Catalytic Enhancement of Cyclohexene Hydration by Ga-Doped ZSM-5 Zeolites

Abstract

Ga-doped ZSM-5 zeolites were directly synthesized by a facile one-step hydrothermal method without organic templates and calcination and then investigated in the cyclohexene hydration reaction. The structure, component, textural properties, and acidity of the as-prepared samples were examined by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray fluorescence (XRF), Brunauer–Emmett–Teller (BET), ammonia temperature-programmed desorption (NH3-TPD), pyridine-chemisorbed IR (Py-IR), and 71Ga, 27Al, 29Si, and 1H magic-angle spinning (MAS) NMR techniques. The characterization results showed that the introduction of Ga atoms into the ZSM-5 zeolite framework is much easier than Al atoms and beneficial to promote the formation of small-sized crystals. The number of Brønsted acid sites of Ga-doped ZSM-5 samples obviously increased compared with Ga0-ZSM-5. Additionally, the highest cyclohexanol yield (10.1%) was achieved over the Ga3-ZSM-5 sample, while the cyclohexanol yield of the Ga0-ZSM-5 sample was 8.6%. This result indicated that the improved catalytic performance is related to its larger external surface area, smaller particle size, and more Brønsted acid sites derived from Si–OH–Al and Si–OH–Ga of Ga3-ZSM-5. Notably, the green route reduces harmful gas emission and provides a basis for doping other heteroatoms to regulate the catalytic performance of zeolites, especially in industrial production.