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

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.

• Authors: Zhi-Jun Zuo, Le Wang, Pei-de Han, Wei Huang
• Journal: Journal of molecular modeling (J Mol Model) Vol. 19 Issue 11 Pg. 4959-67 (Nov 2013) ISSN: 0948-5023 [Electronic] Germany
• PMID: 24057976 (Publication Type: Journal Article, Research Support, Non-U.S. Gov't)