Mechanism of catalytic oxidation of toluene by copper–manganese bimetallic doped ZSM-5
摘要
In this study, a series of Cu–Mn modified ZSM-5 zeolites (CuxMny/ZSM-5) were synthesized via the solgel method to investigate their catalytic oxidation performance towards toluene. The influence of Cu–Mn modification on the catalytic oxidation of toluene was systematically examined using various characterization techniques, including XRD, FTIR, BET, XRF, XPS, and TEM. The results indicated that CuxMny/ZSM-5 maintained the complete framework characteristics of ZSM-5 zeolites and possessed a hierarchical pore structure with pore size distribution dominated by micropores and mesopores. The highly dispersed CuxMny on ZSM-5 significantly enhanced the relative content of surface Cu+ and Mn3+ species, with the presence of Cu+ facilitating the formation of oxygen vacancies. More oxygen vacancies can significantly improve the oxygen migration rate and thus enhance the catalytic oxidation activity. Among them, Cu0.5Mn0.5/ZSM-5 exhibited a higher proportion of low-valence Mn, low-valence Cu, and adsorbed oxygen (Oads), which is beneficial for the low-temperature catalytic oxidation of toluene. The evaluation of the catalytic oxidation performance towards toluene showed that Cu0.5Mn0.5/S-0.1 had the best catalytic effect, with the lowest apparent activation energy of 131.19 kJ mol−1 and a T90 of 256 °C. This research provides a new approach for the development of catalysts for the low-temperature catalytic oxidation of toluene.