Status and integration of the gas generation studies performed for the Hydrogen Safety Program

Abstract

Waste in Tank 241-SY-101 on the Hanford Site generates and periodically releases hydrogen, nitrous oxide, and nitrogen gases. Studies have been conducted at several laboratories to determine the chemical mechanisms for the gas generation and release. Results from these studies are presented and integrated in an attempt to describe current understanding of the physical properties of the waste and the mechanisms of gas generation and retention. Existing tank data are consistent with the interpretation that gases are uniformly generated in the tank, released continuously from the convecting layer, and stored in the nonconvecting layer. Tank temperature measurements suggest that the waste consists of gobs'' of material that reach neutral buoyancy at different times. The activation energy of the rate limiting step of the gas generating process was calculated to be about 7 kJ/mol but measured in the laboratory at 80 to 100 kJ/mol. Based on observed temperature changes in the tank the activation energy is probably not higher than about 20 kJ/mol. Several simulated waste compositions have been devised for use in laboratory studies in the place of actual waste from Tank 241-SY-101. Data from these studies can be used to predict how the actual waste might behave when heatedmore » or diluted. Density evaluations do not confirm that heating waste at the bottom of the tank would induce circulation within the waste; however, heating may release gas bubbles by dissolving the solids to which the bubbles adhere. Gas generation studies on simulated wastes indicated that nitrous oxide and hydrogen yields are not particularly coupled. Solubility studies of nitrous oxide, the most soluble of the principal gaseous products, indicate it is unlikely that dissolved gases contribute substantially to the quantity of gas released during periodic events.« less