Coupling CFD with detailed microkinetic modeling in heterogeneous catalysis
Coupling CFD with detailed microkinetic modeling in heterogeneous catalysis
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DOI：
10.1016/j.ces.2013.03.048
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发表时间：
2013-06-07
影响因子：
4.7
通讯作者：
Cuoci, Alberto
中科院分区：
文献类型：
--
作者：
Maestri, Matteo;Cuoci, Alberto
对催化过程的原子尺度理解对于催化技术的合理发展至关重要。它要求确定主要的反应机制，这是系统固有的多尺度性质。在这方面，对催化剂反应性与反应器中周围流场的相互作用有一个基本的了解是至关重要的。在这里，我们提出了一种新的求解器（catalyticFOAM），它可以根据表面反应性的详细微动力学描述，求解表面反应流的复杂和一般几何形状的Navier-Stokes方程。该催化剂利用了基于输运项和反应项分离的操作符分裂技术。所提出的数值算法使具有复杂和详细的动力学机制的多维系统的模拟成为可能，克服了全耦合算法所需要的不可行的计算工作量。以结构堆和随机堆为例，介绍了H-2在Rh上的富燃料燃烧。提出的方法代表了基于第一性原理的催化过程多尺度分析的重要一步，并为合理理解和发展新的反应/反应器概念铺平了道路。(c) 2013 Elsevier Ltd.版权所有。
The atomic-scale understanding of a catalytic process is crucial for the rational development of catalytic technologies. It requires the identification of the dominant reaction mechanism, that is an intrinsic multiscale property of the system. In this respect, it is of utmost importance to obtain a fundamental understanding about the interactions of the catalyst reactivity with the surrounding flow field in the reactor. Here, we propose a new solver (catalyticFOAM), that allows for the solution of Navier-Stokes equations for complex and general geometries for reacting flows at surfaces, based on a detailed microkinetic description of the surface reactivity. The catalyticFOAM solver exploits the operator-splitting technique, based on the separation of transport and reaction terms. The proposed numerical algorithm makes possible the simulation of multidimensional systems with complex and detailed kinetic mechanisms, overcoming the unfeasible computational effort that would be required by fully-coupled algorithms. Examples concerning the H-2 fuel rich combustion on Rh are presented as showcases in structured and randomly packed reactors. The proposed approach represents an essential step for the first-principles based multiscale analysis of catalytic processes and paves the way toward the rational understanding and development of new reaction/reactor concepts. (c) 2013 Elsevier Ltd. All rights reserved.