Zeolitic Framework Ta and MoO3 Confined in Beta Zeolite Cooperatively Enhance Activity and Stability for Oxidative Desulfurization.

Abstract

Oxidative desulfurization (ODS), as a novel desulfurization technique of fuel oil, possesses high desulfurization efficiency for aromatic sulfide and low cost, making it a promising approach. The key to the technology lies in the rational design of catalysts with high activity and stability. Polyoxometalates, which are environmentally friendly, cost-effective, and abundantly available, face constraints in the development of ODS applications due to their low specific surface area and difficulty in regeneration. Introducing metal oxides into carriers with large specific surface areas to obtain heterogeneous catalysts is an effective solution to this problem. Beta zeolites, with regular three-dimensional channel systems, large specific surface area, and superior thermal/hydrothermal stability, are usually used as carriers. In this work, we developed a strategy to enhance zeolite carrier utilization efficiency by introducing Ta⁵⁺ species into the rigid framework of zeolites containing confined MoO₃. The Ta species in the zeolite framework and the confined MoO₃ produce a synergistic effect, exhibiting extremely high catalytic activity for the aerobic oxidative desulfurization of various organic aromatic sulfur compounds under mild conditions (90 °C and atmospheric pressure) in a deep eutectic solvent, surpassing common heterogeneous catalysts for oxidative desulfurization. Moreover, it can resist the adverse effects of interferents, such as naphthalene and indole. Additionally, the confined nature of Beta zeolite endows it with exceptional stability, demonstrating distinctive recyclability.