Department of Chemistry, Chung Yuan Christian University, Taoyuan City, Chungli District, 32023, Taiwan.
Phys Chem Chem Phys. 2018 Nov 7;20(41):26414-26421. doi: 10.1039/c8cp04745f. Epub 2018 Oct 11.
The catalytic reaction of carbon monoxide oxidation on boron-doped and boron-nitrogen co-doped penta-graphene materials has been systematically studied by utilizing spin-polarized density functional theory (DFT) calculations. Various pathways including the Eley-Rideal (ER), Langmuir-Hinshelwood (LH), and tri-molecular Eley-Rideal (TER) mechanisms were considered in which the TER mechanism is a newly proposed reaction mechanism for CO oxidation. According to the calculation results, the ER, LH and TER mechanisms of CO oxidation can occur and compete with each other because of the related small overall reaction energy barriers (0.11-0.35 eV for the ER mechanism, 0.16-0.17 eV for the LH mechanism, and no activation energy for the TER mechanism). Our study helps to understand the various pathways for the CO oxidation process and suggests that both B-doped and BN co-doped penta-graphene sheets may serve as effective metal-free catalysts for low-temperature CO oxidation.
利用自旋极化密度泛函理论（DFT）计算，系统地研究了掺硼和硼氮共掺五重石墨烯材料上一氧化碳氧化的催化反应。考虑了各种途径，包括 Eley-Rideal（ER）、Langmuir-Hinshelwood（LH）和三分子 Eley-Rideal（TER）机制，其中 TER 机制是 CO 氧化的新提出的反应机制。根据计算结果，由于相关的总反应能垒较小（ER 机制为 0.11-0.35 eV，LH 机制为 0.16-0.17 eV，而 TER 机制无活化能），CO 氧化的 ER、LH 和 TER 机制可以发生并相互竞争。我们的研究有助于理解 CO 氧化过程的各种途径，并表明掺硼和 BN 共掺五重石墨烯片可能作为低温 CO 氧化的有效无金属催化剂。
