Chemical Reaction Network Theory: The Dynamics of Reactors with Complex Chemistry

通常在真实的化学反应中，大量不同的物种通过复杂的化学反应网络相互作用。这种复杂的系统可能以意想不到的方式运行，导致多个稳态、不稳定、失控反应、爆炸、这项研究的目标是创造理论，为执业工程师和化学家提供随时可用的分析工具，以用于：(1)具有复杂但很好理解的化学的反应堆的运行(该理论将提供应引起关注的稳定性问题的指示)，以及(2)对化学性质知之甚少的反应堆的研究(该理论将为解释实验室观察所提出的相互竞争的机制之间的敏感区分提供手段)。PI的化学反应理论植根于这样一个想法，即无论化学反应工程的领域看起来多么广阔，呈现在研究中的微分方程组都有一个非常特殊的结构。至少当动力学是质量作用时，每个体系都是从基本的化学反应网络中以非常精确的方式确定的(直到速率常量)，因此询问关于反应网络结构和相应微分方程的定性性质之间的关系是有意义的。这项拨款下的工作将包括三个新的项目：(1)PI早期的面向缺陷的理论与基于他的物种-络合物-连接图(SCL图)的新发展的统一，并应用于更复杂的系统，如电化学反应；(2)将现有的和新发展的理论应用于多相催化，特别强调操作催化途径是如何通过一个特征的“机械特征”在多个稳态数据中揭示自身的；以及(3)开发面向用户的个人计算机软件，该软件不需要基本的复杂数学分析知识。

Often in real chemical reactors, a large number of distinct species interact through an intricate network of chemical reactions. Such complex systems can behave in unexpected ways, causing multiple steady states, instabilities, runaway reactions, explosions, etc. The goal of this research is the creation of theory that provides practicing engineers and chemists with readily applicable analytical tools to be used for: (1) the operation of reactors with complex but well understood chemistry (the theory would provide an indication of the stability problems that should be a source of concern), and (2) the study of reactors with poorly understood chemistry (the theory would provide means for the sensitive discrimination between rival mechanisms put forward to account for laboratory observations). The PI's chemical reaction theory is rooted in the idea that, however vast the territory of chemical reaction engineering might seem, the systems of differential equations that present themselves for study have a very special structure. At least when the kinetics is mass action, each system is determined (up to rate constant values) in a very precise way from the underlying network of chemical reactions, and so it becomes meaningful to ask questions about the relationship between reaction network structure and qualitative properties of the corresponding differential equations. Work under this grant will consist of three new projects: (1) unification of the PI's earlier deficiency-oriented theories with newer developments based on his Species-Complex-Linkage graph (SCL Graph) and application to more complex systems such as electrochemical reactions; (2) application of existing and newly developed theory to heterogeneous catalysis with special emphasis on the way in which the operative catalytic pathway reveals itself in multiple steady state data by way of a characteristic "mechanistic signature"; and (3) development of user-oriented personal computer software which would not require knowledge of the underlying complex mathematical analysis.