Gas retention and release from Hanford Site sludge waste tanks - 15491

Radioactive wastes from nuclear fuel processing are stored in large underground storage tanks at the Hanford Site. Solid wastes can be divided into salt-cake (mostly precipitated soluble sodium nitrate and nitrite salts with some interstitial liquid consisting of concentrated salt solutions) and sludge (mostly low solubility aluminum and iron compounds with relatively dilute interstitial liquid). Waste generates hydrogen through the radiolysis of water and organic compounds, radio-thermolytic decomposition of organic compounds, and corrosion of a tank's carbon steel walls. Nonflammable gases, such as nitrous oxide and nitrogen, are also produced. Additional flammable gases (e.g., ammonia and methane) are generated by chemical reactions between various degradation products of organic chemicals present in the tanks. Six double-shell tanks (DSTs) containing salt-cake wastes began showing signs of gas accumulation and buoyant instability in the form of periodic waste level drops in the 1980's. Studies in the 1990's indicated that gas would accumulate in the settled solids layer until its bulk density was lower than the supernatant liquid. The resultant gas release caused by this instability was termed a Buoyant Displacement Gas Release Event (BDGRE). Criteria were developed to prevent forming additional waste tanks that exhibited BDGREs. Significant gas accumulation and BDGREs were never observed in tanks containing predominantly sludge wastes. Literature reviews, data from Hanford Site waste tanks, and experiments with waste simulants have led to new conclusions on gas retention and release in sludge waste. The data show similar overall behavior where initially the settled solids volume increases as gas bubbles form. Gas fraction in the settled solids increases to a peak concentration after which additional generated gas escapes through connected cracks and there is a balance between gas generation and gas release with little change in gas fraction. Experiments showed that this behavior does not change as sludge waste depth increases. Sufficient data now exist to differentiate between gas retention and release behavior in Hanford Site sludge waste tanks and salt-cake waste tanks. The salt-cake criteria do not need to be applied to sludge waste tanks that exhibit certain gas retention and release behavior. Criteria for waste characteristics and process behavior have been defined that identify specific wastes and tanks that, based on previous operating experience, will have low gas retention and will not exhibit large, spontaneous releases. The first criterion defines what waste is considered sludge and what waste is considered salt-cake. If the mass ratio of soluble to insoluble constituents is below 2.5, then the waste is sludge. The second criterion is a density difference criterion that prevents tanks being operated in a region where sludge buoyancy might occur. For large gas releases to occur, the settled solids must accumulate sufficient gas to become less dense than the overlying supernatant (i.e., the settled solids would become buoyant). Based on previous operating experience, the ratio of liquid density to degassed settled solids bulk density (ρl/ρB) should be maintained at ≤ 0.84. This ensures that retained gas content in the sludge would need to exceed 16% by volume for the settled solids to become buoyant in the overlying supernatant. Tank waste that satisfies the mass ratio criterion, the liquid to bulk solids density criterion, and has process data supporting typical Hanford waste sludge behavior does not pose a significant risk for a large spontaneous gas release event. (authors)