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Nitrate-Cancrinite Precipitation on Quartz Sand in Simulated Hanford Tank Solutions

Journal Article · · Environmental Science and Technology
DOI:https://doi.org/10.1021/es0108234· OSTI ID:15005648
 [1];  [2];  [3];  [4]
  1. Virginia Tech
  2. 1800
  3. BATTELLE (PACIFIC NW LAB)
  4. ROCKWELL HANFORD OPER.

High pH, high NaNO3 solutions with varying amounts of dissolved Al were reacted with quartz sand at 88.7 degrees Celcius in order to simulate possible reactions between leaked nuclear waste fluid and primary subsurface minerals at the U.S. Department of Energy's Hanford site in Washington. After 2-10 days, nitrate-cancrinite, a feldspathoid mineral with a zeolite-like crystal structure, precipitated onto the quartz surfaces, cementing the grains together. Estimates of the Keq for the precipitation reaction differ for solutions with 0.1 or 1.0 m OH- (log Keq= 30.4+/- 0.8 and 36.2+/-, respectively). It is inferred that the difference in solubility is attribute to more perfectly crystallinity (i.e., fewer stacking faults) in the higher-pH cancrinite structure. This hypothesis is supported by electron micrographs of crystal morphology and measured rates of Na volatilization under an electron beam. Precipitate crystallinity may be important for radionuclide mobility, because stacking faults in the cancrinite structure can negate its zeolitic cation exchange properties. The log of the precipitation rate depends linearly on the activity of Al(OH)4-in solution. The evolution of Si concentration in experimental solutions was successfully modeled by considering the dependence of quartz dissolution rate on Al(OH)4- activity, cancrinite precipitation, and the reduction of reactive surface area of quartz due to coverage by cancrinite.

Research Organization:
Pacific Northwest National Lab., Richland, WA (US)
Sponsoring Organization:
US Department of Energy (US)
DOE Contract Number:
AC06-76RL01830
OSTI ID:
15005648
Report Number(s):
PNNL-SA-34540; KP1301030
Journal Information:
Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 22 Vol. 35
Country of Publication:
United States
Language:
English