DOE provided a revised reaction rate range (Table 12-1) based on an evaluation of the reaction rate data in Zhang et al. (2000) that corresponds to even shorter reaction times of 18 to 1,180 years (Shrader 2016). The rate calculation assumed order of magnitude uncertainties around the induction periods extrapolated to 25ºC by Zhang et al. (2000), resulting in DOE's prediction of induction periods ranging from 3.3 to 33 years for ERDA-6 brine and 33 to 364 years for GWB brine. These induction period ranges were used with the mean reaction rates and calculated standard deviations from Zhang et al. (2000) to calculate a range of rates for hydromagnesite to magnesite conversion. Using 3.3 years as the minimum induction period at 25ºC in ERDA-6 brine is indefensible because conversion of hydromagnesite to magnesite at 25ºC in laboratory experiments has not been reported. In the absence of any experimental evidence over this reasonably achievable time frame for laboratory experiments, this lower limit is unjustified.
EPA has previously reviewed the Zhang et al. (2000) study and extrapolation of its rate data to low temperature and concluded the extrapolation had many issues, including uncertainties regarding the form of the rate equation, unknown effects of hydromagnesite chemical and physical properties on the induction period, uncertainties in determining the rates during the induction period and questions regarding whether the activation energy would remain constant at lower temperatures. DOE did not consider more recent data, such as investigations showing that citrate, which is present in WIPP repository brines (Table 6-1), can inhibit magnesite growth (Gautier 2012, Gautier et al. 2016), or that higher pH can slow magnesite precipitation (Saldi et al. 2012). DOE's evaluation results are not supported by the available geologic record, which was reviewed by SCA (2008a). Although it is true that magnesite may form under low-temperature hypersaline conditions with high Mg/Ca ratios (SCA 2008a), DOE has not demonstrated that such conditions will exist in the repository. Consequently, DOE's evaluation of the hydromagnesite to magnesite conversion rate (Shrader 2016) is inadequate.
Because of the lack of experimental evidence that hydromagnesite converts to magnesite at 25ºC and uncertainties associated with extrapolating higher temperature data to lower temperature, it is possible that no hydromagnesite will convert to magnesite during the 10,000-year repository performance period. Accordingly, the minimum reaction rate for hydromagnesite conversion must be 0 mol kg[-1] sec[-1]. The Zhang et al. (2000) experiments in saturated NaCl solution are less applicable to WIPP than the GWB experiments because of the possible effects of other WIPP brine constituents on the hydromagnesite conversion rate. The rate data from Zhang et al. (2000) is expressed as an induction period plus a reaction half time. Using the 25ºC extrapolation of the induction period of 273 years and 10 times the reaction half-time of 73 years for essentially complete reaction yields a reaction time of 1,000 years. However, given the uncertainty in the extrapolations, using a smaller reaction time of 200 years would provide a reasonably bounding estimate that is consistent with the "hundreds" of years mentioned by EPA (1998d) and accepted by Clayton (2013) (Table 12-1). The effect of a lower rate range compared to the range used in the CRA-2014 would be less brine production in the repository.
Effects of Water Balance Assumptions on PA
The following issues have been identified in DOE's implementation of the water balance for the CRA-2014 PA:
       DOE developed revised ranges of humid and inundated steel corrosion rates that are higher than the ranges used in the CRA-2014 PA by including data collected at low CO2 concentrations (Section 3.1.2) and EPA has revised the inundated rate upward to account for the effects of higher repository pressure. These higher corrosion rate ranges are more appropriate for the CRA-2019 PA, which would increase gas pressure and decrease brine volumes in the repository
       DOE's assumption that all H2S created by CPR degradation will react instanteously and completely with iron-based metals in the waste and waste containers was not adequately supported (Section 3.1.2). EPA wants to see the stoichiometric coefficients for these reactions set to zero, which will increase gas pressure and decrease brine volumes in the repository
       The MgO hydration rates were based on data from Premier MgO, which is present in smaller quantities than Martin Marietta MgO and also hydrates more slowly than Martin Marietta MgO. It would be appropriate for DOE to develop hydration rates using Martin Marietta MgO and use these rates with Premier MgO hydration rates in the CRA-2019 PA (Section 12.4.1). Including the Martin Marietta MgO hydration rate data is likely to decrease brine volumes in the repository.
       The hydromagnesite conversion rate used in the CRA-2014 PA was inadequately justified. EPA recommends the lower rate range identified in Section 12.4.3 to be included in the CRA-2019 PA, which will decrease brine in the repository.
EPA requested that DOE assess the likely cumulative effects of water balance assumptions on PA (Edwards 2015b, Comment 2-C-5). DOE's response indicated that the effects of the updated water balance and steel corrosion rates implemented for the CRA-2014 PA should be relatively small (Bryson 2015). This assessment was justified by comparing the total normalized releases calculated for the CRA14-BV PA to total normalized releases for the CRA-2014 PA. The total normalized releases for the two PAs differed only slightly because the CRA-2014 PA included implementation of the revised iron corrosion rates, which would increase brine and reduce gas in the repository compared to the previous rates (Section 3.1.2) and implementation of the revised water balance.
Incorporation of chemical processes in addition to anoxic corrosion in the water balance represents a significant step toward a more realistic and defensible water balance calculations for WIPP PA. The available information indicates that the issues identified by EPA with the CRA-2014 PA water balance are likely to have reasonably minor effects on PA. DOE stated that the overall impacts of the water balance assumptions on the normalized releases from the repository are likely to be small because DBRs would be dominated by the large amount of brine entering the repository from a pressurized brine pocket in the Castile (Bryson 2015, Response to Comment 2-C-3). Nevertheless, the interactions of brine with repository contents can be influenced by the brine saturation, including iron corrosion rates and CPR degradation, which can affect gas pressures. Because increased gas pressures have the potential to affect repository releases, EPA will expect DOE to revise the water balance in the CRA-2019 PA to incorporate the changes listed above.

Sensitivity Study

At EPA's request, DOE performed an additional PA (CRA14_SEN4) to assess the effects of a limited number of parameter changes on repository releases. Chemistry parameter changes included revised uncertainty distributions for the +III (SOLMOD3:SOLVAR) and +IV actinide solubility uncertainties (SOLMOD3:SOLVAR) based on EPA-selected experimental data (Section 6.7) and changes to the stoichiometric parameters for reaction of H2S with Fe(s) and Fe(OH)2(s) to correspond with zero reaction rates (Section 12.1). Other changes included in the CRA14_SEN4 PA were the use of an EPA-developed distribution for the probability of encountering pressurized brine during a drilling intrusion (GLOBAL:PBRINE, EPA 2017), use of a reduced lower bound for the distribution of the effective shear strength for erosion of waste (BOREHOLE:TAUFAIL), use of a new version of the DRSPALL code to calculate spallings releases and use of the correct representative length of the northernmost set of panel closures. Changes to the +III and +IV actinide solubility uncertainties increased the ranges of dissolved and total mobilized Am(III) and Pu(III) concentrations and reduced the ranges of dissolved and total mobilized Th(IV), U(IV), Np(IV) and Pu(IV) concentrations in the CRA14_SEN4 PA relative to the CRA-2014 PA (Section 8.0). Comparison of the mean total mobilized actinide concentrations in Castile brine (Table 8-4) shows that the mean Am(III) and Pu(III) concentrations were increased by an order of magnitude in the CRA14_SEN4 PA compared to the CRA-2014 PA. Removing sulfidation from the gas generation and water balance models in the WIPP PA resulted in more gas with higher pressure and less brine with lower saturations in the repository in the CRA14_SEN4 PA calculations than in the CRA-2014 PA calculations (Section 12.1).
Effects of CRA14_SEN4 PA Parameter Changes on Releases

Cuttings and cavings releases are important to PA because these releases dominate total releases at high probabilities. The combined changes made for the CRA14_SEN4 PA resulted in minimal increases in cuttings and cavings releases because of the change to the BOREHOLE:TAUFAIL distribution lower bound (Zeitler and Day 2016).
Spallings releases were affected by the changes related to the iron sulfidation reactions and changes to the GLOBAL:PBRINE distribution. Removing the effects of the iron sulfidation reactions in the CRA14_SEN4 PA resulted in slightly higher gas pressures and decreased saturations in the waste areas, and the revised, higher GLOBAL:PBRINE distribution increased the number of intrusions into pressurized brine below the repository and increased pressures in the repository. The increased pressures caused by the removal of the iron sulfidation reactions and the increased probability of drilling into pressurized brine resulted in increased spallings releases (Zeitler and Day 2016). Spallings releases, however, have minimal effects on total releases in both the CRA-2014 PA and CRA14_SEN4 PA.
Releases through the Culebra can be affected by the volume of brine reaching the Culebra and the actinide concentrations in the brine. The brine volumes flowing up the borehole to the Culebra decreased slightly in the CRA14_SEN4 PA relative to the CRA-2014 PA, which Zeitler and Day (2016) attributed to the removal of iron sulfidation and modification of the northernmost panel closure (Zeitler and Day 2016). The effects of the changed actinide solubility uncertainty distributions were to increase the +III actinide total mobilized concentrations and decrease the +IV actinide total mobilized concentrations, which would be expected to increase Culebra releases because of the higher baseline solubilities of the +III actinides. The increased pressures caused by the revised, higher GLOBAL:PBRINE distributions would tend to increase releases to the Culebra. The combined effects of all changes to the CRA14_SEN4 PA were to generally increase Culebra releases, with a slight decrease in Culebra releases at the lowest probabilities (Zeitler and Day 2016). Releases through the Culebra do not significantly affect total releases.
Removal of the iron sulfidation reactions, the increased GLOBAL:PBRINE distribution, and the changes to the distributions for the +III and +IV actinide solubility uncertainties affected DBR in the CRA14_SEN4 PA. The combined effects of these changes increased DBR at all probabilities (Zeitler and Day 2016). The increase in DBR from the increased SOLMOD3:SOLVAR uncertainty distribution is consistent with regression analysis results for both the CRA-2014 PA and CRA14_SEN4 PA that showed that this parameter is a significant contributor to the uncertainty in total releases. The parameter GLOBAL:PBRINE is a significant contributor to total releases for the CRA14_SEN4 PA as a result of the increased distribution range for this parameter in the CRA14_SEN4 PA.
Total releases calculated for the CRA14_SEN4 PA were minimally changed at high probabilities, because the high-probability releases are dominated by cuttings and cavings. Higher total releases were calculated for the CRA14_SEN4 PA at low probabilities than for the CRA-2014 PA because DBR is the most important cause of releases at low probability. The mean DBR CCDF increased significantly from the CRA-2014 PA to the CRA14_SEN4 PA (Zeitler and Day 2016, Figure 4-4). Because both the GLOBAL:PBRINE distribution and total mobilized +III actinide concentrations increased from the CRA-2014 PA and CRA14_SEN4 PA, the relative importance of these two changes cannot be distinguished.
Possible Effects of Additional Chemistry Parameter Changes

Chemistry-related issues identified by EPA during the CRA-2014 PA completeness review that were not addressed in the CRA14_SEN4 PA included:
 Underestimates of humid and inundated steel corrosion rates,
 Possible increase in gas generation rates due to lead corrosion
 Underestimation of the MgO hydration rate
 Overestimation of the hydromagnesite conversion rate
 Increased probability of the Pu(III) oxidation state
The combined effects of addressing the first four issues would be to reduce brine saturation and to increase gas pressures. Because of the relatively small effects of implementing the revised water balance and steel corrosion rates on releases noted when comparing CRA14-BV and CRA-2014 PA results (Zeitler 2013), it is reasonable to assume that the effects on PA of the steel corrosion rates, lead corrosion, MgO hydration rate, water consumption by brucite carbonation and hydromagnesite conversion rates would be relatively minor. The effects of changes in water saturation would be expected to be relatively unimportant because the amount of water introduced by a borehole intrusion into pressurized brine would likely overwhelm the brine already present in the repository. Higher gas pressures would be expected to increase spallings and possibly other release mechanisms, but it is reasonable to believe that these effects would be overwhelmed by the pressure increases caused by an intruding borehole into pressurized brine.
The effects of a higher likelihood of the Pu(III) oxidation state because of reductive dissolution of Pu(IV) solid (Section <IP_ADDRESS>) were not considered in the CRA14_SEN4 PA. Because of the higher total mobilized Pu(III) concentrations compared to Pu(IV) total mobilized concentrations in the CRA14_SEN4 PA (Table 8-3) and the regression analysis results showing the sensitivity of releases to the +III actinide concentrations through the SOLMOD3:SOLVAR (Zeitler and Sarathi 2017), an increased probability of the Pu(III) oxidation state would be expected to increase DBR releases and consequently to increase total releases at low probabilities. Because of the importance of an increased probability of the Pu(III) oxidation state to repository releases, EPA expects an independent technical review of likely Pu oxidation states to be performed prior to the CRA-2019 PA.
Sensitivity Calculations Conclusions

EPA requested DOE to perform an additional PA, the CRA14_SEN4,  to assess the sensitivity of releases to a limited number of physical and chemical parameter changes:

 EPA-specified actinide uncertainty distributions that increased total mobilized +III actinides and reduced total mobilized +IV actinides
 Iron sulfidation rate parameters equal to zero, simulating iron passivation by H2S
 An EPA-developed distribution for the probability of encountering pressurized brine during a drilling intrusion
 A reduced lower bound for the distribution for the effective shear strength of waste for erosion
The combined changes affected CRA14_SEN4 PA releases compared to the CRA-2014 PA:

       The combined changes resulted in minimal changes to cuttings and cavings releases
       Spallings releases were slightly increased due to slightly higher gas pressures from the removal of sulfidation reactions
       Releases through the Culebra were generally increased, with a slight decrease in releases at the lowest probabilities
       Direct brine releases were increased at all probabilities
       Total releases calculated minimally changed at high probabilities where total releases are dominated by cuttings and cavings, but were increased at low probabilities where releases are dominated by DBR
Summary and Conclusions

This technical support document summarizes EPA's review of chemistry-related CRA-2014 PA issues, with the conclusions outlined below. DOE updated many of the chemistry-related PA parameters and EPA has identified issues with a number of these changes. The results of this review, including the CRA14_SEN4 PA sensitivity analysis, show that predicted repository releases will remain within regulatory limits. However, EPA's review indicated many of the chemistry related parmaters that DOE's adopted in the 2014-CRA PA were not aligned with the available experimental data. Consequently, EPA would like to see DOE address those specific issues identified by EPA in this technical report for the CRA-2019 PA to minimize uncertainties associated with the PA results and to increase its defensibility.
The conceptual model and implementation of gas generation from anoxic corrosion of iron-based metals used for the CRA-2014 PA are supported by the available data. Iron corrosion rates for the CRA-2014 PA were lower than previous WIPP PAs based on new project-specific investigations of humid and inundated iron corrosion rates. EPA would like the sampled distributions for the humid and inundated rates to be modified for the CRA-2019 PA to account for the presence of low CO2 concentrations in the WIPP repository and the inundated corrosion rate also increased to account for the effects of high repository pressures. For the CRA-2014 PA, DOE assumed that all H2S generated by CPR degradation would instantaneously react with iron metal and Fe(OH)2. This assumption is inconsistent with project-specific data that show H2S may passivate iron. Because the reaction of H2S with Fe(OH)2 can result in lower gas pressures and reduce spallings releases and DBRs, EPA would also like these iron sulfidation reactions eliminated from the CRA-2019 PA by setting the appropriate stoichiometric coefficients to zero.
Metals and alloys other than iron-based materials in the WIPP waste or packaging materials, such as aluminum and lead, may generate gas through anoxic corrosion. Inventories of these metals for the CRA-2014 PA were insignificant relative to iron-based metals and alloys, so aluminum and lead corrosion were not included in the CRA-2014 PA gas generation calculations. However, future lead inventories are likely to significantly increase compared to the CRA-2014 PA inventory because of the recent approval of shielded containers for RH waste disposal. Bounding calculations based on the volumes of waste streams that are candidates for disposal in shielded containers would be appropriate to assess the possible significance of gas generation from lead corrosion, which will provide a more defensible calculation of potential WIPP gas generation rates.
The microbial gas generation rates used for the CRA-2014 PA are suitable for modeling gas generation rates from degradation of cellulosic materials, but may overestimate gas generation rates from the degradation of plastics and rubber. DOE accounted for uncertainties regarding the rates of plastic and rubber degradation in the WIPP repository environment by assuming plastic and rubber degradation occurs in only 25% of the realizations. Based on the available data, the current approach for modeling microbial gas generation rates is appropriate for PA.
The assumption that radiolytic processes will not significantly influence overall rates of gas generation has remained unchanged since the CCA PA. However, lower microbial gas generation rates used in the PABC04, PABC09 and CRA-2014 PA may invalidate this assumption. DOE has perfomed H2(g) monitoring in WIPP Panels 3 and 4 and concluded that radiolytic H2(g) generation is occurring. Future PAs will be strengthened if DOE assesses the possible significance of radiolytic gas generation relative to the rates of gas generation by microbial degradation and anoxic corrosion for the CRA-2019 PA.
The available data indicate that the MgO backfill will adequately control brine pH and CO2 fugacities, and thereby limit actinide solubilities in WIPP brines under inundated conditions. Because of uncertainties in the rate at which hydromagnesite will convert to magnesite in the repository environment, PA calculations of actinide solubilities assume that the brucite-hydromagnesite reaction will buffer CO2 fugacity at low levels consistent with relatively low actinide solubilities under inundated conditions. Calculation of the amount of emplaced MgO appropriately accounts for the uncertainties associated with the rate of hydromagnesite conversion to magnesite and the chemical composition of the MgO. The current MgO emplacement plan ensures that a sufficient quantity of MgO is emplaced in each room of the repository. The MgO reactivity testing procedure and test results provided by DOE demonstrate that the current backfill material contains a sufficient percentage of reactive periclase plus lime to control chemical conditions in the repository, and that the current testing procedure would detect any MgO shipments with inadequate reactive material percentages.
Assumptions related to actinide oxidation states in the WIPP repository have remained unchanged since they were developed and peer reviewed for the CCA. It is assumed for PA that Th(IV), Am(III), and Cm(III) are the only oxidation states of these actinides that will be present in the WIPP repository. It is also assumed that neptunium may be present in the +IV or +V oxidation states and uranium may be present in the +IV or +VI oxidation states. Because reducing conditions will be established in the repository shortly after closure, the peer-reviewed oxidation state assumptions for neptunium and uranium remain appropriate, although conservative.
For all WIPP PAs, DOE has assumed equal probabilities that aqueous and solid-phase plutonium will be present in either the +III or +IV oxidation states. EPA's interpretation of data that have become available since the CRA-2009 is that the data demonstrate a high likelihood that plutonium concentrations in WIPP brines will be controlled by the solubility of Pu(III) solids in equilibrium with Pu(III) aqueous species or by the solubility of Pu(IV) solids in equilibrium with Pu(III) aqueous species, also referred to as reductive dissolution. Reductive dissolution of Pu(IV) solids in equilibrium with Pu(III) aqueous species results in higher dissolved plutonium concentrations than would occur if Pu(IV) solids are in equilibrium with Pu(IV) aqueous species.
Dissolved Pu(III) and total mobilized Pu(III) used in the more oxidizing realizations may have beensignificantly underestimated in the CRA-2014 PA. This underestimation in turn likely caused an underestimation of total mobilized plutonium concentrations in DBRs for the CRA14_SEN4 and a consequent underestimation of total releases at low probabilities. Because plutonium oxidation state will significantly influence total mobilized plutonium in PA, EPA would like to see an independent technical review of the likely plutonium oxidation states in the repository setting as soon as possible, with an update incorporated into PA calculations.
DOE included the solubility for phase 5 in the EQ3/6 database (DATA0.FM1) used to calculate actinide solubilities for the CRA-2014 PA, because this solid has been shown to form in GWB brines. DOE (2014b, Appendix SOTERM-2014) provided a qualitative review of actinide solubility and speciation data relevant to WIPP brines that have become available since the PABC04. However, DOE did not revise the actinide aqueous speciation or solubility data in DATA0.FM1. Consideration of all new geochemical data and other relevant data is required for each CRA [40 CFR 194.15(a)]. Because DOE did not quantitatively re-evaluate the data in the DATA0.FM1 database, there is uncertainty regarding the possible effects of the new data on the CRA-2014 PA predictions of the +III and +IV actinide solubilities.
In response to EPA comments during the CRA-2014 completeness review, DOE revised the EQ3/6 database used in the CRA-2014 PA actinide solubility calculations and produced DATA0.FM2. The revised database included revisions to the hydromagnesite solubility, addition of borate aqueous and solid species, revisions to EDTA aqueous and solid species, revisions to citrate aqueous and solid species, addition of the MgSO4(aq) aqueous species and addition of lead aqueous and solid species. EPA performed a preliminary review of the revised database and concluded that the hydromagnesite solubility previously used for WIPP PA is much more preferable for inclusion in the CRA-2019 because of uncertainties associated with the experiments used to determine the revised hydromagnesite solubility. EPA acceptance of the new borate, lead data and MgSO4(aq) data added to the database and the revised EDTA and citrate data will require review of more recent data and analysis of the revised data with respect to appropriate acceptance criteria. In addition, EPA has determined that aqueous speciation and Pitzer parameters for the Th(IV)-carbonate species from Altmaier et al. (2005, 2006) and thermodynamic and Pitzer parameters from Neck et al. (2009) for Am(III) aqueous species and solids phases would be appropriate revisions to the EQ3/6 database. Both sets of thermodynamic data are more consistent with existing actinide solubility results from the literature than the data currently in DATA0.FM1. EPA encourages DOE to update the geochemical database for the next CRAwith the latest data and to provide the Agency with proper justifications for the updates.
DOE has not developed an aqueous speciation and solubility model for U(VI) and continues to use a fixed concentration of 1.0  10[-3] M for the dissolved concentration. DOE has reported the results of U(VI) solubility measurements in carbonate-free WIPP brines. Because of the likely importance of carbonate complexation on the solubility of U(VI), these results cannot be used to determine likely U(VI) concentrations under anticipated WIPP repository conditions. Thus, continued use of a fixed concentration is appropriate.
Inconsistencies were identified in DOE's selection of +III and +IV actinide solubility data that were used to develop the CRA-2014 PA solubility uncertainty distributions. EPA re-evaluated the selection criteria and the +III and +IV actinide solubility data selection process and specified the solubility data used to develop revised +III and +IV actinide solubility uncertainty distributions. The revised +III actinide solubility uncertainty distribution had a higher mean and median than the distribution used for the CRA-2014 PA, and the revised +IV actinide solubility uncertainty distribution had a lower mean and median than the distribution used for the CRA-2014 PA. Because of the importance of +III actinides for DBR and consequently for total releases from the repository at low probabilities, results of the CRA14_SEN4 PA show that these changed actinide solubility uncertainty distributions result in higher repository releases at low probabilities.
Additional mineral-fragment colloid data from experiments with Pu(VI) in the presence of iron metal and magnetite in WIPP brines indicated that the current parameters are adequately bounding of the data. However, DOE has not investigated the potential formation of pseudocolloids from MgO hydration and carbonation products under WIPP conditions. Because colloids capable of transporting actinides have been demonstrated to form from reaction of MgO in brines under some conditions, this omission introduces some uncertainty into the colloidal actinide source term model. To minimize this uncertainty, we recommend DOE evaluate the potential formation of mineral-fragment colloids from MgO hydration and carbonation under WIPP-relevant conditions before the CRA-2019 PA.
Intrinsic colloid concentrations used in the CRA-2014 PA were revised based on new WIPP-specific data. The Th(IV) intrinsic colloid data were developed using experimental data from an extremely narrow pcH range of 9  -  10. EPA expects DOE to revise the Th(IV) intrinsic colloid parameter to reflect upper bounding values for data collected from experiments within the pcH range of 8.5  -  10.5. The Pu(III) intrinsic colloid parameter does not appear to be an upper, bounding value and should also be revised to be consistent with a reasonable upper bound.
DOE revised the microbial colloid parameters for the CRA-2014 PA based on newly collected data. DOE changed the maximum concentrations for the microbially associated actinides based on a revised conceptual model assumption regarding the upper limit on microbially associated actinides. Whereas for previous WIPP PAs it was assumed the maximum microbial colloids concentration would be the concentration at which no growth was observed, DOE revised this upper limit to be the concentration calculated from an assumed maximum cell concentration multiplied by the moles of actinides per cell. This change alters the conceptual model and has significant effects on total mobilized actinides.
Because of the short reaction times in tests reported by DOE, the CRA-2014 PA microbial proportionality constants likely include only biosorption and not bioaccumulation or biomineralization. Omission of bioaccumulation and biomineralization represents a conceptual model change because previous WIPP PAs included biosorption, bioaccumulation and biomineralization. DOE has stated that further research into the biosorption, bioaccumulation and biomineralization processes is planned, and EPA would like these investigations to include longer reaction times to substantiate steady state conditions and to include the possible effects of bioaccumulation and biomineralization. Uncertainty has been introduced into the biosorption data DOE developed because of the possible inclusion of intrinsic colloids in the experimental solutions which may or may not have sorbed; EPA recommends that DOE use 2 nm filtration to remove intrinsic colloids from their post-test solutions in future experiments to establish the dissolved concentration for calculating microbial colloid proportionality constant parameter values.
Based on EPA's assessment of DOE's microbial colloid conceptual model changes and microbial colloid experiments, EPA will reject the CRA-2014 PA microbial colloid parameters for the CRA-2019 PA. We encourage DOE to continue their investigation of microbial colloid parameters and expect any updates for the CRA-2019 PA to be consistent with the peer-reviewed conceptual model assumptions.
The results of the mobile actinide source term calculations indicate that for the case using mean values of the CRA-2014 PA parameters, total mobile Am(III) concentrations consist mainly of dissolved Am(III) and Am(III) associated with humic colloids, with microbial colloid Am(III) limited by the maximum concentration. Total mobile Pu concentrations calculated using mean parameter values for the CRA-2014 PA were dominated by dissolved Pu(III) and Pu(III) associated with humic and microbial colloids and by humic and microbial colloids for Pu(IV). Using the mean CRA-2014 PA parameter values, the total mobilized Pu(IV) concentrations for both GWB and ERDA-6 brine exceed the total mobilized Pu(III) concentrations. Higher total mobilized Pu(IV) than Pu(III) concentrations are the result of the negative mean value for the +III solubility uncertainty distribution, and demonstrates the importance of developing a defensible actinide solubility data set for determining this distribution for the CRA-2019 PA. The revised maximum microbial colloid parameter for Am(III) also significantly affects total mobilized Am(III) concentrations, and we expect DOE to resolve the issues surrounding the maximum actinide concentrations associated with microbial colloids as soon as possible and ideally for the CRA-2019 PA.
The total mobilized actinide concentrations calculations using CRA14_SEN4 PA mean parameters differed from the CRA-2014 PA calculations only in the +III and +IV actinide solubility uncertainty parameters. Using the CRA14_SEN4 PA mean parameters, microbially associated Am(III) and Pu(III) concentrations were limited by the maximum concentration established for the CRA-2014 PA. This result illustrates the importance of the issues identified with the revised parameters for the maximum microbially associated actinide concentrations. Because of changes made to the +III and +IV actinide solubility uncertainty distributions for the CRA14_SEN4 PA, the mean total mobilized Pu(III) concentrations in GWB and ERDA-6 brines exceed the mean total mobilized Pu(IV) concentrations, which is consistent with previous WIPP PAs, such as the PABC09.
Distribution coefficients used to model actinide transport through the Culebra for the CRA-2014 PA are consistent with the estimated organic ligand concentrations based on the CRA-2014 PA inventory for these compounds. These Kd values are likely to provide a conservative assessment of actinide transport through the Culebra.
The potential effects of heterogeneous waste loading are unlikely to significantly affect actinide solubilities, except in the case where a large proportion of the organic ligands in the inventory are placed in a single panel. DOE has accounted for this possibility in the actinide solubility calculations by assuming that the entire organic ligand inventory is dissolved in the minimum amount of brine necessary for a release from the repository. Provided that the inventory of organic ligands is adequately bounded, this approach ensures that the effects of heterogeneous waste placement are adequately accounted for in the actinide solubility calculations.
The only chemical process included in the water balance calculations for the CCA PAVT, PABC04 and PABC09 was the consumption of water by anoxic corrosion. DOE modified the water balance for the CRA-2014 PA to also include water production by microbial degradation of CPR, water consumption by the MgO hydration reaction and water produced by conversion of hydromagnesite to magnesite. Incorporation of these chemical processes in addition to anoxic corrosion in the water balance represents a significant improvement in the water balance calculations for WIPP PA. However, EPA has found several outstanding issues to be addressed for CRA-2019 including: using the revised ranges of humid and inundated steel corrosion rates that are higher than the ranges used in the CRA-2014 PA, removing the steel sulfidation reactions from the water balance by setting the relevant stoichiometric parameters to zero, revising the MgO hydration rates to account for the higher rates of hydration of Martin Marietta MgO and modifying the hydromagnesite conversion rate to a lower range of values.
DOE performed an additional PA (CRA14_SEN4 PA) to assess the effects of a limited number of parameter changes on repository releases. The chemistry-related parameter changes relative to the CRA-2014 PA for this sensitivity analysis were revised uncertainty distributions for the +III and +IV actinide solubilities and changes to the stoichiometric parameters for reaction of H2S with Fe(s) and Fe(OH)2(s) to correspond with zero reaction rates. The use of an EPA-developed distribution for the probability of encountering pressurized brine during a drilling intrusion, use of a reduced lower bound for the distribution of the effective shear strength for erosion, use of a new version of the DRSPALL code and use of the correct representative length of the northernmost set of panel closures were also included in the CRA14_SEN4 PA. Total releases calculated for the CRA14_SEN4 PA relative to the CRA-2014 PA were minimally changed at high probabilities, because the high-probability releases are dominated by cuttings and cavings. Higher total releases were calculated for the CRA14_SEN4 PA at low probabilities than for the CRA-2014 PA because DBR is the most important cause of releases at low probability and the mean DBR CCDF increased significantly from the CRA-2014 PA to the CRA14_SEN4 PA. Because both the distribution for the probability of encountering pressurized brine during a drilling intrusion and the sampled range of total mobilized +III actinide concentrations increased from the CRA-2014 PA and CRA14_SEN4 PA, the relative importance of these two changes to DBR cannot be distinguished.
The following is a summary of the issues related to chemical processes EPA would like to see DOE address prior to the CRA-2019:
       Use the revised, higher humid and inundated anoxic corrosion rate ranges identified by EPA that account for the effects of CO2 and high pressure
       Confirm that the steel surface area per unit disposal volume is representative of WIPP waste using updated inventory data, the sheet metal surrogate and 55-gallon drum surrogate assumptions and updated waste emplacement data
       Develop a reasonable upper-bound estimate for the lead inventory and lead surface area per unit disposal volume for the CRA-2019 PA that adequately accounts for the increased lead associated with shielded containers; if the upper-bound lead inventory is significant relative to iron-based metals and alloys, we recommend that DOE use available project-specific lead corrosion data to assess the effects of lead corrosion on gas generation and brine consumption in the WIPP repository
       Use the available radiolytic H2(g) generation data from monitoring of sealed WIPP panels to evaluate whether radiolytic gas generation rate is significant relative to the rates of gas generation by microbial degradation and anoxic corrosion
       Remove the assumption that all H2S(g) generated by CPR degradation will instantaneously react with Fe(s) and Fe(OH)2(s) from the gas generation rate calculations by revising the relevant stoichiometric coefficients
       Perform an independent technical review of likely plutonium oxidation states in solids and aqueous species in the repository and update the model as soon as possible using recommendations from this review
       Use the solubility of hydromagnesite established by Robie and Hemingway (1973) in the EQ3/6 database
       Review the results of investigations published after the CRA-2014 cutoff date related to complexation of +III actinides by borate species and precipitation of borate solid phases, and if appropriate, revise the EQ3/6 thermodynamic database to incorporate the data
       Use the data provided by Altmaier et al. (2005, 2006) to develop revised aqueous speciation and Pitzer parameters for the Th(IV)-carbonate aqueous species and incorporate the results in the EQ3/6 database
       Use the results of the Neck et al. (2009) Nd(OH)3(s) solubility study to update the solubility of Am(OH)3(s) in the EQ3/6 database
       Provide supporting information for the revised data in the EQ3/6 database DATA0.FM2 to demonstrate agreement with acceptance criteria; EPA needs this supporting information in advance of the CRA-2019 to enable EPA review and acceptance before its use to calculate dissolved actinide concentrations for the CRA-2019 PA
       Modify the criteria to select solubility data for the +III and +IV actinide solubility uncertainty distributions
       Experimentally evaluate formation of mineral fragment colloids from MgO hydration and carbonation products and their effects on total mobilized actinides
       Revise the Th(IV) intrinsic colloid parameter to be consistent with upper bounding values for samples collected within the pcH range of 8.5  -  10.5
       Provide documentation for the data used to determine the Pu(III) and Am(III) intrinsic colloid parameters and develop a Pu(III) intrinsic colloid parameter that is an upper bounding value
       Incorporate the effects of bioaccumulation and biomineralization in addition to biosorption in the development of revised microbial colloid parameters; until the effects of bioaccumulation and biomineralization have been included in the revised parameters, we will accept the higher proportionality constants (either from the CCA PA or CRA-2014 PA) for the CRA-2019 PA
       Use the higher CAPMIC parameters developed for the CCA based on the conceptual model assumption that these parameters represent the concentrations at which no growth occurs
       Use 2 nm filtration to remove intrinsic colloids from post-test solutions in future microbial colloid experiments to establish the dissolved concentration for calculating proportionality constants for microbial colloids
       Develop MgO hydration rates that adequately account for the more rapid hydration rates of Martin Marietta MgO relative to Premier MgO for use in the CRA-2019 PA water balance
       Use the lower rate range established by EPA for the hydromagnesite conversion rate for the CRA-2019 PA water balance

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Vugrin, E.D., M.B. Nemer, and S. Wagner, 2007. Uncertainties Affecting MgO Effectiveness and Calculation of the MgO Effective Excess Factor. Revision 1, Sandia National Laboratories, Carlsbad, New Mexico. ERMS 546377.
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Xiong, Y.L. 2011a. Experimental determination of solubility constant of hydromagnesite (5424) in NaCl solutions up to 4.4 m at room temperature. Chemical Geology 284:262-269.

Xiong, Y. 2011b. Release of EQ3/6 Database DATA0.FM1. Email to J.J. Long, Sandia National Laboratories, Carlsbad, New Mexico, March 9, 2011.

Xiong, Y. 2012a. Experimental Determination of Solubility Constant of Di-Calcium Ethylenediaminetetraacetic acid (Ca2EDTA), Ca2C10H12N2O8(s), in the NaCl-H2O System. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 558669.

Xiong, Y. 2012b. Analysis Plan AP-134, Revision 3, Analysis Plan for Derivation of Pitzer Parameters in Support of Experimental Work at LANL-CO. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 557474.

Xiong, Y. 2012c. Second Milestone Report on Test Plan TP 10-01 "Experimental Study of Thermodynamic Parameters of Borate in WIPP Relevant Brines at Sandia National Laboratories Carlsbad Facility." Sandia National Laboratories, Carlsbad, New Mexico, ERMS 557333.

Xiong, Y. 2012d. Thermodynamic Model for the Na-B(OH)3-Cl-SO4 System, Revision 1, Superseding ERMS 558111. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 558566.

Xiong, Y.L. 2013a. AP-154, Revision 2, Analysis Plan for Derivation of Thermodynamic Properties Including Pitzer Parameters for Solubility Studies of Iron, Lead and EDTA. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 561114.

Xiong, Y.L. 2013b. Calculations of Thermodynamic Parameters in EDTA System for Experimental Data from Carlsbad Environmental Monitoring and Research Center. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 560761.

Xiong, Y.L. 2014a. AP-155, Revision 3, Analysis Plan for Derivation of Thermodynamic Properties Including Pitzer Parameters for Solubility Studies of Borate. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 562807.

Xiong, Y. 2014b. Experimental and Thermodynamic Modeling of PbCit[-] Interactions in NaCl and MgCl2 Solutions. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 562836.

Xiong, Y. 2014c. Experimental and Thermodynamic Modeling of PbEDTA[2][-] Interactions in NaCl and MgCl2 Solutions. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 562877.

Xiong, Y. 2015a. Derivation of Thermodynamic Parameters in Borate Systems for Experimental Data Under TP10-01. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 564800.

Xiong, Y. 2015b. Experimental and Thermodynamic Modeling Solubility of Cerussite, PbCO3(cr), in the Carbonate System to High Ionic Strengths, Revision 1, Supersedes ERMS 561917. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 564929.
Xiong, Y. 2015c. Experimental determination of lead carbonate solubility at high ionic strengths: a Pitzer model description. Monatshefte für Chemie 146:1433-1443.
Xiong, Y. 2015d. Experimental Determination of Solubilities of Lead Oxalate (PbC2O4), Di-calcium ethylenediamenetetraacetic acid (Ca2EDTA(s)) in MgCl2-H2O System, and Earlandite (Ca3[C3H5O(COO)3]2·4H2O) in NaCl-H2O and MgCl2-H2O Systems, and Their Respective Pitzer Interaction Parameters, Revision 1, Supersedes ERMS 564844. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 564948.

Xiong, Y. 2015e. Modeling Equilibrium Constant for AmHB4O7[2], by reevaluation of the Nd(III) data for NdHB4O7[2+], and its associated Pitzer parameters to be consistent with the WIPP thermodynamic model. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 564857.
Xiong, Y. 2015f. Recalculation of Solubility Constants of Synthetic Hydromagnesite(5424) Using the Pitzer Model. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 564356.
Xiong, Y.L. in press. Comment on "Hydromagnesite solubility product and growth kinetics in aqueous solution from 25 to 75ºC" by Gautier, Q., Bénézeth, P., Mavormatis, V., and Schott, J. Geochemica et Cosmochimica Acta available online December, 2016.
Xiong, Y., and P.S. Domski. 2016a. Uncertainty Analysis of Actinide Solubilities for CRA 2014 Sensitivity Investigation Number 4 (CRA 2014_SEN4). Sandia National Laboratories, Carlsbad, New Mexico, ERMS 567306.
Xiong, Y., and P.S. Domski. 2016b. Updating the WIPP Thermodynamic Database, Revision 1, Supersedes ERMS 565730. Sandia National Laboratories, Carlsbad, New Mexico, ERMS 566047.