{"title":"载体性质(γ-Al2O3和SiO2-Al2O3)对氧化铼催化剂乙烯和2-戊烯反应性能的影响","authors":"Weena Phongsawat , Benjamas Netiworaruksa , Kongkiat Suriye , Siraprapha Dokjampa , Piyasan Praserthdam , Joongjai Panpranot","doi":"10.1016/S1003-9953(11)60348-4","DOIUrl":null,"url":null,"abstract":"<div><p>The metathesis of ethylene and 2-pentene was studied as an alternative route for propylene production over Re<sub>2</sub>O<sub>7</sub>/γ-Al<sub>2</sub>O<sub>3</sub> and Re<sub>2</sub>O<sub>7</sub>/SiO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub> catalysts. Both NH<sub>3</sub> temperature-programmed desorption (NH<sub>3</sub>-TPD) and H<sub>2</sub> temperature-programmed reduction (H<sub>2</sub>-TPR) results showed that Re<sub>2</sub>O<sub>7</sub>/SiO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub> exhibited stronger acidity and weaker metal-support interaction than Re<sub>2</sub>O<sub>7</sub>/γ-Al<sub>2</sub>O<sub>3</sub>. At 35–60 °C, isomerization free metathesis was observed only over Re<sub>2</sub>O<sub>7</sub>/γ-Al<sub>2</sub>O<sub>3</sub>, suggesting that the formation of metal-carbene metathesis active sites required only weak acidity. Our results suggest that on the Re<sub>2</sub>O<sub>7</sub>/SiO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub>, 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.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 2","pages":"Pages 158-164"},"PeriodicalIF":0.0000,"publicationDate":"2012-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60348-4","citationCount":"19","resultStr":"{\"title\":\"Role of support nature (γ-Al2O3 and SiO2-Al2O3) on the performances of rhenium oxide catalysts in the metathesis of ethylene and 2-pentene\",\"authors\":\"Weena Phongsawat , Benjamas Netiworaruksa , Kongkiat Suriye , Siraprapha Dokjampa , Piyasan Praserthdam , Joongjai Panpranot\",\"doi\":\"10.1016/S1003-9953(11)60348-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The metathesis of ethylene and 2-pentene was studied as an alternative route for propylene production over Re<sub>2</sub>O<sub>7</sub>/γ-Al<sub>2</sub>O<sub>3</sub> and Re<sub>2</sub>O<sub>7</sub>/SiO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub> catalysts. Both NH<sub>3</sub> temperature-programmed desorption (NH<sub>3</sub>-TPD) and H<sub>2</sub> temperature-programmed reduction (H<sub>2</sub>-TPR) results showed that Re<sub>2</sub>O<sub>7</sub>/SiO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub> exhibited stronger acidity and weaker metal-support interaction than Re<sub>2</sub>O<sub>7</sub>/γ-Al<sub>2</sub>O<sub>3</sub>. At 35–60 °C, isomerization free metathesis was observed only over Re<sub>2</sub>O<sub>7</sub>/γ-Al<sub>2</sub>O<sub>3</sub>, suggesting that the formation of metal-carbene metathesis active sites required only weak acidity. Our results suggest that on the Re<sub>2</sub>O<sub>7</sub>/SiO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub>, 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.</p></div>\",\"PeriodicalId\":56116,\"journal\":{\"name\":\"Journal of Natural Gas Chemistry\",\"volume\":\"21 2\",\"pages\":\"Pages 158-164\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2012-03-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60348-4\",\"citationCount\":\"19\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Natural Gas Chemistry\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1003995311603484\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Natural Gas Chemistry","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1003995311603484","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Role of support nature (γ-Al2O3 and SiO2-Al2O3) on the performances of rhenium oxide catalysts in the metathesis of ethylene and 2-pentene
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 °C, 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.
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