Initial Decomposition of Methanol and Water on In2O3(110): A Periodic DFT Study
Initial Decomposition of Methanol and Water on In2O3(110): A Periodic DFT Study
复制标题
In2O3(110) 上甲醇和水的初始分解：定期 DFT 研究
DOI：
10.1002/cjoc.201200714
复制
发表时间：
2012-09-01
影响因子：
5.4
通讯作者：
Xie Daiqian
中科院分区：
文献类型：
--
作者：
Lin Sen;Xie Daiqian
认为纯In_2O_3是一种高效的甲醇水蒸气重整催化剂。尽管在过去的几十年里进行了多项研究，但MSR对In_2O_3的作用机理仍不完全清楚。本文用周期密度泛函理论研究了甲醇和水在In_2O_3(110)表面的初始解离过程。报道了几个基本步骤的活化势垒和热化学。研究发现，在表面In-O配位上，CH3OH和H2O的氢键断裂生成CH3O和OH物种的势垒很低，这表明In_2O_3(110)在低温下可以很容易地催化这两个重要过程。此外，随后的CH3O脱氢为CH2O的反应也是以低势垒进行的。
Pure In2O3 is considered as an efficient methanol steam reforming catalyst. Despite of several studies in the past decades, the mechanism of MSR on In2O3 is still not fully understood. In this work, a periodic density functional theory study of the initial dissociation of methanol and water over the In2O3 (110) surface is presented. The activation energy barriers and thermochemistry for several elementary steps are reported. It is found that the energy barriers for OH bond cleavage of both CH3OH and H2O to produce CH3O and OH species at a surface In-O pair site are very low, indicating that In2O3 (110) can facilely catalyze these two important processes at low temperatures. In addition, the subsequent dehydrogenation of CH3O to CH2O is also found to proceed with a low barrier.