Reduction of microkinetic reaction models for reactor optimization exemplified for hydrogen production from methane
Reduction of microkinetic reaction models for reactor optimization exemplified for hydrogen production from methane
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DOI：
10.1016/j.cej.2015.06.119
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发表时间：
2015-12-01
影响因子：
15.1
通讯作者：
Sundmacher, Kai
中科院分区：
文献类型：
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作者：
Karst, Florian;Maestri, Matteo;Sundmacher, Kai
可持续和高效的流程需要优化的设计和操作条件。然而，确定最佳工艺路线是一项具有挑战性的任务。要么模型和基础化学反应速率方程无法描述各种反应条件下的过程，从而限制了优化空间，要么模型过于复杂且在数值上具有挑战性，无法用于动态优化。为了解决这个问题，在这篇文章中，提出了一种化学反应网络的简化技术。它侧重于反应动力学模型相对于删除选定反应步骤的敏感性，并评估它们对于预测整个系统行为的重要性。该方法通过 C-1 微动力学模型进行了演示，该模型描述了以 Rh/Al2O3 作为催化剂的甲烷转化为合成气的过程。原始和简化的微动力学模型显示出极好的定性和定量一致性。随后，简化的动力学模型用于优化甲烷重整器，以生产富氢气体混合物作为聚合物电解质膜（PEM）燃料电池应用的原料。 (C) 2015 年作者。由 Elsevier B.V. 出版
Sustainable and efficient processes require optimal design and operating conditions. The determination of optimal process routes, however, is a challenging task. Either the models and underlying chemical reaction rate equations are not able to describe the process in a wide ranges of reaction conditions and thus limit the optimization space, or the models are too complex and numerically challenging to be used in dynamic optimization. To address this problem, in this contribution, a reduction technique for chemical reaction networks is proposed. It focuses on the sensitivity of the reaction kinetic model with respect to the removal of selected reaction steps and evaluates their significance for the prediction of the overall system behavior. The method is demonstrated for a C-1 microkinetic model describing methane conversion to syngas on Rh/Al2O3 as catalyst. The original and the reduced microkinetic model show excellent qualitative and quantitative agreement. Subsequently, the reduced kinetic model is used for the optimization of a methane reformer to produce a hydrogen rich gas mixture as feed for polymer electrolyte membrane (PEM) fuel cell applications. (C) 2015 The Authors. Published by Elsevier B.V.