Department of Chemical Engineering, Texas A&M University, College Station, Texas 77843, USA.
J Phys Chem A. 2012 Feb 9;116(5):1409-16. doi: 10.1021/jp208179e. Epub 2012 Feb 1.
A computational study using density functional theory is carried out to investigate the reaction mechanism of ethanol steam reforming on Co(0001) surfaces. The adsorption properties of the reactant, possible intermediates, and products are carefully examined. The reaction pathway and related transition states are also analyzed. According to our calculations, the reforming mechanism primarily consisting of dehydrogenation steps of ethanol, ethoxy, methanol, methoxy, and formic acid, is feasible on Co(0001) surfaces. It is also found that the reaction of formaldehyde yielding formic acid and hydrogen may not be an elementary reaction. The dehydrogenation of ethoxy possesses the highest barrier and is accordingly identified as the rate-determining step.
采用密度泛函理论进行了计算研究，以考察乙醇水蒸气重整在 Co(0001)表面上的反应机理。仔细研究了反应物、可能的中间体和产物的吸附特性。还分析了反应途径和相关的过渡态。根据我们的计算，在 Co(0001)表面上，重整机制主要由乙醇、乙氧基、甲醇、甲氧基和甲酸的脱氢步骤组成，是可行的。还发现甲醛生成甲酸和氢气的反应可能不是基元反应。乙氧基的脱氢具有最高的势垒，因此被确定为速率决定步骤。
