乙醇在氧化物催化剂上脱水脱氢的计算化学研究

Yuji Shinohara, T. Nakajima, Satoshi Suzuki, S. Mishima, H. Ishikawa
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引用次数: 9

摘要

采用DV-Xα方法对6种氧化物催化剂(SiO2、TiO2、ZnO、MnO、MgO和CdO)对乙醇的脱水和脱氢机理进行了计算化学研究。计算了Eucken和Wicke提出的乙氧化物形成连续机理和协同机理的过渡态模型。将计算结果与文献中发表的实验结果进行比较,得出连续机制比协调机制更合理的结论。还得出了乙醇脱水的速率决定步骤是β-氢向表面氧化离子的转移,而转移的难易程度是控制氧化物催化剂脱水/脱氢选择性的一个因素。
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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.
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