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Effect of surface hydroxyls on dimethyl ether synthesis over the γ-Al2O3 in liquid paraffin: a computational study

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Abstract

In a recent paper (Zuo et al., Appl Catal A 408:130–136, 2011), the mechanism of dimethyl ether (DME) synthesis from methanol dehydration over γ-Al2O3 (110) was studied using density functional theory (DFT). Using the same method, the effect of surface hydroxyls on γ-Al2O3 in liquid paraffin during DME synthesis from methanol dehydration is investigated. It is found that DME is mainly formed from two adsorbed CH3O groups via methanol dehydrogenation on both dehydrated and hydrated γ-Al2O3 in liquid paraffin. No close correlation between catalytic activity and acid intensity was found. Before and after water adsorption at typical catalytic conditions (e.g., 553 K), the reaction rate is not obviously changed on γ-Al2O3(100) surface in liquid paraffin, but the reaction rate decreases by about 11 times on the (110) in liquid paraffin. Considering the area of the (110) and (100) surfaces under actual conditions, the catalytic activity decreased mainly because the Al3 sites on the (110) surface gradually become inactive. Catalytic activity decreased mainly due to surface hydrophilicity. The calculated results were consistent with the experiment.

The reaction rate decreases by about 11 times on the (110)/liquid paraffin interface before and after water adsorption at typical catalytic conditions (e.g., 553 K).

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Acknowledgments

The authors gratefully acknowledge the financial support of this study by the National Natural Science Foundation of China (Grant No.20676087), China Postdoctoral Science Foundation Funded Project (Grant No.2012M510784), Shanxi Province Science Foundation for Youths (Grant No.012021005-1), Natural Science Foundation of Shanxi Province (Grant No. 2012011046–1), Special/Youth Foundation of Taiyuan University of Technology (No. 2012L042). The authors especially thank for two anonymous reviewers for their valuable suggestions on the quality improvement of our present paper.

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  1. Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan, Shanxi, China

    Zhi-jun Zuo, Le Wang & Wei Huang

  2. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan, 030024, Shanxi, China

    Pei-de Han

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  1. Zhi-jun Zuo
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Correspondence to Wei Huang.

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Zuo, Zj., Wang, L., Han, Pd. et al. Effect of surface hydroxyls on dimethyl ether synthesis over the γ-Al2O3 in liquid paraffin: a computational study. J Mol Model 19, 4959–4967 (2013). https://doi.org/10.1007/s00894-013-1993-7

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