene 31 22 28 30 Methylpyrenes/fluoranthenes Benzotc~phenanthrene Chrysene/benz~ajanthracene Benzo~aipyrene aData from Bennett et al.2 2 2 3 2 ~_ 10 11 17 13 25 23 28 25 1 1 1 1 bN = corrected to 70°F and 1 atm.
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From page 78... ...
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From page 79... ...
TABLE 2-19 Estimated Total Annual Benzo~aipyrene Emission for 1975 and 1985 Benz o~a~pyrene Emission, metric tons Estimate 19751985 Minimum 34667 Intermediate 588- 358 Maximum 1,676885 2-37 1
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From page 80... ...
Total PAH concentrations, in ng/m3: tunnel, 42.8 BaP; coke oven, 58.5 BaP and 44.2 BghiP; and ambient air, 1.01 BaP. Reprinted with permission from Miguel and Rubenich.24 2-38
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From page 81... ...
Cook. Emissions and Efficiency Performance of Industrial Coal Stoker Fired Boilers: Inorganic Trace Elements and Polynuclear Aromatic Hydrocarbons.
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From page 82... ...
Polynuclear Aromatic Hydrocarbons: 5th International Symposium -- Chemical Analysis and Biological Fate. Columbus, Ohio: Battelle Press, 1981.
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From page 83... ...
Polynuclear Aromatic Hydrocarbons: 5th International Symposium -- Chemical Analysis and Biological Fate. Columbus, Ohio: Battelle Press, 1981.
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From page 84... ...
Polynuclear Aromatic Hydrocarbons: 5th International Symposium -- Chemical Analysis and Biological Fate. Columbus, Ohio: Battelle Press, 1981.
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From page 85... ...
Some analytical aspects of the quantitative determination of polynuclear aromatic hydrocarbons in fugitive emissions from coal liquefaction processes, pp.
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From page 86... ...
Polynuclear Aromatic Hydrocarbons: 5th International Symposium -- Chemical Analysis and Biological Fate. Columbus, Ohio: Battelle Press, 1981.
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From page 87... ...
Pertinent information concerning the chemical and physical processes governing atmospheric persistence of PAHs is summarized first, followed by chemical reactions of PAHs, with an attempt to organize the somewhat conflicting published data according to reactant species and substrate, i.e., carrier particles and other substrates, including filters. PAH FORMATION: CHEMISTRY AND PHYSICS CHEMISTRY The exact synthetic chemistry that produces PAHs in a fuel-rich flame is not well known, but PAHs can be produced from almost any fuel burned under oxygen-deficient conditions.2 As an example of the PAH assemblage produced by combustion systems, Figure 3-1 (top)
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From page 88... ...
As the effluent temperature decreases, PAHs initially present largely as vapors become adsorbed on condensing carriers, such as soot and fly ash.3 ,67 It is generally accepted that the adsorption process is virtually completed at or near the point of emission into the ambient air, and that PAHs in ambient air are adsorbed on carrier particles. Studies of the distribution of selected PAHs between the gaseous and particulate phases in ambient airily have shown that, even though the smaller PAHs (e.g., with three and four aromatic rings)
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From page 89... ...
PHYSICAL REMOVAL PROCESSES FOR ATMOSPHERIC PAHs Once PAHs are released from the combustion system and adsorbed on soot or fly ash, they are exposed to potential atmospheric degradation. In the absence of major photodecomposition or other chemical transformations PAHs would be removed from the atmosphere by dry and wet deposition.7 Dry deposition involves sedimentation, turbulence-induced collision with surface electrostatic deposition, and inertial impaction.
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From page 90... ...
Assuming a constant wind speed of 4 m/s and constant wind direction over the 4-d period, this atmospheric residence time is equivalent to atmospheric transport over a distance of 1,400 km. Experimental evidence of such regional- and subcontinentalscale transport of PAHs in the atmosphere is discussed below.
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From page 91... ...
At that point, the total PAH concentration is about 100 ppb; remarkably, that is what is seen in almost all other samples from areas remote from urban centers. On the basis of these and other measurements of PAH concentrations, the following scenario is suggested for the transport of PAHs.
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From page 92... ...
With the observed PAH concentrations and information on the sedimentation rates and in situ dry densities, the fluxes of individual PAHs to five remote and three urban sites were calculated.32 Table 3-3 (top) shows the results of these flux calculations for core subsections reflecting PAH deposition in remote sites at present, in the interval including 1950, and at the turn of the century (1900)
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From page 93... ...
As seen in Table 3-4, PAH concentrations in air masses originating in industrialized areas in western Europe were 20 times higher than those measured in air masses originating in Norway and were as high as those typically measured in urban and industrial areas. These results support the concept, at least for the 20 PAHs listed in Table 3-4 and collected during the winter (i.e., low temperature and low light intensity, resulting in little, if any, photochemical activity)
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From page 94... ...
Later research has focused on BaP and a number of other PAHs; on photolysis and photooxidation, as well as on thermal reactions of PAHs with 03, NOX, and sulfur dioxide (SOLD; and on the influence of the physical and chemical nature of the substrate on the reactivity of adsorbed PAHs. The corresponding literature is somewhat conflicting, owing in part to the large number of characteristics that influence these complex and still only partially understood heterogeneous reactions.
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From page 95... ...
In all product studies cited above, exposure of adsorbed PAHs to NO2 at parts-per-million concentrations resulted in the formation of nitro-PAH derivatives. These are also listed in Table 3-6 and include mononitro as well as dinitro derivatives, the latter identified as nitration products of BaP42 and pyrene.37 In the study of Jager and Hanus,42 dinitroBaP was readily produced under conditions relevant to air pollution, i.e., by exposure of BaP adsorbed on fly ash to NO2 at 1.33 ppm for 4 h at 20°C.
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From page 96... ...
3~77' Two nitro-PAHs, 1-nitropyrene and 3-nitrofluoranthene, are carcinogenic in rats.69 The effect of substrate on the nitration of adsorbed PAHs has recently been investigated. Hughes et al.37 compared silica gel, alumina, and coal fly ash and noted that the extent of nitration of pyrene depends on the acidity of the substrate.
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