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Propene production from ethene and methane using silver- and proton-exchanged zeolite catalysts

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JOURNAL OF THE JAPAN PETROLEUM INSTITUTE
卷 51, 期 4, 页码 205-216

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JAPAN PETROLEUM INST
DOI: 10.1627/jpi.51.205

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methane activation; propene production; silver-exchanged zeolite catalyst; ethene conversion; proton-exchanged zeolite catalyst

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Two new methods for the catalytic synthesis of propene using solid acid catalysts are presented. The first approach is a new method for the activation of methane, involving conversion of methane to propene over silver-exchanged zeolite in the presence of ethene. In the second method, ethene conversion proceeds directly and selectively over proton-exchanged zeolite under the control of a molecular sieving effect. The heterolytic dissociation of methane over silver cationic clusters (Ag-n(+)) in Ag+ -exchanged zeolites, leading to the formation of silver hydride (Ag-n-H) and CH(3)(delta+)species, which reacts with ethene to form propene around 673 K. Using C-13-labeled methane as a reactant, propene is shown to be a primary product from methane and ethene. Thus, a significant proportion of propene was singly C-13-labeled ((CC2H6)-C-13). Under these reaction conditions, H+-exchanged zeolites, such as H-ZSM-5 do not catalyze the methane conversion, only ethene being converted into higher hydrocarbons, such as propene. Ethene is selectively converted to propene over SAPO-34 at 723 K with a yield of 52.2% and selectivity of 73.3% at ethene conversion of 71.2%. The high and selective propene yields achieved over SAPO-34 can be attributed to a shape selectivity effect of the small-pore SAPO-34.

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