Esrafili Mehdi D, Heydari Safa
Department of Chemistry, Faculty of Basic Sciences, University of Maragheh, P.O. Box 55136-553, Maragheh, Iran.
Department of Chemistry, Faculty of Basic Sciences, University of Maragheh, P.O. Box 55136-553, Maragheh, Iran.
J Mol Graph Model. 2019 Nov;92:320-328. doi: 10.1016/j.jmgm.2019.08.011. Epub 2019 Aug 17.
It is well-known that the catalytic oxidation of CO molecule into CO is one of the most important strategies for the removing of this toxic gas from the atmosphere. In the present study, we investigate the reaction pathways and energy barriers for the oxidation of CO by O molecule over the Si-doped CN nanosheet. According to our results, doping of CN nanosheet with a Si atom could greatly modify its surface reactivity and electronic structure. Due to the large positive charge on the Si, this atom acts as the most active site to adsorb CO and O molecules. Three possible reaction mechanisms are studied for the CO oxidation, namely the Eley-Rideal (ER), Langmuir-Hinshelwood (LH) and new Eley-Rideal (NER). Comparing the activation energies indicates that the CO oxidation reaction proceeds via the LH mechanism over the title surface. The energy barrier needed to remove the activated oxygen atom (O*) from the Si atom is only 0.22 eV, which is most likely to overcome at room temperature. The results of this study may be useful to fabricate noble-metal free catalysts to remove toxic CO molecules from the atmosphere.
众所周知，将一氧化碳（CO）分子催化氧化为二氧化碳（CO₂）是从大气中去除这种有毒气体的最重要策略之一。在本研究中，我们研究了在硅掺杂的碳氮（CN）纳米片上，氧（O）分子氧化CO的反应途径和能垒。根据我们的结果，用一个硅原子掺杂CN纳米片可以极大地改变其表面反应性和电子结构。由于硅上带有大量正电荷，该原子成为吸附CO和O分子的最活跃位点。我们研究了CO氧化的三种可能反应机制，即埃利-里德（Eley-Rideal，ER）机制、朗缪尔-欣谢尔伍德（Langmuir-Hinshelwood，LH）机制和新埃利-里德（new Eley-Rideal，NER）机制。比较活化能表明，在所述表面上，CO氧化反应通过LH机制进行。从硅原子上去除活化氧原子（O*）所需的能垒仅为0.22电子伏特，在室温下最有可能被克服。本研究结果可能有助于制备无贵金属催化剂，以从大气中去除有毒的CO分子。
