Yuji Shinohara, T. Nakajima, Satoshi Suzuki, S. Mishima, H. Ishikawa
{"title":"乙醇在氧化物催化剂上脱水脱氢的计算化学研究","authors":"Yuji Shinohara, T. Nakajima, Satoshi Suzuki, S. Mishima, H. Ishikawa","doi":"10.2477/JCHEMSOFT.4.89","DOIUrl":null,"url":null,"abstract":"A computational chemical investigation has been made into the mechanisms of the dehydration and the dehydrogenation of ethanol on six oxide catalysts (SiO2, TiO2, ZnO, MnO, MgO and CdO) using the DV-Xα method. Transition state models of the consecutive mechanism including ethoxide formation and the concerted mechanism proposed by Eucken and Wicke were computed.By comparing the computed results with experimental ones published in the literature, it was concluded that the consecutive mechanism is more reasonable than the concerted one. It was also concluded that the rate-determing step of the ethanol dehydration is for a β-hydrogen shift to a surface oxide ion and that the ease of theshift is a factor controlling the dehydration/ dehydrogenation selectivities of oxide catalysts.","PeriodicalId":205210,"journal":{"name":"Journal of Chemical Software","volume":"27 1","pages":"0"},"PeriodicalIF":0.0000,"publicationDate":"1998-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"9","resultStr":"{\"title\":\"A Computational Chemical Investigation of the Dehydration and Dehydrogenation of Ethanol on Oxide Catalysts\",\"authors\":\"Yuji Shinohara, T. Nakajima, Satoshi Suzuki, S. Mishima, H. Ishikawa\",\"doi\":\"10.2477/JCHEMSOFT.4.89\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"A computational chemical investigation has been made into the mechanisms of the dehydration and the dehydrogenation of ethanol on six oxide catalysts (SiO2, TiO2, ZnO, MnO, MgO and CdO) using the DV-Xα method. Transition state models of the consecutive mechanism including ethoxide formation and the concerted mechanism proposed by Eucken and Wicke were computed.By comparing the computed results with experimental ones published in the literature, it was concluded that the consecutive mechanism is more reasonable than the concerted one. It was also concluded that the rate-determing step of the ethanol dehydration is for a β-hydrogen shift to a surface oxide ion and that the ease of theshift is a factor controlling the dehydration/ dehydrogenation selectivities of oxide catalysts.\",\"PeriodicalId\":205210,\"journal\":{\"name\":\"Journal of Chemical Software\",\"volume\":\"27 1\",\"pages\":\"0\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"1998-09-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"9\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Chemical Software\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.2477/JCHEMSOFT.4.89\",\"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 Chemical Software","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.2477/JCHEMSOFT.4.89","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
A Computational Chemical Investigation of the Dehydration and Dehydrogenation of Ethanol on Oxide Catalysts
A computational chemical investigation has been made into the mechanisms of the dehydration and the dehydrogenation of ethanol on six oxide catalysts (SiO2, TiO2, ZnO, MnO, MgO and CdO) using the DV-Xα method. Transition state models of the consecutive mechanism including ethoxide formation and the concerted mechanism proposed by Eucken and Wicke were computed.By comparing the computed results with experimental ones published in the literature, it was concluded that the consecutive mechanism is more reasonable than the concerted one. It was also concluded that the rate-determing step of the ethanol dehydration is for a β-hydrogen shift to a surface oxide ion and that the ease of theshift is a factor controlling the dehydration/ dehydrogenation selectivities of oxide catalysts.