Gas Concentration Measurements in Underground Waste Storage Tanks

Abstract

Currently over 100 underground tanks at the Hanford facility in eastern Washington state are being used to store high-level radioactive waste. With plans for a long-term nuclear-waste repository in Nevada in place (though not yet approved), one promising use for these underground storage tanks is as a temporary waystation for waste destined for the Nevada repository. However, without a reasonable understanding of the chemical reactions going on within the tanks, transporting waste in and out of the tanks has been deemed to be unsafe.

One hazard associated with such storage mechanisms is explosion of flammable gases produced within the tank. Within many of the storage tanks is a sludge layer. This layer, which is a mixture of liquid and solids, contains most of the radioactive material. Radioactive decay and its associated heat can produce several flammable materials within this layer. Two components of particular concern are hydrogen (H2) and nitrous oxide (N2O), since they are highly volatile in the gaseous phase. Though the tanks have either forced or natural convection systems to vent these gases, the possibility of an explosion still exists.

Measurements of these gases are taken in several ways. Continuous measurements are taken in the headspace, which is the layer between the tank ceiling and the liquid (supernatant) or sludge layer below. In tanks where a supernatant layer sits atop the sludge layer, there are often rollovers or gas release events (GREs), where a large chunk of sludge, after attaining a certain void fraction, becomes buoyant, rising through the supernatant and releasing its associated gas composition to the headspace. Such changes trigger a sensor, and thus measurements are also taken at that time.

Lastly, a retained gas sample (RGS) can be taken from either the supernatant or sludge layer. Such a core sample is quite expensive, but can yield crucial data about the way gases are being produced in the sludge and convected through the supernatant.

Unfortunately, the measurements from these three populations do not seem to match. In particular, the ratio r = [N2O]/[H2] varies from population to population. r also varies from tank to tank, but this can more readily be explained in terms of the waste composition of each tank. Since H2 is more volatile than N2O (and since there are more sources of oxygen in the headspace), lower values of r correspond to more hazardous situations.

This variance in r is troubling, since we need to be able to explain why certain values of r are lower (and hence more dangerous) in certain areas of the tank. In this report we examine the data from three tanks. We first verify that the differences in r among populations is significant. We then postulate several mechanisms which could explain such a difference.