To promote catalytic ozonation of toluene by tuning Brönsted acid sites via introducing alkali metals into the OMS-2-SO42-/ZSM-5 catalyst

Abstract

Although free hydroxyl radical (·OH) generated on OMS-2-based catalysts during the catalytic ozonation process have been shown as important reactive oxygen species (ROSs) for toluene degradation, improvement of surface ·OH formation ability remains challenging. Here, Na, K, Rb, and Cs-OMS-2-SO42-/ZSM-5 catalysts were prepared, characterized and evaluated for catalytic ozonation of toluene. Both characterizations and DFT calculations showed that the appropriate alkali metal introduction made the catalyst possess with appropriate crystalline, reducibility, and acidity, which was favorable for catalytic ozonation of toluene. Characterizations also showed that alkali metal introduction resulted in water molecule adsorption on Brönsted acid sites of the catalysts, which made water molecule activation by ozone to form ·OH more easily. The introduction of K+ content of ∼ 5.9 wt% yielded K-OMS-2-SO42-/ZSM-5 catalyst with the highest Brönsted acid sites and thus formed the most ·OH among the five prepared catalysts. As a result, the catalyst exhibited excellent toluene conversion and COx selectivity for catalytic ozonation of toluene at room temperature and ambient humidity. Furthermore, the catalytic activity of deactivated K-OMS-2-SO42-/ZSM-5 catalyst was recovered after regeneration by a combination of water washing and heat treatment. Finally, a complete mechanism for toluene catalytic ozonation, catalyst deactivation, and regeneration was proposed.