Uranium Pyrophoricity Phenomena and Prediction (FAI/00-39)

摘要

The purpose of this report is to provide a topical reference on the phenomena and prediction of uranium pyrophoricity for the Hanford Spent Nuclear Fuel (SNF) Project with specific applications to SNF Project processes and situations. Spent metallic uranium nuclear fuel is currently stored underwater at the K basins in the Hanford 100 area, and planned processing steps include: (1) At the basins, cleaning and placing fuel elements and scrap into stainless steel multi-canister overpacks (MCOs) holding about 6 MT of fuel apiece; (2) At nearby cold vacuum drying (CVD) stations, draining, vacuum drying, and mechanically sealing the MCOs; (3) Shipping the MCOs to the Canister Storage Building (CSB) on the 200 Area plateau; and (4) Welding shut and placing the MCOs for interim (40 year) dry storage in closed CSB storage tubes cooled by natural air circulation through the surrounding vault. Damaged fuel elements have exposed and corroded fuel surfaces, which can exothermically react with water vapor and oxygen during normal process steps and in off-normal situations, A key process safety concern is the rate of reaction of damaged fuel and the potential for self-sustaining or runaway reactions, also known as uranium fires or fuel ignition. Uranium metal and one of its corrosion products, uranium hydride, are potentially pyrophoric materials. Dangers of pyrophoricity of uranium and its hydride have long been known in the U.S. Department of Energy (Atomic Energy Commission/DOE) complex and will be discussed more below; it is sufficient here to note that there are numerous documented instances of uranium fires during normal operations. The motivation for this work is to place the safety of the present process in proper perspective given past operational experience. Steps in development of such a perspective are: (1) Description of underlying physical causes for runaway reactions, (2) Modeling physical processes to explain runaway reactions, (3) Validation of the method against experimental data, (4) Application of the method to plausibly explain operational experience, and (5) Application of the method to present process steps to demonstrate process safety and margin. Essentially, the logic above is used to demonstrate that runaway reactions cannot occur during normal SNF Project process steps, and to illustrate the depth of the technical basis for such a conclusion. Some off-normal conditions are identified here that could potentially lead to runaway reactions. However, this document is not intended to provide an exhaustive analysis of such cases. In summary, this report provides a ''toolkit'' of models and approaches for analysis of pyrophoricity safety issues at Hanford, and the technical basis for the recommended approaches. A summary of recommended methods appears in Section 9.0.