Nuclear magnetic resonance measurement of ammonia diffusion in dense solid-liquid slurries. Revision 1

Abstract

The flammability and toxicity of ammonia released from the nuclear waste tanks at Hanford have been the subject of several recent studies. These releases may occur episodically, such as the buoyant plume releases occurring in various double-shell tanks (DSTs); gradually through the surface of the waste; or from the partially saturated saltcakes in the single-shell tanks during salt-well pumping. The diffusion of ammonium ions in aqueous solutions was measured by nuclear magnetic resonance (NMR) using the pulsed field gradient (PFG) method. The ammonium ions were obtained from aqueous solutions of ammonium chloride, ammonium sulfate, ammonium bicarbonate, and ammonium hydroxide. The translational diffusion of the ammonium ions was determined by measuring the diffusion of nitrogen nuclei in solution. Results showed that the ammonium diffusion coefficient can be measured in aqueous solutions with concentrations as low as 20 {times} 10{sup {minus}3} {und M}. Typical values measured for the diffusion coefficient of the ammonium ion are 2 {times} 10{sup {minus}5} cm{sup 2}/s ({+-}10%), similar to the values found for pure water. Due to the effect of the solution pH upon the NMR relaxation parameters for {sup 14}N, measurements are constrained to pH values below 8.5. However, {sup 15}N labeled ammonia is less sensitive to the solution pH, extending the measurement range to pH of 9.5. The results show that the solution viscosity has a measurable impact on the diffusion coefficient. The diffusion coefficient is almost inversely proportional to the relative viscosity of the solution, irrespective of how the viscosity is increased. Further, a randomly-packed porous bed of 200 {micro}m PMMA resulted in a reduction of {approximately} 30% in the diffusion coefficient as a result of hindered diffusion.