Results of the FY09 Enhanced DOE High Level Waste Melter Throughput Studies at SRNL

Johnson, F. ; Edwards, T.

Savannah River Site (S.C.)

关键词: Waste Processing;    X-Ray Diffraction;    Waste Forms;    Chemical Composition;    Leachates;   

DOI  :  10.2172/983400
RP-ID  :  SRNL-STI-2009-00778
RP-ID  :  DE-AC09-08SR22470
RP-ID  :  983400

美国|英语

来源: UNT Digital Library

【 摘 要 】

High-level waste (HLW) throughput (i.e., the amount of waste processed per unit time) is a function of two critical parameters: waste loading (WL) and melt rate. For the Waste Treatment and Immobilization Plant (WTP) at the Hanford Site and the Defense Waste Processing Facility (DWPF) at the Savannah River Site (SRS), increasing HLW throughput would significantly reduce the overall mission life cycle costs for the Department of Energy (DOE). The objective of this task is to develop data, assess property models, and refine or develop the necessary models to support increased WL of HLW at SRS. It is a continuation of the studies initiated in FY07, but is under the specific guidance of a Task Change Request (TCR)/Work Authorization received from DOE headquarters (Project Number RV071301). Using the data generated in FY07, FY08 and historical data, two test matrices (60 glasses total) were developed at the Savannah River National Laboratory (SRNL) in order to generate data in broader compositional regions. These glasses were fabricated and characterized using chemical composition analysis, X-ray Diffraction (XRD), viscosity, liquidus temperature (TL) measurement and durability as defined by the Product Consistency Test (PCT). The results of this study are summarized below: (1) In general, the current durability model predicts the durabilities of higher waste loading glasses quite well. A few of the glasses exhibited poorer durability than predicted. (2) Some of the glasses exhibited anomalous behavior with respect to durability (normalized leachate for boron (NL [B])). The quenched samples of FY09EM21-02, -07 and -21 contained no nepheline or other wasteform affecting crystals, but have unacceptable NL [B] values (> 10 g/L). The ccc sample of FY09EM21-07 has a NL [B] value that is more than one half the value of the quenched sample. These glasses also have lower concentrations of Al{sub 2}O{sub 3} and SiO{sub 2}. (3) Five of the ccc samples (EM-13, -14, -15, -29 and -30) completely crystallized with both magnetite and nepheline, and still had extremely low NL [B] values. These particular glasses have more CaO present than any of the other glasses in the matrix. It appears that while all of the glasses contain nepheline, the NL [B] values decrease as the CaO concentration increases from 2.3 wt% to 4.3 wt%. A different form of nepheline may be created at higher concentrations of CaO that does not significantly reduce glass durability. (4) The T{sub L} model appears to be under-predicting the measured values of higher waste loading glasses. Trends in T{sub L} with composition are not evident in the data from these studies. (5) A small number of glasses in the FY09 matrix have measured viscosities that are much lower than the viscosity range over which the current model was developed. The decrease in viscosity is due to a higher concentration of non-bridging oxygens (NBO). A high iron concentration is the cause of the increase in NBO. Durability, viscosity and T{sub L} data collected during FY07 and FY09 that specifically targeted higher waste loading glasses was compiled and assessed. It appears that additional data may be required to expand the coverage of the T{sub L} and viscosity models for higher waste loading glasses. In general, the compositional regions of the higher waste loading glasses are very different than those used to develop these models. On the other hand, the current durability model seems to be applicable to the new data. At this time, there is no evidence to modify this model; however additional experimental studies should be conducted to determine the cause of the anomalous durability data.