Polychlorinated Benzene, Phenol, Dibenzo-p-dioxin, and Dibenzofuran in Heterogeneous Combustion Reactions of Acetylene
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Abstract
Acetylene was reacted with HCl/air under heterogeneous combustion conditions between 300 and 600 °C. Model catalyst mixtures of SiO2/metal oxides (Al2O3, Fe2O3, TiO2, and CuO) were compared with municipal waste incinerator (MWI) fly ash. Chlorinated benzenes (ClxBz), chlorinated phenols (ClxPh), and PCDD/F were detected in both gas-phase products as well as catalyst-adsorbed products. ClxBz production increased exponentially to 600 °C (HCB: 4 × 104 ng/g of C2H2), while ClxPh production (2.5 × 104 ng/g of C2H2) was maximized at 500 °C (ca. 104−105 ng/g of C2H2). PCDF displayed a dramatic peak at 500 °C (TCDF: 2 × 106 pg/g of C2H2), in contrast to the generally accepted de novo and aromatic precursor formation temperature of 300 °C. Comparison of gas-phase ClxBz congener distribution patterns revealed that the CuO-catalyzed reaction closely matched the ClxBz pattern produced in the reactions with MWI fly ash, providing further evidence of the importance of Cu in the fly ash matrix. Comparison of fly ash-catalyzed gas-phase ClxBz with MWI flue gas and 300 °C de novo synthesized ClxBz demonstrated the relevance of mid-temperature (600 °C) heterogeneous combustion reactions of C2 aliphatics in real combustion systems.
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