Low Temperature Catalytic Oxidation of Binary Mixture of Toluene and Acetone in the Presence of Ozone

Abstract

This work reports on gas phase catalytic ozonation of a binary mixture of toluene and acetone and compares it with catalytic ozonation of single component acetone and toluene. Catalytic ozonation was conducted at 25–90 °C on MnOx/γ-Al2O3 catalyst. XANES and EXAFS were used to identify formal oxidation state of Mn and local structure of manganese oxide in the catalyst. Absorption energy of Mn K-edge of the catalyst was determined to be 6553.86 eV indicating that the majority of manganese in the catalyst was in 3+ oxidation state. Catalytic ozonation in the mixture was favourable for removal of toluene, and repressive for removal of acetone. This was due to (a) lower apparent activation energy of catalytic ozonation of toluene (Ea, Toluene = 31 kJ mol−1 < Ea, Acetone = 40 kJ mol−1) that led to higher reactivity of toluene with active oxygen species, and (b) inhibitory effect of accumulated carbonaceous byproducts on the acetone removal. Increase of reaction temperature enhanced conversion of both compounds, decreased the gap between toluene and acetone conversions, and improved COx yield. Overall degradation pathway of toluene and acetone in the mixture was determined by identifying the reaction intermediates and carbonaceous deposits on the catalyst. The observed mixture effects helped to understand potentials and limitations of catalytic ozonation in treating mixture of VOCs, which will aid in developing commercial air treatment systems.