当前位置: X-MOL 学术Surf. Sci. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Ethylene oxidation on unpromoted silver catalysts: Reaction pathway and selectivity analysis using DFT calculations
Surface Science ( IF 1.9 ) Pub Date : 2021-02-22 , DOI: 10.1016/j.susc.2021.121834
Siyuan Wu , Bruce J. Tatarchuk , Andrew J. Adamczyk

Chemical conversions in catalytic partial oxidation processes of light hydrocarbons are responsible for the production of numerous industrial chemicals, plastics, and intermediates. These processes are relatively expensive to perform, and are typically operated at high thermodynamic inefficiency, so the development of novel, highly efficient catalysts would prove to be very cost effective. Herein, our study focused on surface catalytic mechanisms of the ethylene oxide (EO) formation process. Periodic plane-wave Density Functional Theory (DFT) methods were used to analyze related reaction mechanisms on the Ag(111) surface facet with low coverage. Energetic changes of related species and pathways were calculated. Key surface species are identified to suggest the factors for the observed selectivity during EO formation. Our results are consistent with previous kinetic modeling efforts in the literature which did not employ DFT analysis. Lastly, our study demonstrates how fundamental theoretical investigations and multi-scale modeling techniques are currently impacting the advancement of rational catalyst design and microkinetic modeling techniques in the light hydrocarbon processing industry.



中文翻译:

未助催化的银催化剂上的乙烯氧化:使用DFT计算的反应途径和选择性分析

轻烃的催化部分氧化过程中的化学转化负责生产多种工业化学品,塑料和中间体。这些方法执行起来相对昂贵,并且通常在高热力学效率低下操作,因此开发新型高效催化剂将证明非常具有成本效益。在本文中,我们的研究集中于环氧乙烷(EO)形成过程的表面催化机理。周期性平面波密度泛函理论(DFT)方法用于分析低覆盖率的Ag(111)表面的相关反应机理。计算了相关物种和途径的能量变化。确定了关键的表面物种,以暗示在EO形成过程中观察到的选择性的因素。我们的结果与之前未使用DFT分析的动力学建模方法一致。最后,我们的研究表明,基础理论研究和多尺度建模技术当前如何影响轻烃加工行业中合理的催化剂设计和微动力学建模技术的发展。

更新日期:2021-03-05
down
wechat
bug