A reactive molecular dynamics simulation study of methane oxidation assisted by platinum/graphene-based catalysts
A reactive molecular dynamics simulation study of methane oxidation assisted by platinum/graphene-based catalysts
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DOI：
10.1016/j.proci.2018.05.109
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发表时间：
2019-01-01
影响因子：
3.4
通讯作者：
Luo, Kai H.
中科院分区：
文献类型：
--
作者：
Feng, Muye;Jiang, Xi Zhuo;Luo, Kai H.
铂修饰的功能化石墨烯片（Pt@FGS）是一种很有前途的催化燃料燃烧纳米添加剂。在这项研究中，四个案件涉及纯甲烷氧化和甲烷氧化在各种Pt/石墨烯基纳米粒子催化剂的存在下进行了研究，使用反应力场分子动力学（ReaxFF MD）模拟，以揭示甲烷氧化的催化机制和动力学。结果表明，Pt@FGS是本研究中涉及的所有纳米颗粒候选者中最有效的催化剂。与纯甲烷氧化相比，Pt@FGS反应中Pt和FGS的组合通过显著降低约73%的活化能来提高催化活性。此外，甲烷的催化氧化是通过C-H键的断裂和羟基的产生而引发的。所观察到的H转移过程表明，Pt@FGS的增强脱氢和原子间交换激活催化循环并主导催化过程。此外，FGS可以主要在片材的边缘处进一步氧化以增加功能性。总之，这项研究揭示了在Pt@FGS存在下增强燃料燃烧的催化机制。(C)2018作者（S）爱思唯尔公司出版代表燃烧研究所
Platinum-decorated functionalized graphene sheet (Pt@FGS) is a promising nanoparticle additive for catalytic fuel combustion. In this study, four cases involving pure methane oxidation and methane oxidation in the presence of various Pt/graphene-based nanoparticle catalysts are investigated using the reactive force field molecular dynamics (ReaxFF MD) simulations to reveal catalytic mechanisms and kinetics of methane oxidation. The results demonstrate that Pt@FGS is the most effective catalyst among all the nanoparticle candidates involved in this research. Compared with pure methane oxidation, the combination of Pt and FGS in the Pt@FGS reaction improves the catalytic activity by dramatically lowering the activation energy by approximately 73%. Additionally, the catalytic methane oxidation is initiated by the cleavage of C-H bond and the production of hydroxyl. The observed H transfer process suggests that enhanced dehydrogenation of Pt@FGS and interatomic exchanges activate the catalytic cycle and dominate the catalytic process. Moreover, FGS can be further oxidized mostly at the edge of the sheet to increase the functionality. In summary, this research sheds light on the catalytic mechanisms for enhanced fuel combustion in the presence of Pt@FGS. (C) 2018 The Author(s). Published by Elsevier Inc. on behalf of The Combustion Institute.