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Degradation kinetics of anthracene by ozone on mineral oxides
Authors:Jinzhu Ma  Yongchun Liu  Hong He
Institution:1. State Key Joint Laboratory of Environmental Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;2. Key Laboratory of Beijing on Regional Air Pollution Control, Beijing University of Technology, Beijing 100022, China;3. State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China;1. Beijing National Laboratory for Molecular Science (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.;2. Beijing National Laboratory for Molecular Science (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Peking University, Beijing 100871, China
Abstract:To further understand the role of substrates on the heterogeneous reactions of polycyclic aromatic hydrocarbons, the reactions of ozone with anthracene adsorbed on different mineral oxides (SiO2, α-Al2O3 and α-Fe2O3) and on Teflon disc were investigated in dark at 20 °C. No reaction between ozone and anthracene on Teflon disc was observed when the ozone concentration was ~1.18 × 1014 molecules cm?3. The reactions on mineral oxides exhibited pseudo-first-order kinetics for anthracene loss, and the pseudo-first-order rate constant (k1,obs) displayed a Langmuir–Hinshelwood dependence on the gas-phase ozone concentration. The adsorption equilibrium constants for ozone (KO3) on SiO2-1, SiO2-2, α-Al2O3 and α-Fe2O3 were (0.81 ± 0.26) × 10?15 cm3, (2.83 ± 1.17) × 10?15 cm3, (2.48 ± 0.77) × 10?15 cm3 and (1.66 ± 0.45) × 10?15 cm3, respectively; and the maximum pseudo-first-order rate constant (k1,max) on these oxides were (0.385 ± 0.058) s?1, (0.101 ± 0.0138) s?1, (0.0676 ± 0.0086) s?1 and (0.0457 ± 0.004) s?1, respectively. Anthraquinone was identified as the main surface product of anthracene reacted with ozone. Comparison with previous research and the results obtained in this study suggest that the reactivity of anthracene with ozone and the lifetimes of anthracene adsorbed on mineral dust in the atmosphere are determined by the nature of the substrate.
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