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纳米晶χ-和γ-氧化铝催化剂上乙醇催化脱水制乙烯

Catalytic Ethanol Dehydration to Ethylene over Nanocrystalline χ- and γ-AlO Catalysts.

作者信息

Janlamool Jakrapan, Jongsomjit Bunjerd

机构信息

Center of Excellence on Catalysis and Catalytic Reaction Engineering, Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University.

出版信息

J Oleo Sci. 2017;66(9):1029-1039. doi: 10.5650/jos.ess17026.

Abstract

The study is aimed to investigate the combination of nanocrystalline γ- and χ- alumina that displays the attractive chemical and physical properties for the catalytic dehydration of ethanol. The correlation between the acid density and ethanol conversion was observed. The high acid density apparently results in high catalytic activity, especially for the equally mixed γ- and χ- phase alumina (G50C50). In order to obtain a better understanding on how different catalysts would affect the ethylene yield, one of the most powerful techniques such as X-ray photoelectron spectroscopy (XPS) was performed. Hence, the different O 1s surface atoms can be identified and divided into three types including lattice oxygen (O, 530.7 eV), surface hydroxyl (OH, 532.1 eV) and lattice water (HO, 532.9 eV). It was remarkably found that the large amount of O 1s surface atoms in lattice water can result in increased ethylene yield. In summary, the appearance of metastable χ-alumina structure exhibited better catalytic activity and ethylene yield than γ- alumina. Thus, the introduction of metastable χ- alumina structure into γ- alumina enhanced catalytic activity and ethylene yield. As the result, it was found that the G50C50 catalyst exhibits the ethylene yield (80%) at the lowest reaction temperature ca. 250°C among other catalysts.

摘要

本研究旨在探究纳米晶γ-氧化铝和χ-氧化铝的组合,该组合对乙醇催化脱水显示出有吸引力的化学和物理性质。观察到酸密度与乙醇转化率之间的相关性。高酸密度显然会导致高催化活性,尤其是对于γ-和χ-相氧化铝等量混合的情况(G50C50)。为了更好地理解不同催化剂如何影响乙烯产率,采用了最强大的技术之一,如X射线光电子能谱(XPS)。因此,可以识别不同的O 1s表面原子,并将其分为三种类型,包括晶格氧(O,530.7 eV)、表面羟基(OH,532.1 eV)和晶格水(HO,532.9 eV)。值得注意的是,发现晶格水中大量的O 1s表面原子会导致乙烯产率增加。总之,亚稳态χ-氧化铝结构的出现比γ-氧化铝表现出更好的催化活性和乙烯产率。因此,将亚稳态χ-氧化铝结构引入γ-氧化铝中可提高催化活性和乙烯产率。结果发现,在其他催化剂中,G50C50催化剂在约250°C的最低反应温度下表现出80%的乙烯产率。

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