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Modelling of concrete/clay interaction : taking into account complex mineralogy influence of non-saturated conditions and temperature effects F. Claret, A. Burnol, S. Gaboreau, N. Marty, C.Tournassat, P.Blanc, EC. Gaucher BRGM, Orlans With

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2nd International Workshop: Mechanisms and modelling of waste/cement interactions, Le Croisic, October 12-16,2008

Modelling of concrete/clay interaction :

taking into account complex mineralogy influence of non-saturated conditions and temperature effects

  • F. Claret, A. Burnol, S. Gaboreau, N. Marty,

C.Tournassat, P.Blanc, EC. Gaucher BRGM, Orléans With the partnership of: Andra: X. Bourbon, S. Dewonck, I. Munier, N. Michau

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CONTEXT: COX/CONCRETE/BENTONITE INTERACTION

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MODELLING AS A TOOL

> To size a future underground experiment in the

Bure’s Laboratory

  • MLH experiment (see S.DEWONCK’s poster)
  • pH evolution of an alkaline solution in contact with the COX

> To make some predictive calculations

  • Long term modelling of concrete/clay interactions for PA purposes

6.5 7 7.5 8 8.5 9 9.5 10 10.5 11 11.5 12 12.5 13 13.5 0.25 0.5 0.75 1 1.25 1.5 1.75 2 2.25 2.5 2.75 3 3.25 3.5 3.75 4 4.25 4.5 4.75 5 5.25 5.5 5.75 6 Temps (années) pH 1L 3L 5L 10L 15L

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CRITICAL ELEMENTS FOR THE MODELLING

> A coherent thermodynamic database to work in

temperature

> A “complete” mineralogical description of the

initial system

> Transport parameters (porosities, permeabilities,

diffusion coefficients, heat conductivities…)

> A Transport reactive code

  • PHREEQC (1D)
  • TOUGHREACT (radial geometry, non saturated condition,

….)

> Experiments to test and improve the modelling > ….

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CRITICAL ELEMENTS FOR THE MODELLING

> A coherent thermodynamic database to work in

temperature

> A “complete” mineralogical description of the

initial system

> Transport parameters (porosities, permeabilities,

diffusion coefficients, heat conductivities…)

> A Transport reactive code

  • PHREEQC (1D)
  • TOUGHREACT (radial geometry, non saturated condition,

….)

> Experiments to test and improve the modelling > ….

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http://thermoddem.brgm.fr/

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AMORPHOUS CSH

> Among the various models published that

take into account the solubility of CSH, two main families may be distinguished:

  • Discrete phases
  • Solid solutions

> Nowdays integration of solid solutions in

transport geochemical codes lead to crippling computing times

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COMPOSITION OF AMORPHOUS CSH PHASES (1/4)

> According to the literature and given the

crystallographic constraints a 3-phases model was chosen

> Such model already exist (CSH0.8/1.1/1.8)

  • Stronach and Glasser (1997) Adv. Cem. Res. Vol. 36 pp.167
  • A.C. Courault (2000) Thesis Université de Bourgogne

> Strategy used : fitting of the literatures data

with a least squares algorithm

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COMPOSITION OF AMORPHOUS CSH PHASES (2/4)

0.0 0.5 1.0 1.5 2.0 2.5 5 10 15 20 Dissolved Ca (in mmol/l) Ca/Si in solid 2 Courault [15] Grutzeck et al. [49] Fuji and Kondo [55] Greenberg and Chang [48] Kalousek [56] Taylor [51] Roller and Erwin [54] Flint and Wells [47]

Dispersion in the values can be link to : The synthesis route followed The pathway followed to reach equilibrium (by dissolution or precipitation) The assessment of the C/S ratio in the solid A solid/liquid equilibrium not reached due to kinetic constraints

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COMPOSITION OF AMORPHOUS CSH PHASES (3/4)

0.0 0.5 1.0 1.5 2.0 2.5 5 10 15 20 Dissolved Ca (in mmol/l) Ca/Si in solid 2 Courault [15] Grutzeck et al. [49] Fuji and Kondo [55] Greenberg and Chang [48] Kalousek [56] Taylor [51] Roller and Erwin [54] Flint and Wells [47]

C/S = 1.6 ± 0.1 C/S = 1.2 ± 0.18 C/S = 0.8 ± 0.16

Blanc, P. et al. accepted. Chemical conceptual model for cement-based materials: Thermodynamic data assessment of stoichiometric and non- stoichiometric CSH phases. J.Hazardous.Materials

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COMPOSITION OF AMORPHOUS CSH PHASES (3/4)

0.0 0.5 1.0 1.5 2.0 2.5 5 10 15 20 Dissolved Ca (in mmol/l) Ca/Si in solid 2 Courault [15] Grutzeck et al. [49] Fuji and Kondo [55] Greenberg and Chang [48] Kalousek [56] Taylor [51] Roller and Erwin [54] Flint and Wells [47]

C/S = 1.6 0.1 C/S = 1.2 0.18 C/S = 0.8 0.16 C/S = 1.8 C/S = 1.1 C/S = 0.8

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> 12 0.001 0.01 0.1 1 10 5 10 15 20 25 Dissolved Ca (mmol/l) Dissolved Si (mmol/l) Flint and Wells [47] Roller et Ervin, 1940 Taylor [51] Kalousek [56] Greenberg and Chang [48] Fuji and Kondo [55] Courault [15] Grutzeck et al. [49] CSH1.6/CSH0.8 solid solution CSH0.8 CSH1.2 CSH1.6

COMPOSITION OF AMORPHOUS CSH PHASES (4/4)

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log a Ca++/H+.2.0 T (° C)

blanc Fri Jun 15 2007

Log(aCa++)-2log(aH+) Temperature (° C) Portlandite Gyrolite Tobermorite-11A Foshagite Tobermorite-14A Xonotlite Hillebrandite Quartz

CRYSTALLINE CSH PHASES (1/2)

Diagram calculated using the estimates of Babushkin et al. (EQ3.6)

Temperature transition to low Authors see this phase at least up to 200° C Foshagite considered as high temperature phase Absence of okenite, afwillite and jennite Temperature (ºC) Log(aCa++) – 2 log(aH+)

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CRYSTALLINE CSH PHASES (2/2)

10 12 14 16 18 20 22 24 50 100 150 200

log a Ca++/H+.2.0 T (° C)

Afwillite Gyrolite Hillebrandite Jennite Quartz,alpha Tobermorite_11A Tobermorite_14A Xonotlite

blanc Thu Jun 28 2007

Log(aCa++)-2log(aH+) Temperature (° C) Portlandite Gyrolite Tobermorite-11A Afwillite Tobermorite-14A Xonotlite Hillebrandite Quartz Jennite

Hypotheses : Use of triple point (Gibbs phases rule) H of Tobermorite 11A° , Xonotlite, Foshagite and Hillebrantite are fixed The Cp of Babushkin were used

Blanc, P. et al. accepted. J.Hazardous.Materials Temperature (ºC) Log(aCa++) – 2 log(aH+)

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CRITICAL ELEMENTS FOR THE MODELLING

> A coherent thermodynamic database to work in

temperature

> A “complete” mineralogical description of the

initial system

> Transport parameters (porosities, permeabilities,

diffusion coefficients, heat conductivities…)

> A Transport reactive code

  • PHREEQC (1D)
  • TOUGHREACT (radial geometry, non saturated condition,

….)

> Experiments to test and improve the modelling > ….

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STARTING MINERALOGICAL CONDITIONS (CONCRETE)

Pore water composition after resaturation with COX pore water Amorphous hypothesis @ 25ºC (1) Cristalline hypothesis @ 25ºC (2) Hyp1 Hyp2

CEM I + calcite aggregate

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STARTING MINERALOGICAL CONDITIONS (COX)

Fe Si Sr K Mg Ca Na Cl S(6) TIC 0.001 0.01 0.1 1 10 100

Concentrations (mmol/L)

  • PAC experiment

Gaucher et al. Submitted to GCA

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STARTING MINERALOGICAL CONDITIONS (MX80 bentonite)

70% MX80 + 30% Sand

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CRITICAL ELEMENTS FOR THE MODELLING

> A coherent thermodynamic database to work in

temperature

> A “complete” mineralogical description of the

initial system

> Transport parameters (porosities, permeabilities,

diffusion coefficients, heat conductivities…)

> A Transport reactive code

  • PHREEQC (1D)
  • TOUGHREACT (radial geometry, non saturated condition,

….)

> Experiments to test and improve the modelling > ….

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TRANSPORT PARAMETERS

The release of the MCD option in PHREEQC permits to treat multi-porosity cases However, MCD option still under improvement : => use of Mix Cells instead

  • cf. Appelo et al. (2008) Journal of Contaminant Hydrology Vol 101 pp 67

1D cartesian saturated conditions: PHREEQC 1D radial non-saturated conditions: TOUGHREACT

T T

T D D η η298

298 , ,

. 298 . =

exp

) 109 ) 20 .( 10 . 36 . 8 ) 20 .( 37023 . 1 *( 10 ln

2 4

tc tc tc T + − + − −

−

= η

Ratio 2.54 between 70° C and 25° C

Effective Poral

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INFLUENCE OF MESH SIZE (at local equilibrium)

y = 4106x2.01 R2 = 1

Diffusion controlled : x2 = Dt 2logx =logD + log t

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2nd International Workshop: Mechanisms and modelling of waste/cement interactions, Le Croisic, October 12-16,2008

Diffusion-contolled regime Kinetic-controlled regime 0.001 0.01 0.1 1 1 10 100 1000 10000 100000 1000000

Space step size (m) Time necessary for porosity clogging (years) Local equilibirum Kinetic

Slope: 1.84

INFLUENCE OF MESH SIZE See N. Marty’s Poster Marty et al. Journal of Hydrology. In press To determined the good mesh : size confrontation between experiments and calculations are needed

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CRITICAL ELEMENTS FOR THE MODELLING

> A coherent thermodynamic database to work in

temperature

> A “complete” mineralogical description of the

initial system

> Transport parameters (porosities, permeabilities,

diffusion coefficients, heat conductivities…)

> Transport reactive calculation

  • PHREEQC (1D)
  • TOUGHREACT (radial geometry, non saturated condition,

….)

> Experiments to test and improve the modelling > ….

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2nd International Workshop: Mechanisms and modelling of waste/cement interactions, Le Croisic, October 12-16,2008

Concrete with crystalline CSH MX80

6 m 6 m De 9.10-12 m2s-1 De 1.10-11 m2s-1

  • 1. Calculations made at thermodynamic equilibrium
  • 2. No retroaction on porosity

pH 12.5 @ 25 ºC pH 8.2 @ 25 ºC

t=0

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Time for porosity clogging = 2700 years

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« Young » concrete pH13.2 Time for porosity clogging 3500 ans

Illitization

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Clogging time ratio 2.6 Clogging time ratio 1.7

70 ºC 25 ºC

TEMPERATURE INFLUENCE ON CLOGGING

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Hydrogrenat_Al Jennite Hydrogrenat_Fe Smectite Quartz Dolomite Microcline Albite

Diffusion

Portlandite

Concrete with crystalline phases MX80 Dissolution sequence of primary phases Altered zone: less than 50 cm at the clogging time

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Diffusion

Concrete with crystalline phases MX80 Altered zone: less than 50 cm at the clogging time

Calcite Chabazite Phillipsite Saponite Illite Tobermorite Ettringite Chlorite Analcime

Precipitation sequence of secondary phases

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CRITICAL ELEMENTS FOR THE MODELLING

> A coherent thermodynamic database to work in

temperature

> A “complete” mineralogical description of the

initial system

> Transport parameters (porosities, permeabilities,

diffusion coefficients, heat conductivities…)

> Transport reactive calculation

  • PHREEQC (1D)
  • TOUGHREACT (radial geometry, non saturated condition,

….)

> Experiments to test and improve the modelling > ….

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TOWARD A MORE REALISTIC GEOMETRY

Primary package: Diameter = 0.44m Height = 1.45m Disposal package: 1.5x1.5x2 (hexahedral) Disposal Chamber: Height = 6.3m, Width = 5.4m 36 Primary package in the disposal chamber

Hypothesis of volume conservation

Space :

  • Saturated case : concrete porewater
  • Non Saturated case : air
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CAPILLARY PRESSURE FONCTION

NON SATURATED CONDITIONS

0.3 0.4 0.5 0.6 0.7 0.8 0.9 1x105 1x106 1x107 1x108 1x109 1x1010

Liquid saturation Capillary pressure (Pa) Calculated with COX parameters Calcuted with concrete parameters

λ λ − −

− − =

1 1 *

) 1 ] ([S P P

cap lr ls lr l

S S S S S − − =

*

Van Genuchten function

λ λ λ λconcrete and λ λ λ λclay slightly different λ λ λ λconcrete ~0.35 and λ λ λ λclay ~0.33 P0 concrete 2MPa P0 clay 15MPa

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RELATIVE PERMEABILITY FUNCTION

[ ]

2 1 *

1 1 .

*

  • −

− =

λ λ

S S krl

lr gr lr l e

S S S S S − − − = 1

( )

λ λ 2 / 1

1 . 1

S e

e rg

S k − − =

Water : van Genuchten Gas : Parker

0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1 Saturation liquide (eau) Perméabilité relative Krl (van Genuchten) Krg (Parker) Krg (=1-Krl) Krg (Corey)

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TRANSPORT PARAMETERS

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RESATURATION TIME

  • Initial
  • 0.1 y
  • 100 y
  • 500 y
  • 1000 y

Initial COX desaturation

Concrete container COX air/water Concrete

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SATURATED CONDITIONS

  • Sat. Cas.
  • Starting

. 1500 y

air/water Concrete container Concrete COX

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NON SATURATED CONDITIONS

  • Non. Sat. Cas.
  • Starting

. 1500 y

M RT d PN RT D

m a gaz

Π Π = 8 2 3

2

With Dgaz = diffusion coefficient (m2/s) R = universal gaz constant (8,31451 m2kgs-2mol-1K-1) T = temperature in Kelvin P = pressure (kgm-1s-2) Na = Avogadro number (6,0221367.1023 molecules/mol) Dm = molecular diameter (m) M = molar mass (kg/mol)

air/water Concrete container Concrete COX

Carbonation due to CO2 gas diffusion

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CRITICAL ELEMENTS FOR THE MODELLING

> A coherent thermodynamic database to work in

temperature

> A “complete” mineralogical description of the

initial system

> Transport parameters (porosities, permeabilities,

diffusion coefficients, heat conductivities…)

> Transport reactive calculation

  • PHREEQC (1D)
  • TOUGHREACT (radial geometry, non saturated condition,

thermal gradient….)

> Experiments to test and improve the modelling > ….

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TRANSIENT THERMAL STATE

Input ToughReact

270 W after 20 years

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TEMPERATURE EVOLUTION

T(ºC) max. Waste

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CONCLUSIONS

> Alteration of concrete/clay: limited in space

(~50cm) with saturated conditions and clogging

> Clogging porosity is mesh size dependent at

local equilibrium

> Transient states (non-saturated period,

thermal period) : ~ 2000 years

> Carbonation: increased by CO2(g) diffusion

in non-saturated conditions

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OUTLOOK

> Fully coupled reactive transport considering

complex mineralogy and complex geometry with both non-saturated and non-isothermal conditions

> Simulation of fractures of EDZ (due to excavation)

by “Multiple INteracting Continua” (MINC function of TOUGH2)

> Kinetics instead of local equilibrium > Archie law: retroaction of chemical reactions on

effective diffusion coefficient

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ACKNOWLEDGMENT

MLH : S. Dewonck, Y. Linard UPS : I. Munier, N. Michaud, B. Cochepin GL ESC : X. Bourbon

  • A. Dauzeres P. Le Bescop

Lawrence Berkeley Lab. :N. Spycher, T. Xu

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