Synthesis, characterization and catalytic performance of metal-incorporated SAPO-34 for chloromethane transformation to light olefins

SAPO-34 and MeAPSO-34s (Me=Co, Mn, Fe) molecular sieves have been synthesized and used as catalysts for chloromethane transformation to light olefins. The influences created by metal incorporation are characterized with XRD, XRF, SEM, NMR, TG and H-2-TPR. The synthesized MeAPSO-34s have the same CHA topology structure, while metal incorporation gives rise to the increase of unit cell parameter and crystalline particle size. The coexistence of metal species in the synthesis starting gel has effect on the Si substitution into AlPO framework. Co, Mn or Fe incorporation generates a negligible difference on the chemical shift in P-31 and Al-27 MAS NMR. Si-29 MAS NMR study has demonstrated that metal incorporation favors the Si island formation, predicting the stronger acidity. The reducibility of metal species in the synthesized MeAPSO-34s has been investigated by H-2-TPR with the comparison of metal-impregnated SAPO-34. Two weight losses in TG analysis from template decomposition in diluted oxygen suggest different chemical location of template molecules in the molecular sieves. For MeAPSO-34, more template removal occurrence at high temperature range indicates stronger template-framework interaction and stronger acidity than SAPO-34 after calcinations. All the SAPO-34 and MeAPSO-34 molecular sieves are very active and selective catalyst for light olefins production. Metal incorporation improves the catalyst life and favors the ethylene and propylene generation. These catalytic properties enhancements are possibly related to the mechanism of chloromethane conversion with deposited coke species as reaction center. (c) 2007 Elsevier B.V. All rights reserved.