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Section 1: Identification RPP-RPT-50703 Rev.01A 8/23/2016 - 10:10 AM 1 of 77 Release Stamp DOCUMENT RELEASE AND CHANGE FORM Prepared For the U.S. Department of Energy, Assistant Secretary for Environmental Management By Washington River Protection Solutions, LLC., PO Box 850, Richland, WA 99352 Contractor For U.S. Department of Energy, Office of River Protection, under Contract DE-AC27-08RV14800 DATE: TRADEMARK DISCLAIMER: Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States government or any agency thereof or its contractors or subcontractors. Printed in the United States of America. Aug 23, 2016 1. Doc No: RPP-RPT-50703 Rev. 01A 2. Title: Development of a Thermodynamic Model for the Hanford Tank Waste Simulator (HTWOS) 3. Project Number: ☒ N/A 4. Design Verification Required: ☐ Yes ☒ No 5. USQ Number: ☒ N/A 6. PrHA Number Rev. ☒ N/A Clearance Review Restriction Type: public 7. Approvals Title Name Signature Date Checker CREE, LAURA H CREE, LAURA H 08/16/2016 Clearance Review RAYMER, JULIA R RAYMER, JULIA R 08/23/2016 Document Control Approval MANOR, TAMI MANOR, TAMI 08/23/2016 Originator BRITTON, MICHAEL D BRITTON, MICHAEL D 08/16/2016 Quality Assurance DELEON, SOSTEN O DELEON, SOSTEN O 08/16/2016 Responsible Manager CREE, LAURA H CREE, LAURA H 08/16/2016 8. Description of Change and Justification Updated the reduced chemical potential coefficient vlaues for Na2SO4 and Na2SO4·10H2O in Table A.1, as the original values were incorrect. Added mineral names for double salts NaNO2·Na2SO4·H2O, Na3FSO4, and Na7F(PO4)2·19H2O for consistency with other double sales evaluated. Changed the name of the author's company from EnergySolutions to Atkins Global on the cover page. 9. TBDs or Holds ☒ N/A 10. Related Structures, Systems, and Components a. Related Building/Facilities ☒ N/A b. Related Systems ☒ N/A c. Related Equipment ID Nos. (EIN) ☒ N/A 11. Impacted Documents – Engineering ☒ N/A Document Number Rev. Title 12. Impacted Documents (Outside SPF): N/A 13. Related Documents ☐ N/A Document Number Rev. Title RPP-51192 00 Plan for Evaluation of the HTWOS Integrated Solubility Model Predictions RPP-PLAN-46002 00 WASH AND LEACH FACTOR WORK PLAN SVF-2375 00 SVF-2375-Rev0_GEMS.xlsm 14. Distribution Name Organization ARM, STUART T ONE SYS RPP INTEGRTD FLOWSHEET BELSHER, JEREMY D ONE SYS SYSTEM PLNG & MODELING BERGMANN, LINDA M ONE SYS SYSTEM PLNG & MODELING BRITTON, MICHAEL D ONE SYS PROJECT FLOWSHEETS HERTING, DANIEL L PROCESS CHEMISTRY HO, QUYNH-DAO T ONE SYS PROJECT FLOWSHEETS JASPER, RUSSELL T ONE SYS SYSTEM PLNG & MODELING REAKSECKER, SEAN D ONE SYS SYSTEM PLNG & MODELING REYNOLDS, JACOB G TNK WST INVENTORY & CHARACTZTN 1 SPF-001 (Rev.D1) RPP-RPT-50703 Rev.01A 8/23/2016 - 10:10 AM 2 of 77 RPP-RPT-50703, Rev. 1A Development of a Thermodynamic Model for the Hanford Tank Waste Simulator (HTWOS) R. Carter Atkins Global, LLC 2345 Stevens Drive, Suite 240 Richland, WA 99352 U.S. Department of Energy Contract DE-AC27-08RV14800 EDT/ECN: DRF UC: Cost Center: 2PH00 Charge Code: B&R Code: Total Pages: 77 TM 08/23/16 Key Words: Thermodynamics, Pitzer ion interaction model, water activity, solute activity, molality, ionic strength, solubility, Hanford crystal phases, osmotic coefficient, activity coefficient, HTWOS. Abstract: This report describes the multicomponent Pitzer ion interaction model and the development of a database of temperature dependent parameter coefficients for ultimate use with the model in the Hanford Tank Waste Simulator (HTWOS). The bulk components included in the termodynamic model include sodium nitrate, sodium nitrite, sodium hydroxide, sodium fluoride, sodium chloride, sodium carbonate, sodium phosphate, sodium oxalate and gibbsite. To ensure the final parameters were self-consistent, they were optimized by fitting the model to experimentally determined solubility data.This optimized model allows predictions of phase speciation to high ionic strengths and temperatures from 0 to 100 °C for Hanford Tank waste. TRADEMARK DISCLAIMER. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof or its contractors or subcontractors. DATE: Aug 23, 2016 By Julia Raymer at 10:32 am, Aug 23, 2016 Release Approval Date Release Stamp Approved For Public Release A-6002-767 (REV 3) RPP-RPT-50703 Rev.01A 8/23/2016 - 10:10 AM 3 of 77 RPP-RPT-50703 Rev.1A Development of a Thermodynamic Model for the Hanford Tank Waste Operations Simulator (HTWOS) R Carter Atkins Global, LLC Richland, WA 99354 U.S. Department of Energy Contract DE-AC27-08RV14800 ABSTRACT Complex equilibria exist between the aqueous phase and solid phases in Hanford waste. Because these solutions contain components at high concentration, it is necessary to obtain accurate parameterizations of water activity for retrieval, transfer, and for the vitrification plant at relevant temperatures and concentrations where storage, processing, and treatment are to be performed. This information can be used to predict identity and concentrations of solid hydrates known to exist in Hanford waste at the same time as aqueous species concentrations. The components included in the thermodynamic model described in this report are those constituents considered most important in Hanford Tank waste, i.e. NaNO2, NaNO3, NaOH, NaAl(OH)4, NaF, Na2CO3, Na2SO4, Na2C2O4, Na2HPO4, Na3PO4, and water. The solid phase components considered are: Al(OH)3, Na2C2O4, Na2CO3·H2O, Na2CO3·7H2O, Na2CO3·10H2O, Na2SO4, Na2SO4·10H2O, NaF, NaF·Na2SO4, Na2HPO4·12H2O, NaNO3·Na2SO4·H2O, NaNO2, NaNO3, Na3PO4·¼NaOH·12H2O, NaF·2Na3PO4·19H2O, and NaAlCO3(OH)2. The thermodynamic model described here is the well-known Pitzer ion-interaction model for calculation of ion activity coefficients and water activity (via the osmotic coefficient) in aqueous multicomponent electrolyte systems. The parameters required by the Pitzer model for the components considered here have been obtained from the open literature. To ensure the final model is self-consistent, these parameters were optimized by fitting the model to solubility data of simple mixtures available in the open literature. This optimized model allows predictions of phase speciation to high ionic strengths and temperatures from 0 to 100 °C. The ultimate goal is to include this thermodynamic model into the Hanford Tank Waste Operations Simulator (HTWOS) to replace existing simple wash and leach factors for the species listed above. KEY WORDS Thermodynamics, Pitzer ion-interaction model, water activity, solute activity, molality, ionic strength, solubility, Hanford crystal phases, osmotic coefficient, activity coefficient, HTWOS. RPP-RPT-50703 Rev.01A 8/23/2016 - 10:10 AM 4 of 77 TABLE OF CONTENTS 1 INTRODUCTION ......................................................................................................................... 1 2 THERMODYNAMIC MODEL DESCRIPTION....................................................................... 3 2.1 EXCESS GIBBS FREE ENERGY............................................................................................... 3 2.2 MULTICOMPONENT OSMOTIC COEFFICIENT ...................................................................... 4 2.3 MULTICOMPONENT ACTIVITY COEFFICIENTS ................................................................... 5 2.4 HIGHER ORDER UNSYMMETRICAL MIXING PARAMETERS............................................. 6 2.5 TEMPERATURE DEPENDENCE OF THE PITZER PARAMETERS ........................................ 8 3 GIBBS ENERGY MINIMIZATION ......................................................................................... 10 3.1 GIBBS ENERGY MINIMIZATION SPREADSHEET (GEMS) ................................................. 10 3.1.1 GEM Worksheet......................................................................................................................11 3.1.2 Pitzer Model Worksheet..........................................................................................................12 3.1.3 Gibbs Energy (Felmy) Worksheet...........................................................................................13 3.1.4 Gibbs Energy (Weber) Worksheet ..........................................................................................13 3.1.5 Gibbs Energy (HTWOS) Worksheet.......................................................................................14 3.1.6 Binary Parameters Worksheet .................................................................................................14 3.1.7 Ternary Parameters Worksheet ...............................................................................................14 3.1.8 V & V Worksheet....................................................................................................................15 4 VERIFICATION OF THE INITIAL PITZER MODEL IMPLEMENTATION.................. 16 5 DEVELOPMENT OF THE HTWOS PITZER DATABASE.................................................. 20 5.1 EVALUATION OF SINGLE SOLUTES...................................................................................... 20 5.1.1 NaNO3 .....................................................................................................................................20 5.1.2 NaNO2 .....................................................................................................................................23
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