Much of the work described in this report was done under the sponsorship of the U.S. Nuclear Regulatory Commission to enhance the ability to predict releases and consequences of LWR severe accidents. Thus, considerable credit is due to the NRC Office of Nuclear Regulatory Research, and to technical monitors Lisa Chan, Tom Walker, and Richard Lee. The final publication, however, has been supported by the ORNL Research Reactors Division in order to adequately document models that have been used in the safety analysis of the High Flux Isotope Reactor. The authors are especially grateful to Lamar Lepard, David Cook, and George Flanagan of Research Reactors Division for this sponsorship of this work. Finally, thanes go to Lindy Norris for her diligent efforts in typing and revising the manuscript. vii _CT Models are developed for many phenomena of interest concerning iodine behavior in reactor containments during severe accidents. Processes include speciation in both gas and liquid phases, reactions with surfaces, airborne aerosols, and other materials, and gas-liquid interface behavior. Although some models are largely empirical formulations, every effort has been made to construct mechanistic and rigorous descriptions of relevant chemical processes. Ali are based on actual experimental data generated at the Oak Ridge National Laboratory (ORNL) or elsewhere, and, hence, considerable data evaluation and parameter estimation are contained in this study. No application or encoding is attempted, but each model is stated in terms of rate processes, with the intention of allowing mechanistic simulation. Taken together, this collection of models represents a best estimate iodine behavior and transport in reactor accidents.