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Role of support nature (γ-Al_2O_3 and SiO_2-Al_2O_3) on the performances of rhenium oxide catalysts in the metathesis of ethylene and 2-pentene

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Journal of Natural Gas Chemistry 2012年第2期21卷 158-164页

作者： Weena Phongsawat Benjamas Netiworaruksa Kongkiat Suriye Siraprapha Dokjampa Piyasan Praserthdam Joongjai Panpranot Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical Engineering Faculty of Engineering Chulalongkorn University SCG Chemicals CO. Ltd. 1 Siam Cement Rd. Bangsue Bangkok 10800 Thailand

The metathesis of ethylene and 2-pentene was studied as an alternative route for propylene production over Re2O7/γ-Al2O3 and Re2O7/SiO2-Al2O3 catalysts. Both NH3 temperature-programmed desorption （NH3-TPD） and H2 temperature-programmed reduction （H2-TPR） results showed that Re2O7/SiO2-Al2O3 exhibited stronger acidity and weaker metal-support interaction than Re2O7/γ-Al2O3. At 35 60℃, isomerization free metathesis was observed only over Re2O7/γ-Al2O3, suggesting that the formation of metal-carbene metathesis active sites required only weak acidity. Our results suggest that on the Re2O7/SiO2-Al2O3, hydrido-rhenium species （[Re]-H） were formed in addition to the metathesis active sites, resulting in the isomerization of the initial 1-butene product into 2-butenes. A subsequent secondary metathesis reaction between these 2-butenes and the excess ethylene could explain the enhanced yields of propylene observed. The results demonstrate the potential for high yield of propylene from alternative feedstocks.

关键词： metathesis isomerization propylene production 2-pentene rhenium

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Production of propylene from an unconventional metathesis of ethylene and 2-pentene over Re_2O_7/SiO_2-Al_2O_3 catalysts

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Journal of Natural Gas Chemistry 2012年第1期21卷 83-90页

作者： Weena Phongsawat Benjamas Netivorruksa Kongkiat Suriye Siraprapha Dokjampa Piyasan Praserthdam Joongjai Panpranot Center of Excellence on Catalysis and Catalytic Reaction Engineering Department of Chemical Engineering Faculty of Engineering Chulalongkorn University SCG Chemicals CO. LTD. 1 Siam Cement Rd. Bangsue Bangkok 10800 Thailand

An unconventional metathesis of ethylene and 2-pentene over Re2O7/SiO2-A1203 catalysts has been studied as an alternative route for the production of propylene. Complete conversion of 2-pentene and propylene yield as high as 88 wt% were obtained under mild reaction conditions at 35 ℃ and atmospheric pressure. Unlike the conventional metathesis of ethylene and 2-butenes in which isomerization is a competing side reaction, the isomerization of 1-butene product from the unconventional metathesis of ethylene and 2-pentene to 2-butenes can further react with excess ethylene in the feed, resulting in additional increase in propylene yield. The secondary metathesis reaction was found to be favored under ethylene/2-pentene （E/2P） molar ratio ≥3 and gas hourly space velocity （GHSV） ≤ 1000 h-1 at the reaction temperature of 35 ℃. No catalyst deactivation was observed during the 455 min time-on-stream under the selected reaction conditions.

关键词： metathesis propylene production 2-pentene rhenium silica-alumina

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