REDUCTION OF CONSTRAINTS FOR COUPLED OPERATIONS

[摘要] The homogeneity constraint was implemented in the Defense Waste Processing Facility (DWPF) Product Composition Control System (PCCS) to help ensure that the current durability models would be applicable to the glass compositions being processed during DWPF operations. While the homogeneity constraint is typically an issue at lower waste loadings (WLs), it may impact the operating windows for DWPF operations, where the glass forming systems may be limited to lower waste loadings based on fissile or heat load limits. In the sludge batch 1b (SB1b) variability study, application of the homogeneity constraint at the measurement acceptability region (MAR) limit eliminated much of the potential operating window for DWPF. As a result, Edwards and Brown developed criteria that allowed DWPF to relax the homogeneity constraint from the MAR to the property acceptance region (PAR) criterion, which opened up the operating window for DWPF operations. These criteria are defined as: (1) use the alumina constraint as currently implemented in PCCS (Al{sub 2}O{sub 3} {ge} 3 wt%) and add a sum of alkali constraint with an upper limit of 19.3 wt% ({Sigma}M{sub 2}O < 19.3 wt%), or (2) adjust the lower limit on the Al{sub 2}O{sub 3} constraint to 4 wt% (Al{sub 2}O{sub 3} {ge} 4 wt%). Herman et al. previously demonstrated that these criteria could be used to replace the homogeneity constraint for future sludge-only batches. The compositional region encompassing coupled operations flowsheets could not be bounded as these flowsheets were unknown at the time. With the initiation of coupled operations at DWPF in 2008, the need to revisit the homogeneity constraint was realized. This constraint was specifically addressed through the variability study for SB5 where it was shown that the homogeneity constraint could be ignored if the alumina and alkali constraints were imposed. Additional benefit could be gained if the homogeneity constraint could be replaced by the Al{sub 2}O{sub 3} and sum of alkali constraint for future coupled operations processing based on projections from Revision 14 of the High Level Waste (HLW) System Plan. As with the first phase of testing for sludge-only operations, replacement of the homogeneity constraint with the alumina and sum of alkali constraints will ensure acceptable product durability over the compositional region evaluated. Although these study glasses only provide limited data in a large compositional region, the approach and results are consistent with previous studies that challenged the homogeneity constraint for sludge-only operations. That is, minimal benefit is gained by imposing the homogeneity constraint if the other PCCS constraints are satisfied. The normalized boron releases of all of the glasses are well below the Environmental Assessment (EA) glass results, regardless of thermal history. Although one of the glasses had a normalized boron release of approximately 10 g/L and was not predictable, the glass is still considered acceptable. This particular glass has a low Al{sub 2}O{sub 3} concentration, which may have attributed to the anomalous behavior. Given that poor durability has been previously observed in other glasses with low Al{sub 2}O{sub 3} and Fe{sub 2}O{sub 3} concentrations, including the sludge-only reduction of constraints study, further investigations appear to be warranted. Based on the results of this study, it is recommended that the homogeneity constraint (in its entirety with the associated low frit/high frit constraints) be eliminated for coupled operations as defined by Revision 14 of the HLW System Plan with up to 2 wt% TiO{sub 2}. The use of the alumina and sum of alkali constraints should be continued along with the variability study to determine the predictability of the current durability models and/or that the glasses are acceptable with respect to durability. The use of a variability study for each batch is consistent with the glass product control program and it will help to assess new streams or compositional changes. It is also recommended that the influence of alumina and alkali on durability be studied in greater detail. Limited data suggests that there may be a need to adjust the lower Al{sub 2}O{sub 3} limit and/or the upper alkali limit in order to prevent the fabrication of unacceptable glasses. An in-depth evaluation of all previous data as well as any new data would help to better define an alumina and alkali combination that would avoid potential phase separation and ensure glass durability.

[发布日期] 2009-12-15

[学科分类] 核能源与工程

[关键词] AR FACILITIES;RADIOACTIVE WASTE PROCESSING;VITRIFICATION;GLASS;SLUDGES;FLOWSHEETS;LIMITING VALUES;MODIFICATIONS;ALUMINIUM OXIDES;CORROSION RESISTANCE