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Formation of Phenoxy-type Environmental Persistent Free Radicals (EPFRs) from Dissociative Adsorption of Phenol on Cu/Fe and their Partial Oxides
Journal article   Open access   Peer reviewed

Formation of Phenoxy-type Environmental Persistent Free Radicals (EPFRs) from Dissociative Adsorption of Phenol on Cu/Fe and their Partial Oxides

O.H. Ahmed, M. Altarawneh, M. Al-Harahsheh, Z-T Jiang and B.Z. Dlugogorski
Chemosphere, Vol.240
2019
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Abstract

The interplay of phenolic molecules with 3d transition metals, such as Fe and Cu, and their oxide surfaces, provide important fingerprints for environmental burdens associated with thermal recycling of e-waste and subsequent generation of notorious dioxins compounds and phenoxy-type Environmental Persistent Free Radicals (EPFRs). DRIFTS and EPR measurements established a strong interaction of the phenol molecule with transition metal oxides via synthesis of phenolic- and catecholic-type EPFRs intermediates. In this contribution, we comparatively examined the dissociative adsorption of a phenol molecule, as the simplest model for phenolic-type compounds, on Cu and Fe surfaces and their partially oxidized configurations through accurate density functional theory (DFT) studies. The underlying aim is to elucidate the specific underpinning mechanism forming phenoxy- or phenolate-type EFPRs. Simulated results show that, the phenol molecule undergoes fission of its hydroxyl’s O-H bond via accessible activation energies. These values are lower by 46.5 - 74.1% when compared with the analogous gas phase value. Physisorbed molecules of phenol incur very low binding energies in the range of -2.1 - -5.5 over clean Cu/Fe and their oxides surfaces. Molecular attributes based on charge transfer and geometrical features are in accord with the very weak interaction in physisorbed states. Thermo-kinetic parameters established over the temperature region of 300 and 1000 K, exhibit a lower activation energy for scission of phenolic’s O-H bonds over the oxide surfaces in reference to their pure surfaces (24.7 and 43.0 kcal mol-1 vs 38.4 and 47.0 kcal mol-1).

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8 Earth Sciences
8.124 Environmental Sciences
8.124.552 Air Pollution
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Environmental Sciences
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Environment/Ecology
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