Dynamic Particle Growth Testing - Phase I Studies

There is clearly a great need to understand the processes of crystallization and solid scale formation that led to the shutdown of 2H evaporator operation at the Savannah River Site (SRS) and could possibly cause similar problems in the future in other evaporators. Waste streams from SRS operations that enter the evaporators generally contain alkaline, sodium nitrate/nitrite-based solutions with various changing concentrations of silicates and aluminates. It has been determined. that the silicates and aluminates served as precursor reactants for forming unwanted minerals during solution evaporation, upon transport, or upon storage. Mineral forms of the Zeolite Linde A group--sodalites and cancrinite--along with gibbsite, have often been identified as contributing to deposit (scale) formation on surfaces of the 2H evaporator as well as to the formation of solid plugs in the gravity drain line and lift line. Meanwhile, solids (amorphous or crystalline minerals) are believed, without direct evidence, to form in the bulk solutions in the evaporator. In addition, the position of deposits in the 2H evaporator suggests that scale formation depends on the interplay of heat and mass transfer, hydrodynamics, and reaction mechanisms and kinetics. The origin of solid scale formation on walls could be due to heterogeneous nucleation and/or to homogeneous nucleation followed by cluster/particle deposition. Preliminary laboratory tests at the Savannah River Technology Center (SRTC) with standing metal coupons seem to support the latter mechanism for initial deposition; that is, the solid particles form in the bulk solution first and then deposit on the metal surfaces. Further buildup of deposits may involve both mechanisms: deposition and crystal growth. Therefore, there may be a direct linkage between the solid particle growth in bulk solution and the scale buildup on the wall surfaces. On the other hand, even if scale formation is due solely to a heterogeneous mechanism, particle growth in the bulk would still affect scale formation by consuming a portion of the scale-forming precursor materials. In either case, solid-particle-formation data must be obtained to understand the problem. Previous and ongoing testing based on the measurement of [Al] and [Si] consumption kinetics have indicated that the format of aluminosilicate may be rapid under evaporator conditions. However, the kinetics of particle formation (both in bulk solution and on surfaces) has not been studied. Conditions that cause extremely rapid particle formation are of particular interest, because in that case the solids-formation reactions in the evaporator would be sensitively dependent on process conditions such as chemical composition, temperature, fluid flow, and heat transfer