Title: Laboratory studies of 2H evaporator scale dissolution in dilute nitric acid

The rate of 2H evaporator scale solids dissolution in dilute nitric acid has been experimentally evaluated under laboratory conditions in the SRNL shielded cells. The 2H scale sample used for the dissolution study came from the bottom of the evaporator cone section and the wall section of the evaporator cone. The accumulation rate of aluminum and silicon, assumed to be the two principal elemental constituents of the 2H evaporator scale aluminosilicate mineral, were monitored in solution. Aluminum and silicon concentration changes, with heating time at a constant oven temperature of 90 deg C, were used to ascertain the extent of dissolution of the 2H evaporator scale mineral. The 2H evaporator scale solids, assumed to be composed of mostly aluminosilicate mineral, readily dissolves in 1.5 and 1.25 M dilute nitric acid solutions yielding principal elemental components of aluminum and silicon in solution. The 2H scale dissolution rate constant, based on aluminum accumulation in 1.5 and 1.25 M dilute nitric acid solution are, respectively, 9.21E-04 ± 6.39E-04 min{sup -1} and 1.07E-03 ± 7.51E-05 min{sup -1}. Silicon accumulation rate in solution does track the aluminum accumulation profile during the first few minutes of scale dissolution. It however diverges towards the end of the scale dissolution. This divergence therefore means the aluminum-to-silicon ratio in the first phase of the scale dissolution (non-steady state conditions) is different from the ratio towards the end of the scale dissolution. Possible causes of this change in silicon accumulation in solution as the scale dissolution progresses may include silicon precipitation from solution or the 2H evaporator scale is a heterogeneous mixture of aluminosilicate minerals with several impurities. The average half-life for the decomposition of the 2H evaporator scale mineral in 1.5 M nitric acid is 12.5 hours, while the half-life for the decomposition of the 2H evaporator scale in 1.25 M nitric acid is 10.8 hours. Based on averaging the two half-lives from the 2H scale acid dissolution in 1.25 and 1.5 M nitric acid solutions, a reasonable half-live for the dissolution of 2H scales in dilute nitric acid is 11.7 ± 1.3 hours. The plant operational time for chemically cleaning (soaking) the 2H evaporator with dilute nitric acid is 32 hours. It therefore may require about 3 half-lives or less to completely dissolve most of the scales in the Evaporator pot which come into contact with the dilute nitric acid solution. On a mass basis, the Al-to-Si ratio for the scale dissolution in 1.5 M nitric acid averaged 1.30 ± 0.20 and averaged 1.18 ± 0.10 for the 2H scale dissolution in 1.25 M nitric acid. These aluminum-to-silicon ratios are in fairly good agreement with ratios from previous studies. Therefore, there is still more aluminum in the 2H evaporator scales than silicon which implies that there are no significant changes in scale properties which will exclude nitric acid as a viable protic solvent for aluminosilicate scale buildup dissolution from the 2H evaporator. Overall, the monitoring of the scale decomposition reaction in 1.25 and 1.5 M nitric acid may be better ascertained through the determination of aluminum concentration in solution than monitoring silicon in solution. Silicon solution chemistry may lead to partial precipitating of silicon with time as the scale and acid solution is heated.