Plasma-enhanced catalysis for the upgrading of methane: a review of modelling and simulation methods
Plasma-enhanced catalysis for the upgrading of methane: a review of modelling and simulation methods
复制标题
DOI：
10.1039/d0re00024h
复制
发表时间：
2020-05
影响因子：
3.9
通讯作者：
P. Maitre;M. Bieniek;P. Kechagiopoulos
中科院分区：
文献类型：
--
作者：
P. Maitre;M. Bieniek;P. Kechagiopoulos
由于分子的高增值潜力以及甲烷在化石和可持续来源中的广泛可用性，通过等离子体催化将甲烷直接升级为高级碳氢化合物受到了特别关注。大量的实验工作集中在等离子体催化系统性能的研究上。然而，人们认识到，大多数等离子体与表面的相互作用仍然没有被完全理解，实验、理论和建模研究的结合对于获得基本的机制洞察，从而导致该领域的进步至关重要。当前的综述介绍了等离子体相动力学、等离子体流体建模和等离子体-催化剂相互作用的最先进的模拟方法，因为这些方法已应用于甲烷等离子体。重点放在建模过程中应考虑的物种，从稳定分子和自由基到离子和激发态。讨论了这些物种参与的等离子体化学过程的类型，并提出了计算其速率的方法。涵盖了从空间均匀且计算成本低廉的零维代码到更复杂的流体建模方法的建模方法。最后总结了有关等离子体相关物质与金属表面相互作用的第一原理计算。
The direct upgrading of methane to higher hydrocarbons via plasma-catalysis has received particular attention due to the high valorisation potential of the molecule and methane's wide availability in both fossil and sustainable sources. Extensive experimental work has focused on the study of the performance of plasma-catalytic systems. However, it is recognised that most plasma-surface interactions are still not fully understood, and that the combination of experimental, theoretical and modelling studies is essential to gain a fundamental mechanistic insight, leading to advancements in the field. The current review presents the state-of-the-art of simulation methodologies for plasma-phase kinetics, plasma fluid modelling and plasma-catalyst interactions as these have been applied for methane plasmas. Focus is placed on the species that should be considered during modelling, ranging from stable molecules and radicals to ions and excited states. The types of plasma-chemical processes these species participate in are discussed and the methods for calculating their rates are presented. Modelling approaches spanning from spatially homogeneous and computationally inexpensive zero-dimensional codes to more complex fluid modelling approaches are covered. First principles calculations concerning plasma relevant species interactions with metal surfaces are finally summarised.