Characterization of metal-containing molecular sieves and their catalytic properties in the selective oxidation of cyclohexane

• Published in: Catalysis today 2004-09, Vol.93, p.735-742
• Main Authors: Tian, Peng, Liu, Zhongmin, Wu, Zongbin, Xu, Lei, He, Yanli
• Format: Article
• Language: English
• Subjects: Catalysis; Characterization; Chemistry; Colloidal state and disperse state; Cyclohexane; Exact sciences and technology; General and physical chemistry; Metal-containing molecular sieve; Microporous aluminophosphate; Oxidation; Porous materials; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
• ISSN: 0920-5861; 1873-4308
• DOI: 10.1016/j.cattod.2004.06.100

Three types of metal-containing molecular sieves with AFI, AEL and CHA structures (Me=Co, Mn, Cr and V) were synthesized hydrothermally and characterized by XRD, XRF, TG, TPR, NH 3-TPD and FT-IR. It was revealed that metals were incorporated into the framework of molecular sieves and induced the presence of charge centers. Both cobalt and manganese in the framework of AlPO-5, AlPO-11 and SAPO-34 were not reducible before the structure collapse. The redox behaviours of these catalysts in cyclohexane oxidation at 403 K using O 2 as oxidant were examined. CoAPO-11 exhibited best activity and good selectivities for the monofunctional oxidation products (88.5%). Cyclohexanol was the major product over most catalysts, whereas for Cr-containing molecular sieves, high selectivity of cyclohexanone was observed. Investigation of reaction mechanism based on CoAPO-11 and CrAPO-5 catalysts indicated that the decomposition of cyclohexyl hydroperoxide (CHHP), the intermediate in cyclohexane oxidation, followed the pathway: cyclohexanone ← CHHP → cyclohexanol → cyclohexanone.