Used Fuel Disposition Campaign UFD Disposal in Argillite R&D: - - PowerPoint PPT Presentation

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Used Fuel Disposition Campaign UFD Disposal in Argillite R&D: - - PowerPoint PPT Presentation

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Used Fuel Disposition Campaign UFD Disposal in Argillite R&D: Geochemical Modeling Activities of Barrier Material Interactions Carlos F. Jov Coln Sandia National Laboratories Las Vegas, Nevada June 7 9, 2016 SAND2016-5371

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SLIDE 1

Used Fuel Disposition Campaign UFD – Disposal in Argillite R&D: Geochemical Modeling Activities

  • f Barrier Material Interactions

Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-AC04-

  • 94AL85000. SAND2016-nnnnn

Carlos F. Jové Colón Sandia National Laboratories Las Vegas, Nevada – June 7 – 9, 2016 SAND2016-5371 PE

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SLIDE 2

Used Fuel Disposition

Overview UFD EBS: DR Argillite Disposal R&D

 Work Package #: FT-16SN08030207  1D reactive-transport modeling with decay heat effects  Engineered barrier system model integration with performance assessment (PA)  Thermodynamic and sorption assessment of barrier materials  Clay interaction experiments: High temperature mineral phase stability, thermal limits, clay – metal interactions, RN transport  High temperature mechanical (TM) modeling  International Collaborations (e.g., FEBEX-DP, DECOVALEX, SKB TF)

2 DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

Clay-Metal Interactions FEBEX-DP

GDSA PA Level Of Integration

Clay Pent

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SLIDE 3

Used Fuel Disposition

1D Reactive Transport of Layered EBS – Argillite Disposal Media

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016 3

PFLOTRAN 1D Reactive Transport Modeling Argillite Rock

Cement Outer Clay + Quartz Barrier Inner Clay Barrier Metal Canister Waste

 1D reactive transport (RT) PFLOTRAN calculations:

– 24 minerals, 4 initial pore solution chemistries – Efficient model scoping in High Performance Computing (HPC) platforms – Evolution of mineral volume fraction and aqueous speciation with time: equilibrium & kinetics

 Temperature effects case:

– SNF decay heat profile – Peak temperature: 125°C – Capture mineral phase transitions: gypsum  anhydrite + 2 H2O

0.475 m 0.1 m 1.24 m 1.24 m 0.75 m >>10 m (RED Font: Domains Considered)

50 years storage Observation Points

Observation Points

(Work in Progress!)

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SLIDE 4

Used Fuel Disposition

1D Reactive Transport of Layered EBS – Argillite Disposal Media (Cont.)

4

Gypsum fraction decreases during heating Anhydrite stable at T>44°C

Gypsum stable at T<44°C

CaSO4(s) transitions

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

(Work in Progress!)

 1D reactive transport modeling in PFLOTRAN:

– Decay heat effects capture CaSO4(s) phase transitions (T≈44°C) – Porosity changes

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SLIDE 5

Used Fuel Disposition

Thermodynamic Assessments: Solid – Fluid Data Evaluations

 Evaluation of clay and zeolite thermodynamic data at elevated pressures and temperatures  Sensitivity evaluations:

– Clay stability relations – Redox: Fe++-- Fe+++ activities – Silica analcime(Si) stability – Temperature

 Thermodynamic Database Development

– Chemical Thermodynamic Data. I: Links to the chemical elements. Paper revised for resubmission to Geochim. Cosmo. Acta – Chemical Thermodynamic Data. II: Water in SUPCRT92 & similar codes. Paper to be submitted soon!

 Rest of FY16 and FY17:

– Focus on compositional & redox sensitivities on clay stability relations

– e.g., illite, smectite, & Fe

– Chemical Thermodynamic Data. III: revising the Helgeson et al. (1978) mineral dataset – Corrosion reactions and relations to Fe- smectite

5

(Work in Progress!)

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

T฀ ฀ ฀ C log฀

฀

aFe++ a

2฀

H

+฀

50 100 150 200 250 300

  • 30
  • 25
  • 20
  • 15
  • 10
  • 5

illite(IMt-2) illSmc(ISCz1)

Illite(IMt-2) Ill/Smec (SCz-1) Log(aFe++) pH=7 kaolinite Smectite(MX80) Saponite (sapCa-2)

Analcime(Si)

Illite(IMt-2) Log(aSiO2(aq)) pH=7

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SLIDE 6

Used Fuel Disposition

FEBEX-DP (Grimsel URL)

6

  • Shotcrete/bentonite

interface sampling

  • Characterization studies

cement/bentonite interactions

  • Phase identification (SEM-

EDS, XRD)

  • X-ray CT Scan: micron-scale

structures Over-coring Technique

Mäder (2014)

Shotcrete Bent.

CFJC (SNL)

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

FEBEX-DP Sampling Plan

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Used Fuel Disposition

 So far – no indication of strong elemental gradients beyond the interface region  Cracks (desiccation?) tend to be abundant at the interface  Portlandite (Ca(OH)2) mineralization at the interface?  More elemental line-scans needed to resolve compositional gradients

FEBEX-DP: Bentonite – Concrete Interface Characterization (SEM – EDS – BSEI)

7

Back-Scattered Electron Image (BSEI) of Bentonite – Cement Interface

X-ray Map Line Scan: Ca counts

Portlandite Grain?

  • Approx. Interface

Location

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

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SLIDE 8

Used Fuel Disposition

FEBEX-DP: Bentonite – Concrete Interface Characterization (X-ray CT Scan)

8

 X-ray CT Scan:

– Non destructive – Can manage hand-size samples – Scan resolution: 10.5 microns

 Can resolve important features: – Cracks – Large pores  3D image analysis – Continuous pores and cracks – “Heavy” minerals: oxides, sulfides Bentonite Cracks Cement

1.66 mm Imaging by J. Eric Bower (SNL)

Interface Core Specimen

Cement Bentonite

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

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SLIDE 9

Used Fuel Disposition

FEBEX-DP: Sampling Close to Heater

9

Sampling Locations Bentonite Block (Close to Heater) Carbon Steel Liner (Surrounding Heater)

Heater

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

FEBEX-DP Sampling Plan

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Used Fuel Disposition

FY17 Outlook

 1D reactive-transport (RT) modeling of EBS in PFLOTRAN

– Leveraging High Performance Computing (HPC) – Decay heat effects – assess code stability at T>125°C – Applications to disposal in argillite/crystalline media – Implementation of metal corrosion model conceptualizations (Fe, Cu) – Capture temperature effects: dehydration, phase transformations (gypsum  anhydrite)

 Integration of process models with GDSA PA  Evaluation of clay phase stability at elevated temperatures

– Redox effects on Fe-bearing clay stability and related phases – Comparison with other studies on smectite alteration in the presence of Fe

 Thermodynamic data analysis and applications to geochemical modeling

– Paper/Report: “Chemical Thermodynamic Data. II”: Water in SUPCRT92 and similar computer codes (mentored by Tom Wolery (LLNL)) – Submittal in 2016 – Work on “Chemical Thermodynamic Data. III”: Revising the Helgeson et al. (1968) mineral dataset

 International Collaborations

– Continue SKB TF, FEBEX-DP, – DECOVALEX: Groundwater Recovery experiment (GREET) at Mizunami URL, Japan

10 DOE UFD WG Meeting, Las Vegas, NV June 9-11, 2015

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SLIDE 11

Used Fuel Disposition

ACKNOWLEDGMENTS

 Dr. Michael C. Cheshire (currently at ORNL) conducted the experimental and characterization work on clay steel-interactions presented here.  Discussions with Charles R. Bryan (SNL) on steel corrosion are greatly appreciated.  This work supported by the DOE-NE Used Fuel Disposition Campaign Fuel Cycle Technologies R&D program.

Date Presentation or Meeting Title 11

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SLIDE 12

Used Fuel Disposition

Backup Slides

12 DOE UFD WG Meeting, Las Vegas, NV June 9-11, 2015

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SLIDE 13

Used Fuel Disposition

Overview UFD EBS: DR Argillite Disposal R&D

 Work Package #: FT-16SN08030207  Engineered barrier system model integration with performance assessment  Thermodynamic and sorption modeling of barrier materials  Clay interaction experiments: U transport, mineral phase stability and thermal limits  High temperature mechanical (TM) modeling  International Collaborations (e.g., THM, FEBEX-DP, SKB TF)

13 DOE UFD WG Meeting, Las Vegas, NV June 9-11, 2015

Clay-Metal Interactions SKB TF

GDSA PA Level Of Integration

Clay Pent

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SLIDE 14

Used Fuel Disposition

14

Reactive-Transport Modeling

  • f the Near- and Field with PFLOTRAN

 Reactive-transport simulations

  • f base-case scenarios on the

near- and far-field domains  1D or 2D scoping model representation for a single canister  Coupled processes (THC):

– Solute transport – Fluid-rock-canister interactions (solution-mineral equilibria, dissolution/ precipitation, sorption) – Heat load according to waste type – Variable backfill saturation(?)

 Evaluate U transport from wasteform source to the EBS / host-rock interface  Evaluate changes in mineral volume fractions and porosity

Rock Canister Rock Backfill Backfill EDZ EDZ

DOE UFD WG Meeting, Las Vegas, NV June 9-11, 2015

RN Transport

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SLIDE 15

Used Fuel Disposition

Clay Hydration Modeling and Micro-Porosity Evolution

 Relationships between swelling clay micro-porosity and clay hydration (Sedighi and Thomas 2014)  Thermodynamic relations based on H2O adsorption by swelling clays  Connections with clay water content and relative humidity (RH): Data retrieval from URL and laboratory experiments  Comparisons between theoretical models and field/lab data:

– Predicted trends are in agreement with data – Data scattering can be significant

 Rest of FY15 and FY16:

– Calibrate hydration model to montmorillonite clay compositions – Continue analysis of data generated by international programs (e.g., SKB Task Force

  • n EBS)

– If possible, comparison with parameters used in THM models

15 DOE UFD WG Meeting, Las Vegas, NV June 9-11, 2015

  • Thermodynamic-based

model calibrated by H2O adsorption data

  • Micro-porosity model

calibrated by water content and RH data

  • Effect of clay chemistry on

hydration / swelling

Thermodynamic-Based Model Micro-Porosity Model

(Work in Progress!)

Sedighi and Thomas (2014)

sm c il micro hs dry sm

n n X Fw υ ρ =

Clay micro-porosity = water content Mole fraction of hydrated smectit Formula weight of anhydrous smectite Number of H2Os in the interlayer Molar volume of H2O (interlayer)

il micro wc hs sm c il

n X Fw n θ υ = = = = = = Clay dry density

sm dry

ρ =

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SLIDE 16

Used Fuel Disposition

Thermodynamic Assessments: Solid – Fluid Data Evaluations

 Evaluation of clay and zeolite thermodynamic data at elevated pressures and temperatures  Sensitivity evaluations:

– Clay stability relations – Redox: Fe++-- Fe+++ activities – Silica analcime(Si) stability – Temperature

 Thermodynamic Database Development

– Chemical Thermodynamic Data. I: Links to the chemical elements. Paper revised for resubmission to Geochim. Cosmo. Acta – Chemical Thermodynamic Data. II: Water in SUPCRT92 & similar codes. Paper to be submitted soon!

 Rest of FY16 and FY17:

– Focus on compositional & redox sensitivities on clay stability – Chemical Thermodynamic Data. III: revising the Helgeson et al. (1978) mineral dataset

16

(Work in Progress!)

DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016 Topological relations with respect to Fe are still under evaluation

Illite(IMt-2) Saponite (sapCa-2)

Ill/Smec

T฀ ฀ ฀ C log฀

฀

aFe++ a

2฀

H

+฀

50 100 150 200 250 300

  • 30
  • 25
  • 20
  • 15
  • 10
  • 5

illite(IMt-2) illSmc(ISCz1)

Illite(IMt-2) Ill/Smec (SCz-1) Analcime(Si) Smectite(MX80) Log(aFe++/a2H+) Log(aSiO2(aq))

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SLIDE 17

Used Fuel Disposition

1D Reactive Transport of Layered EBS – Argillite Disposal Media (Cont.)

17 DOE UFD WG Meeting, Las Vegas, NV June 7-9, 2016

 1D reactive transport modeling in PFLOTRAN:

– Changes in pore solution chemistry: FEBEX bentonite porewaters – pH effects during peak heating at EBS interfaces