Insight into the catalytic oxidation of toluene over M/ZSM-5 (M=Cu, Mn, Fe, Ce, Ti) catalysts

Abstract

A series of metal oxide catalysts were prepared by impregnating Cu, Mn, Fe, Ce and Ti on ZSM-5 molecular sieve. The physicochemical properties of the catalysts were characterized by SEM, XRD, N₂ adsorption/desorption, XPS, H₂-TPR, and the catalytic oxidation of toluene was investigated. The results showed that Cu/ZSM-5 had rough surface, uniform distribution of metal, good pore structure, superior low-temperature reducibility and abundant adsorbed oxygen species. Cu/ZSM-5 with 5% loading exhibited excellent catalytic activity for toluene oxidation and the best sulfur resistance performance, with t₉₀ (GHSV=24000 h⁻¹) being 224 °C in SO₂ environment. In-situ DRIFTS experiments revealed that the degradation path of toluene was as follows: toluene was first adsorbed on the surface of the catalyst to form adsorbed toluene, then it was converted into benzaldehyde and benzoic acid successively on the catalyst. And small molecule organics such as maleic acid and carboxylic acid were formed through ring opening reaction, and finally was oxidized to CO₂ and H₂O.