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Elemental Mercury Oxidation over Fe-Ti-Mn Spinel: Performance, Mechanism, and Reaction Kinetics
Shangchao Xiong1, Xin Xiao1, Nan Huang1
1Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology , Nanjing, 210094 P. R. China.
Abstract:
The design of a high-performance catalyst for Hg0 oxidation and predicting the extent of Hg0 oxidation are both extremely limited due to the uncertainties of the reaction mechanism and the reaction kinetics. In this work, Fe-Ti-Mn spinel was developed as a high-performance catalyst for Hg0 oxidation, and the reaction mechanism and the reaction kinetics of Hg0 oxidation over Fe-Ti-Mn spinel were studied. The reaction orders of Hg0 oxidation over Fe-Ti-Mn spinel with respect to gaseous Hg0 concentration and gaseous HCl concentration were approximately 1 and 0, respectively. Therefore, Hg0 oxidation over Fe-Ti-Mn spinel mainly followed the Eley-Rideal mechanism (i.e., the reaction of gaseous Hg0 with adsorbed HCl), and the rate of Hg0 oxidation mainly depended on Cl• concentration on the surface. As H2O, SO2, and NO not only inhibited Cl• formation on the surface but also interfered with the interface reaction between gaseous Hg0 and Cl• on the surface, Hg0 oxidation over Fe-Ti-Mn spinel was obviously inhibited in the presence of H2O, SO2, and NO. Furthermore, the extent of Hg0 oxidation over Fe-Ti-Mn spinel can be predicted according to the kinetic parameter kE-R, and the predicted result was consistent with the experimental result.
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