Abstract
Slurries and sludges across the United States Department of Energy (DOE) complex rank among the most rheologically interesting. Their composition is heterogeneous, spanning a very broad range of particle sizes, densities, and interparticle forces. All exhibit shear thinning, some have yield stresses, and many are thixotropic. Despite the variety, these complex fluids are often represented using the historic Bingham fluid model, which fits higher shear rate data to a simple straight line. The intercept provides a yield stress, which has been a key design parameter in construction of large-scale waste processing facilities. However, many radioactive wastes are simply not Bingham fluids, and this representation extrapolates poorly across low to intermediate shear rates that are characteristic of typical processing conditions. Indeed, processing shear rates as high as 200 1/s, which has been a typical minimum shear rate used in fitting the Bingham fluid model, are seldom encountered in nuclear waste processing. Therefore, more realistic rheological models are necessary to accurately predict waste processing performance.
Pacific Northwest National Laboratory (PNNL) recently re-evaluated the rheology of reconstituted Hanford REDOX (reduction-oxidation) process sludge waste against a wide variety of rheological models including the Bingham, Cross, Cross with yield stress, Carreau, biviscous, Herschel-Bulkley (which includes a power law dependence), Casson, and Gay models. They found that all of the models provided a closer fit than the Bingham model and that the biviscous model and Cross with yield stress model were convincing. However, reconstituted Hanford REDOX sludge waste is but one type of DOE waste and a direct contrast, and comparison of these three models against undiluted, unmixed tank waste (actual not simulant) has not been performed previously. Therefore, the purpose of this paper is to evaluate the rheology of actual tank waste with these more accurate rheological models.
In this paper, we evaluate select rheological data for slurry samples from Hanford’s AZ-101, AZ-102, and SY-101 waste tanks. In each of these cases, we find that Cross’ model with yield stress and the biviscous model significantly outperform the Bingham fluid model. Furthermore, the AZ-101 data also shows that the shear stress peak at startup significantly exceeds the Bingham yield stress, which is commonly observed in the initial moments of rheological measurements on simulants. Remarkably, Cross’ model may empirically accommodate an initial spike in shear stress at modest shear rates. These are important observations because computational and analytical fluid dynamics simulations rely on rheological constitutive models for accurately and conservatively predicting waste processing performance. These findings suggest the need for better rheological modeling of and validation against radioactive waste.
Towards the Development of a Strategy to Characterize and Model the Rheological Behavior of Filled, Uncured Rubber Compounds