One-Step Cyclohexane Nitrosation to ε-Caprolactam over Metal Substituted AlPO-5

doi:10.1016/S1872-2067(11)60354-9

Abstract

Abstract: Crystalline AlPO-5, SAPO-5, and metal substituted AlPO-5 (MeAlPOs) were prepared by the hydrothermal method and characterized by X-ray diffraction, N₂ adsorption-desorption, scanning electron microscopy, particle size distribution, inductively coupled plasma (ICP) spectroscopy, Fourier transform infrared (FT-IR) spectroscopy, NH₃ temperature-programmed desorption (TPD), H₂ temperature-programmed reduction, and thermogravimetric-differential thermogravimetric (TG-DTG) analysis. All the samples crystallized with the AFI structure. TPD profiles showed that stronger Brønsted acid sites appeared and the number of Lewis acid sites increased when Si or a metal was introduced into the framework of AlPO-5. ICP, FT-IR spectra, and TG-DTG curves confirmed that Si or the metals were incorporated into the framework of the AlPO-5. The catalytic properties of the samples in cyclohexane nitrosation to ε-caprolactam were studied. SAPO-5 with a larger BET surface area, more Lewis acid sites, and stronger Brønsted acid sites gave better activity and selectivity than AlPO-5. Among the MeAlPOs, CrAPO-5 with the larger BET surface area, more Lewis acid sites, and stronger Brønsted acid sites gave the better result with a conversion of 8.16% and ε-caprolactam selectivity of 68.17%.

Key words: metal substituted aluminophosphate molecular sieve, ε-caprolactam, cyclohexane, one-step method, nitrosation

HAO Fang, ZHONG Jun, LIU Ping-Le, YOU Kui-Yi, WEI Chao, LUO He-An. One-Step Cyclohexane Nitrosation to ε-Caprolactam over Metal Substituted AlPO-5[J]. Chinese Journal of Catalysis, 2012, 33(4): 670-676.

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