Development and Application of an Analysis Methodology for Interpreting Ambiguous Historical Pressure Data in the WIPP Gas-Generation Experiments

摘要

The potential for generation of gases in transuranic (TRU) waste by microbial activity, chemical interactions, corrosion, and radiolysis was addressed in the Argonne National Laboratory-West (ANL-West) Gas-Generation Experiments (GGE). Data was collected over several years by simulating the conditions in the Waste Isolation Pilot Plant (WIPP) after the eventual intrusion of brine into the repository. Fourteen test containers with various actual TRU waste immersed in representative brine were inoculated with WIPP-relevant microbes, pressurized with inert gases, and kept in an inert-atmosphere environment for several years to provide estimates of the gas-generation rates that will be used in computer models for future WIPP Performance Assessments. Modest temperature variations occurred during the long-term ANL-West experiments. Although the experiment temperatures always remained well within the experiment specifications, the small temperature variation was observed to affect the test container pressure far more than had been anticipated. In fact, the pressure variations were so large, and seemingly erratic, that it was impossible to discern whether the data was even valid and whether the long-term pressure trend was increasing, decreasing, or constant. The result was that no useful estimates of gas-generation rates could be deduced from the pressure data. Several initial attempts were made to quantify the pressure fluctuations by relating these to the measured temperature variation, but none was successful. The work reported here carefully analyzed the pressure measurements to determine if these were valid or erroneous data. It was found that a thorough consideration of the physical phenomena that were occurring can, in conjunction with suitable gas laws, account quite accurately for the pressure changes that were observed. Failure of the earlier attempts to validate the data was traced to the omission of several phenomena, the most important being the variation in the headspace volume caused by thermal expansion and contraction within the brine and waste. A further effort was directed at recovering useful results from the voluminous archived pressure data. An analytic methodology to do this was developed. This methodology was applied to each archived pressure measurement to nullify temperature and other effects to yield an adjusted pressure, from which gas-generation rates could be calculated. A review of the adjusted-pressure data indicated that generated-gas concentrations among these containers after approximately 3.25 years of test operation ranged from zero to over 17,000 ppm by volume. Four test containers experienced significant gas generation. All test containers that showed evidence of significant gas generation contained carbon-steel in the waste, indicating that corrosion was the predominant source of gas generation.