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

ACS Omega. 2022 Jul 19;7(30):26289-26297. doi: 10.1021/acsomega.2c02031. eCollection 2022 Aug 2.

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.