| The multiple-scale singular perturbational analysis of heterogeneous catalytic reaction systems is presented in this Dissertation. Emphasis is on modeling their wide range of complex behavior, including chaos, for which there is abundant experimental evidence in the literature, and in demonstrating the practical utility of the analysis in understanding these important reaction systems.;The applicability of the analysis is first justified from experimental data in Chapter II, which are shown to reveal underlying processes with widely separated time constants, some of whose ratios are then used to introduce the "small" parameter(s) required in a singular perturbation form of the ordinary differential equations derived to describe system dynamics. Various algebraic equations, definable from the degenerate subsystems of said perturbation form, are in turn used to define behavior manifolds whose topological and stability properties in general approximately determine system behavior.;The powerful utility of the analytical approach is amply demonstrated in this work--in aiding model discriminations (Chapter II), in the global location of interesting regions in model parameter space of complex dynamic behavior even before extensive numerical integrations and more rigorous bifurcational analyses are done (Chapter III), and in the first reported use, in Chapter IV, of experimental bifurcation-to-oscillation data in the estimation of the parameters of a proposed nonisothermal model incorporating a slow surface redox scheme, whose derivation and preliminary analysis are first presented in Chapter III. A novel multistage parameter estimation procedure introduced in Chapter IV also employs temporal oscillatory data which, together with bifurcation data, are well known to be significantly more parametrically sensitive than steady-state-type data.;In the course of the work, a novel algorithm named PEFLOQ, suitable for general use, for the calculation, stability analysis and continuation of stable and unstable periodic solutions, is introduced.;The results of this study should have significant effect on the direction for future modeling work on heterogeneous catalytic reaction systems, ultimately enhancing their proper design, control and optimization. Several of the major implications are spelt out in the text of the Dissertation. |
