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Photolysis of polycyclic aromatic hydrocarbons adsorbed on fly ash

Thesis/Dissertation ·
OSTI ID:5413213
Polycyclic aromatic hydrocarbons (PAH) are formed by the combustion of almost any fuel under oxygen-deficient conditions. Previous laboratory studies have found that many PAH degrade with lifetimes as short as a few hours; however, studies of marine and lacustrine sediments, the ultimate sinks of PAH, have shown relative abundances of PAH which are similar to those in combustion sources; this suggests that PAH are stable in the atmosphere. Eighteen PAH adsorbed on carbon black and fifteen coal fly ashes of varying physical and chemical composition were photolyzed in order to study their atmospheric fate. Photolytic half-lives for these particle-bound PAH were found to be highly dependent on the substrate onto which they were adsorbed. On low-carbon fly ash, PAH showed a wide range of half-lives, indicating a relationship between PAH structure and photochemical reactivity. However, PAH on carbon black and fly ashes with a high-carbon content, show similar half-lives for most PAH including reactive PAH such as anthracene and benzo(a)pyrene. This indicates a photolytic process that is independent of structure and dependent on the physical and chemical nature of the fly ash. Surprisingly, no other parameter accounts for observed PAH reactivity. Substrate characteristics such as surface area, porosity, particle size, surface pH, and iron content have all been suggested to influence the rate of PAH degradation. However, these parameters, measured for substrates studied in this thesis, do not correlate with PAH reactivity. Because carbon black and high-carbon fly ashes stabilize reactive PAH, it is these substrates which would facilitate the transport of PAH from combustion sources through the atmosphere to ultimate sinks.
Research Organization:
Indiana Univ., Bloomington (USA)
OSTI ID:
5413213
Country of Publication:
United States
Language:
English