advances in modelling salt stock deposition of nuclear wastes · fdm fvm fct i/o cprocess::create()...
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Advances in Modelling Salt Stock Deposition of Nuclear Wastes
Mingliang Xie and Helge C. Moog
GRS, Braunschweig, Germany
10th Annual GTT-Technologies Workshop
Herzogenrath, GermanyJune 4-6, 2008
Content
� Introduction
� Reactive Transport Modelling
� Reactions and Database
� Application – UO2(s) dissolutionand transport
� Outlook
Content
� Introduction
� Reactive Transport Modelling
� Reactions and Database
� Application – UO2(s) dissolutionand transport
� Outlook
Overburden
Biosphere
Host rock
?
?
?
Waste
Backfill
Solution
Aquifer
?
Of course, a real underground structure of a disposal site is
much more complex…This is just ONE base of an underground disposal site
� Red = BarriersGreen = solid saltBlue = crushed saltBlack = Disposal cavernGrey = Excavation-disturbed zone
� Up to 15 bases possible
Core
Bentonite Buffer
Fractured Rock
Shrinking
Heat Transport
Vaporisation
Condensation
WaterIntrusion
Contact
Mechanics
Mass TransportChemical Reactions
CoupledCoupled ProcessesProcesses in Geotech Systemsin Geotech Systems
ConceptConcept of of CoupledCoupled ProcessesProcesses
C T
MH
Temperature change →→→→Water/air storageWater/vapor/air/dissolved air transfer
Porosity Change →→→→Water/air storageWater/vapor/ions/air/ dissolved air transfer
Suction →→→→Stress/strain field
Ion exchange →→→→Stress/strain field
Temperature →→→→Stress/strain field
Chemical reaction →→→→Heat release/absorb
Porosity Change →→→→Heat conductionHeat storage
Temperature →→→→Chemical ReactionIon transport
Chemical Process →→→→Water/air/dissolved airtransfer
Water/air transfer →→→→Chemical reactionIon transfer
Disposal chamber for waste
Waste
Backfill
Solution
??
?
??
?
??
Thermodynamic Modelling
That is, what a safe disposal site looks like!
Many caverns form one system…
Interaction Waste - Solution
Equilibrium
∏∏ ⋅==j
jjj
jjjj maK
νννγ
Phasecomposition:
( )( )iiif
i
isolution
iPhases
ifisolids
mTGnG
GnG
γlnlnR,
,
++=
⋅=
⊗
⊗
∑
∑
Phase 1
Mm+
Nn+
Xx+
Yy+Thermody-
namic
equilibrium
Phase 2 Phase 3 Phase n
Aq. solutionWaste
Su
ffic
ien
tti
me
∑ ∑∑++=j j k
kjkjijjii mmmIDH ,,, )(ln µλγ
+ -
+ +
+ -
-
+ -
+
SIT -Single Ion Interaction Theory
Pitzer-Modell
� Approaches considering specific ionic iteractions …
Modells for the calculation of activity coefficients
� Debye-Hückel (1923): purely electrostatic interactions
� Extensions to the DH-equation…
Porosity/Permeability change
� Material microstructure � Dissolution/precipitation (C)
� Deformation (M,T)
� Swelling (bentonite)
� Permeability k=k(n)
PorosityPorosity –– permeabilitypermeability relationshiprelationship
(Clauser 2003)
Geochemical Geochemical processesprocesses
(Sonnenthal et al 2005)
Content
� Introduction
� Reactive Transport Modelling
� Reactions and Database
� Application – UO2(s) dissolutionand transport
� Outlook
GoverningGoverning EquationsEquations
n x conservative TransportChemical reactions with
PHREEQC, ChemApp or GEMS-PSI
i=1, 2,...,n
Saturated
GoverningGoverning EquationsEquations
(Suarez & Simunek, 1996)
Unsaturated
Geochemical simulators
GeoSys/RockFlow
CHEMAPP
PHREEQC
GEMS-PSI
RockFLow/GeoSys+ChemAppRockFLow/GeoSys+ChemApp
Old time step
New time step
Transport
Reaction
i=1, 2,...,n
ChemApp
Object-Orientation:Multifield Problems
PCS
MSH
GEO
GeometryPointsPolylinesSurfacesVolumesDomains
TopologyNOD NodesELE Meshes
IC BC ST
MATMFPMSPMMPMCP
NUM
FEMFDMFVM
FCT
I/O
CProcess::Create()CProcess::Config()CProcess::Execute()
EQS
Kolditz & Bauer (2004)J Hydroinformatics
2-D Ele men ts
3-D El eme nt s
1-D Ele men ts
T etrahedr a
Hex ahedraPri sm s
Tr iangles
Quadri lat erals
2-D Elements
3-D Elements
1-D Elements
Tetrahedra
Hexahedra
Prisms
Triangles
Quadrilaterals
Geometric Element Types
C6
C5
C4
C3
C2
C1
RnAn...B4nB1n
.....................
R4B4n...A4B24
R3...A3.B13
R2...B24.A2B12
R1B1n...B13B12A1
=
Dimension: (number of grid nodes * number of components)²
For real world applications: (105 * 20)² = 4*1012
Memory requirement: 4*1012
*
Multi-Componental Systems
PCS1
PCS2
EQS1
EQS2
IC1
ICPCS
ic_name:
PRESSURE1
NOD
ICList
BC .....
.....
.....BC1
BC2
bc_name:
PRESSURE1
bc_name:
PRESSURE1
BCList
TIM
MAT2MAT MAT3solid_property
solid_group1
: soil_property
soil_group1
:fluid_property
fluid_phase1
:
MATListMAT1
KER
FM ker_name:
FLOW1
KERList
OBJ2
OBJ
OBJ3
OBJ5
OBJList
OBJ1
OBJ4
ELE
PCSList
pcs_name:
FLOW1
pcs_primary_function:
PRESSURE1
pcs_name:
MASS_TRANSPORT1
pcs_primary_function:
CONC1
PCSExecute
Process()
PCSCreateProcess() PCSConfigProcess()
ker_name:
MASS_TRANSPORT
MTM IC2 ic_name:
CONC1
BC3 bc_name:
CONC1
PCSExecute
Process()
PCS Implementation
High Performance ComputingParallel Computing
Visualization
ParallelizationParallelization
In cooperation with HLRS Stuttgart
Verification example: Comparison with 1D PHREEQC
1D Transport and Cation exchange (Example 11, PHREEQC – User Instructions)
Flushing a 1D column with CaCl2.
Initial pore water: Na, K
Exchange: Ca-X2, Na-X, K-X
Ca = 6.0x10
Cl = 1.2x10
- 4
- 3
1 m/d
D = 0.002 m, n = 1.0, t=0.24 d C in mol/l
0.08 m
Cout
Ca = 0Cl = 0K = 2.0x10Na = 1.0x10
-4
-3
Ca-X2 = 0Na-X = 5.493x10K-X = 5.507x10
-4
-4
Verification Benchmark
Pore Volumes [-]
Co
nce
ntr
atio
n[m
ol/
l]
1 2 30.0E+00
1.0E-04
2.0E-04
3.0E-04
4.0E-04
5.0E-04
6.0E-04
7.0E-04
8.0E-04
9.0E-04
1.0E-03
1.1E-03
1.2E-03
Ca (RF) mol/lCl (RF) mol/lK (RF) mol/lNa (RF) mol/l
Verification Benchmark
Pore Volumes [-]
Concentr
ation
[mol/l]
1 2 30.0E+00
1.0E-04
2.0E-04
3.0E-04
4.0E-04
5.0E-04
6.0E-04
7.0E-04
8.0E-04
9.0E-04
1.0E-03
1.1E-03
1.2E-03
Ca (RF) mol/l
Cl (RF) mol/lK (RF) mol/lNa (RF) mol/l
Verification Benchmark
Pore Volumes [-]
Co
nce
ntr
atio
n[m
ol/
l]
1 2 30.0E+00
1.0E-04
2.0E-04
3.0E-04
4.0E-04
5.0E-04
6.0E-04
7.0E-04
8.0E-04
9.0E-04
1.0E-03
1.1E-03
1.2E-03
Ca (RF) mol/lCl (RF) mol/lK (RF) mol/lNa (RF) mol/l
Verification Benchmark
Pore Volumes [-]
Co
nce
ntr
atio
n[m
ol/
l]
1 2 30.0E+00
1.0E-04
2.0E-04
3.0E-04
4.0E-04
5.0E-04
6.0E-04
7.0E-04
8.0E-04
9.0E-04
1.0E-03
1.1E-03
1.2E-03
Ca (RF) mol/lCl (RF) mol/lK (RF) mol/lNa (RF) mol/l
Verification Benchmark
Pore Volumes [-]
Co
nce
ntr
atio
n[m
ol/
l]
1 2 30.0E+00
1.0E-04
2.0E-04
3.0E-04
4.0E-04
5.0E-04
6.0E-04
7.0E-04
8.0E-04
9.0E-04
1.0E-03
1.1E-03
1.2E-03
Ca (RF) mol/lCl (RF) mol/lK (RF) mol/lNa (RF) mol/l
Verification Benchmark
Pore Volumes [-]
Concentr
ation
[mol/l]
1 2 30.0E+00
1.0E-04
2.0E-04
3.0E-04
4.0E-04
5.0E-04
6.0E-04
7.0E-04
8.0E-04
9.0E-04
1.0E-03
1.1E-03
1.2E-03
Ca (RF) mol/l
Cl (RF) mol/lK (RF) mol/lNa (RF) mol/l
Verification Benchmark
PV
Co
nce
ntr
atio
n[m
ol/l]
1 2 30.0E+00
1.0E-04
2.0E-04
3.0E-04
4.0E-04
5.0E-04
6.0E-04
7.0E-04
8.0E-04
9.0E-04
1.0E-03
1.1E-03
1.2E-03
Na (PHREEQC) mol/lCl (PHREEQC) mol/l
K (PHREEQC) mol/lCa (PHREEQC) mol/lNa (RF) mol/lCl (RF) mol/lK (RF) mol/lCa (RF) mol/l
Verification Benchmark
0
0.0001
0.0002
0.0003
0.0004
0.0005
0.0006
0.0007
0.0008
0.0009
0.001
0.0011
0.0012
0.0013
0 0.5 1 1.5 2 2.5 3
Pore Volume [-]
Co
ncen
trati
on
[m
ol/
l]
Ca (GeoSys)
Cl (GeoSys)
K (GeoSys)
Na (GeoSys)
Na (PHREEQC)
Cl (PHREEQC)
K (PHREEQC)
Ca (PHREEQC)
analytical solution
Concentrations at the column outlet
Cl
Na
K
Ca
analytical solution
Verification Benchmark
Content
� Introduction
� Reactive Transport Modelling
� Reactions and Database
� Application – UO2(s) dissolutionand transport
� Outlook
Cause of Database DifferenceCause of Database Difference
Example: Thermal Conductivity λλλλ of Liquid Toluene at 25oC
publication year (DDBST, 2006)
1D Benchmark
0.0002M calcite0.001M MgCl2
Verification Example
1D Transport and calcite dissolution
Simulated Program
-- MST1D (by Engesgaard and Kipp 1992)
-- PHT3D (by Prommer 2002)
-- GeoSys/PHREEQC (by Xie et al 2005)
0.0 0.5m
Simulation results comparison
D istance (m )
Cl(m
ol/kg
wa
ter)
0 0.1 0 .2 0 .3 0.4 0.50 .0E+00
2.0E-04
4.0E-04
6.0E-04
8.0E-04
1.0E-03
1.2E-03
1.4E-03
1.6E-03
1.8E-03
2.0E-03
C l (G eoS ys/C hem App)C l (G eoS ys/P H R E E Q C )
C l (P H T 3 D )
D istance (m )
pH
0 0.1 0.2 0.3 0.4 0.56.0E+00
6.5E+00
7.0E+00
7.5E+00
8.0E+00
8.5E+00
9.0E+00
9.5E+00
1.0E+01
1.0E+01
1.1E+01
pH (G eoS ys/C hem App)pH (G eoS ys/P H R E E Q C )pH (P H T3 D )
D istance (m )
Mg
(mo
l/kg
wa
ter)
0 0.1 0.2 0.3 0.4 0.50.0E+00
2.0E-04
4.0E-04
6.0E-04
8.0E-04
1.0E-03
1.2E-03
1.4E-03
M g (G eoS ys/C hem App)M g (G eoS ys/P H R E E Q C )M g (P H T3 D )
D istance (m )
Ca
(mo
l/kg
wa
ter)
0 0.1 0.2 0.3 0.4 0.50.0E+00
2.0E-04
4.0E-04
C a (G eoS ys/C hem App)
C a (G eoS ys/P H R E E Q C )C a (P H T3 D )
Simulation results comparison
Distance (m)
Ca
lcite
(mo
l/kg
so
il)
0 0.1 0.2 0.3 0.4 0.50.0E+00
5.0E-06
1.0E-05
1.5E-05
2.0E-05
2.5E-05
3.0E-05 Calcite (GeoSys/ChemApp)
Calcite (GeoSys/PHREEQC)Calcite (PHT3D)
Distance (m)
Do
lom
ite
(mo
l/kg
so
il)
0 0.1 0.2 0.3 0.4 0.50.0E+00
5.0E-06
1.0E-05
1.5E-05
2.0E-05
Dolomite (GeoSys/ChemApp)Dolomite (GeoSys/PHREEQC)
Dolomite (PHT3D)
Database Database sensitivitysensitivity analysisanalysis
Database Database sensitivitysensitivity analysisanalysis
X
Ion
icco
nce
ntr
atio
n(m
ol/kg
H2O
)
0 0.1 0.2 0.3 0.4 0.5-5.0E-04
0.0E+00
5.0E-04
1.0E-03
1.5E-03
2.0E-03
2.5E-03
Cl (YMF)Cl (NAPSI)
Ca (YMF)Ca (NAPSI)Mg (YMF)Mg (NAPSI)
Database Database sensitivitysensitivity analysisanalysis
Database Database sensitivitysensitivity analysisanalysis
Distance (m)
Min
era
lco
nce
ntr
atio
n(m
ol/kg
so
il)
0 0.1 0.2 0.3 0.4 0.50.0E+00
5.0E-06
1.0E-05
1.5E-05
2.0E-05
2.5E-05
3.0E-05Calcite (YMF)Calcite (NAPSI)Dolomite(ord) (YMF)Dolomite(ord) (NAPSI)
Content
� Introduction
� Reactive Transport Modelling
� Reactions and Database
� Application – UO2(s) dissolutionand transport
� Outlook
1D Benchmark
0.001M NaCl
Application Example
1D Transport and UO2(s) dissolution
Simulated Program
-- GeoSys/Rockflow+ChemApp (by Xie et al 2005)
0.0 0.5m0.01M UO2(s)
0.2 0.3m
Inert porous media
UO2(s) UO2(s) dissolutiondissolution and and transporttransport
Distance (m)
Dis
so
lve
dU
(M)
UO
2(s
)(m
ol/kg
so
il)
0.1 0.2 0.3 0.4 0.50
0.005
0.01
0.015
0.02
0.025
0.03
0
0.002
0.004
0.006
0.008UO2(s)
dissolved U
Initial
UO2(s) UO2(s) dissolutiondissolution and and transporttransport
Distance (m)
Dis
so
lve
dU
(M)
UO
2(s
)(m
ol/kg
so
il)
0.1 0.2 0.3 0.4 0.50
0.005
0.01
0.015
0.02
0.025
0.03
0
0.002
0.004
0.006
0.008UO2(s)
dissolved U
Xp
H,E
h0.1 0.2 0.3 0.4 0.5
0
1
2
3
4
5
6
7
8
9
pH
Eh
310 sec
UO2(s) UO2(s) dissolutiondissolution and and transporttransport
Distance (m)
Dis
so
lve
dU
(M)
UO
2(s
)(m
ol/kg
so
il)
0.1 0.2 0.3 0.4 0.50
0.005
0.01
0.015
0.02
0.025
0.03
0
0.002
0.004
0.006
0.008
UO2(s)
dissolved U
Xp
H,E
h0.1 0.2 0.3 0.4 0.5
0
1
2
3
4
5
6
7
8
9
pH
Eh
910 sec
UO2(s) UO2(s) dissolutiondissolution and and transporttransport
Distance (m)
Dis
so
lve
dU
(M)
UO
2(s
)(m
ol/kg
so
il)
0.1 0.2 0.3 0.4 0.50
0.005
0.01
0.015
0.02
0.025
0.03
0
0.002
0.004
0.006
0.008
UO2(s)
dissolved U
Xp
H,E
h0.1 0.2 0.3 0.4 0.5
0
1
2
3
4
5
6
7
8
9
pH
Eh
1110 sec
UO2(s) UO2(s) dissolutiondissolution and and transporttransport
Distance (m)
Dis
so
lve
dU
(M)
UO
2(s
)(m
ol/kg
so
il)
0.1 0.2 0.3 0.4 0.50
0.005
0.01
0.015
0.02
0.025
0.03
0
0.002
0.004
0.006
0.008
UO2(s)
dissolved U
Xp
H,E
h0.1 0.2 0.3 0.4 0.5
0
1
2
3
4
5
6
7
8
9
pH
Eh
2e4 sec
Content
� Introduction
� Reactive Transport Modelling
� Reactions and Database
� Application – UO2(s) dissolutionand transport
� Outlook
Outlook
� Implementation of coupled effect of volumetric changes due to chemical reaction on HM-behaviour
� Corrosion of HLW container and gas production
� Performance assessment: Application to real systems
� Paralel computing