催化重整单事件反应动力学模型(Ⅰ)反应网络的建立及单事件数的计算

Single-Event Kinetic Model of Catalytic Reforming(Ⅰ) Reaction Network Construction and Single-Event Number Calculation

以经典的双功能催化重整反应机理为基础,对催化重整单事件反应动力学模型进行了研究。采用布尔邻接矩阵及其主对角元素描述反应物种的分子结构,通过布尔邻接矩阵的操作实现基本反应步骤的数字化,进而构建催化重整反应网络。引入单事件概念将基本反应步骤的反应速率常数分解为单事件数和单事件速率常数,通过将分子中相同的原子标记区分,计算了反应物和活化络合物全局对称数,从而得到单事件数。开发了基本反应步骤单事件数的计算方法,并实现了单事件数的自动计算,最后通过实例对计算方法进行了解释。该结果可为催化重整单事件反应动力学模型的建立提供理论基础。

The single-event micro-kinetic model of catalytic reforming was studied based on the classical bi-functional catalytic reforming mechanism.Boolean relation matrix and its diagonal elements were employed to describe the reaction species,and the elementary reaction steps were represented by the Boolean relation matrix operation.The reaction network of catalytic reforming was then constructed.The rate coefficient of an elementary step was separated into single-event rate coefficients and single-event numbers based on the single event concept.The global symmetry numbers of reactants and activated complexes were calculated by labeling the same atoms in the molecules.The single-event number is equaled to the ratio of global symmetry numbers of reactant and activated complex.The algorithm for single-event number calculation of elementary steps was developed,and automatic calculation of single-event number was achieved.At the end,examples were given to explain how to compute the single-event numbers.The results provide the foundation for establishing the single-event micro-kinetic model of catalytic reforming.