A Theory of Chemical Reaction Networks: The Dynamics of Reactors with Complex Chemistry

具有复杂化学反应的反应器，特别是那些涉及多相催化的反应器，在商业上是重要的。这样复杂的系统可能会以意想不到的方式运行，导致多种稳定状态、不稳定、失控反应、爆炸等。本研究的目标是创造理论，为实践工程师和化学家提供易于应用的分析工具，用于：(1)具有复杂但熟知的化学反应的反应器的操作（该理论将提供应引起关注的稳定性问题的指示）和(2)对化学知之甚少的反应器的研究（该理论将为提出的竞争性机制之间的敏感区分提供手段，以解释实验室观察结果）。​对许多系统的多稳态、周期组成振荡和持续非周期振荡进行了研究。PI的主要贡献是对等温反应器（通常用于工业）的分析，其中不稳定行为的来源是在化学本身。等温反应器由耦合的非线性微分方程组控制，其中变量为物质浓度，参数为速率常数、停留时间和进料浓度。这些微分方程有一个特殊的结构，PI利用它来预测某些系统的预期行为类型。在这项更新工作中，他计划将理论扩展到更广泛的问题类别。与此同时，他将与一名实验室设备齐全的实验员合作，开始对乙烯在铂上加氢的理论进行实验测试。此外，PI正计划开发商业软件，用于IBM个人电脑，以实现他的理论。

Reactors with complex chemistry, especially those involving heterogeneous catalysis, are important commercially. 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). Multiple steady states, periodic composition oscillations and sustained aperiodic oscillations have been studied for many systems. The PI's major contributions have been in the analysis of isothermal reactors (commonly used in industry) where the source of the unstable behavior is to be found in the chemistry itself. Isothermal reactors are governed by systems of coupled nonlinear differential equations where the variables are the species concentrations and the parameters are the rate constants, residence times and feed concentrations. These differential equations have a special structure which the PI has exploited to predict the type of behavior to be expected for some systems. In this renewal work he plans to expand the theory to wider classes of problems. At the same time he will begin experimental testing of the theory on the hydrogenation of ethylene on platinum in cooperation with an experimentalist whose laboratory is fully equipped for this effort. Also, the PI is planning to develop commercial software to be used on IBM PC's to implement his theory.