Colloid and colloid-facilitated transport modeling using HPx · Equilibrium – kinetically...
Transcript of Colloid and colloid-facilitated transport modeling using HPx · Equilibrium – kinetically...
© 2017 SCK•CEN
Colloid and colloid-facilitated transport modeling using HPx
D. Jacques1
, D. Zhou2, J. Makselon3, I. Engelhardt2, and S. Thiele-Bruh4
1SCK-CEN, 2TU Berlin, 3Forschungszentrum Jülich GmbH, 4University of
Trier ([email protected])
5th International Hydrus Conference ‘Hydrus software applications to subsurface flow and contaminant transport problems’ March 30-32 2017, Prague
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Slide title
HPx – codes : Overview & recent developments
Applications: Colloidal and colloidal-facilitated transport
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BioGeoChemical Processes +
Leterme et al., 2014 Battle-Aguilar et al., 2011
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Transport phenomena =
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3.4 3.6 3.8 4 4.2pH
1x101
1x102
1x103
1x104
K =
ads
orbe
d U
(mol
/l) /
aque
ous
U (m
ol /
l)
AtmosphericSteady-state 25 cm depth
5 cm depth
Reactive transport
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Generic reactive transport codes
Typically couples flow (Richards) and transport (ADE, heat) with geochemistry(Steefel et al., 2015)
Equilibrium – kinetically controlled biogeochemical reaction processes
Coupling of properties/parameters between different state variables
Flexibility in defining conceptual models : moving towards a Problem-solving environment (Meysman et al., 2003)
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A Coupled Numerical Code for Variably Saturated Water Flow,
Solute Transport and BioGeoChemistry
in Soil Systems
Simulating water flow, transport and bio-geochemical reactions in environmental soil quality problems
Flow and transport model HYDRUS-1D 4.0
HYDRUS (2D/3D) 2.x
Biogeochemical model PHREEQC-3
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Rien van Genuchten Dirk Mallants
Diederik Jacques Jirka Simunek Mirek Senja
International cooperation
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Governing Equations – Flow and Transport
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Governing Equations – Equilibrium
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Governing Equations – Kinetics
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HPx – strong focus on unsaturated zone / soil systems
Heterogeneous media
Atmospheric boundary conditions, heat flow
Various functions for hydraulic properties
Various functions for root water & solute uptake
1D/2D/3D geometry
Coupling transport properties to geochemical state variables
AE
Bh1Bh2
Bh/C
C1
C2
07
192428
50
75
depth(cm)
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Water flow and solute transport models Uniform flow and transport model
13
Three phase system Aqueous, solid and gas phase
Sol
id p
hase
P
oros
ity
Gas phase Aqueous phase
Transport Water flow Heat transport Advection-dispersion in aqueous phase Diffusion in gas phase θa θw
εs
Homogeneous sink/source terms S Root water uptake Sr,w Solute root uptake Sr,s,i Degradation/decay/transformation Sc,i
Sr,w Sr,s,i Sc,i Heterogeneous mass exchange Γ
Aqueous – solid phase Γws Aqueous – air phase Γwa
Γws
Γwa
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Water flow and solute transport models Uniform flow and MIM transport model
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Two domains Mobile / Immobile
Sol
id p
hase
P
oros
ity
Gas phase Aqueous phase
Transport Water flow Heat transport Advection-dispersion in aqueous phase Diffusion in gas phase Solute exchange Γi
θa θw
εs
Homogeneous sink/source terms S Root water uptake Sr,w Solute root uptake Sr,s,i Degradation/decay/transformation Sc,i Sr,w
Sr,s,i Sc,i
Heterogeneous mass exchange Γ Aqueous – solid phase Γws : in both
mobile and immobile domain Aqueous – air phase Γwa
Γws,m
Γwa
Mobile Immobile Three phase system Aqueous, solid and gas phase
Γws,im
Γi
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Water flow and solute transport models Dual-porosity model water flow and solute transport
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Two domains Mobile / Immobile
Sol
id p
hase
P
oros
ity
Gas phase Aqueous phase
Transport Water flow Heat transport Advection-dispersion in aqueous phase Diffusion in gas phase Water exchange Γw Solute exchange Γi Homogeneous sink/source terms S Root water uptake Sr,w Solute root uptake Sr,s,i Degradation/decay/transformation Sc,i Sr,w
Sr,s,i Sc,i
Heterogeneous mass exchange Γ Aqueous – solid phase Γws : in both
mobile and immobile domain Aqueous – air phase Γwa
Γws,m
Γwa
Mobile Immobile Three phase system Aqueous, solid and gas phase
Γws,im Γi
Γw
θa θw
εs
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Numerical Tool - GUI
Geometry and physical processes
Geochemical processes and coupling
Processing of output
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Processes not in the standard HYDRUS
Diffusion in the gas phase
Mayer et al. (2015)
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Processes not in the standard HYDRUS
Update of physical, hydrological and transport parameters
Xie et al. (2015)
0 0.5 1 1.5 2λ (mm/y0.5)
0
0.1
0.2
0.3
0.4
Por
osity
0 0.5 1 1.5 2λ (mm/y0.5)
10-4
10-3
10-2
10-1
100
Tortu
osity
fact
or
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Phreeqc-3
OPEN-MP Scripting
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Include different SOM degradation models
H2O = OH- + H+
CO32- + H+ = HCO3
-
CO32- + 2H+ = CO2 + H2O
CO2(g) = CO2(aq)
Geochemistry
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Accounting for environmental variables result in a spatial-temporal pattern
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Adding a mobile component
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Introducing bioturbation – mixing of SOM between different layers
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Output
Different output files with selected_output and user_punch Recently added 2D – meshlines 2D – crosssections Totals for MIM model Integration over horizons, layers, depths, nodes
GNUPLOT templates Profiles Time series
2D plots generated using the GUI
Viewing with HPxOutput
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Advertisement
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Protection
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Impact of DOC quality on sulfonamide transport in soils
application of pig manure (3 ≠ qualities) to soil contains veterinary antibiotics (3 ≠ sulfonamides - SA)
Zhou, D., S. Thiele-Bruhn, M. G. Arenz-Leufen, D. Jacques, P. Lichtner and I. Engelhardt (2016). "Impact of manure-related DOM on sulfonamide transport in arable soils." Journal of Contaminant Hydrology 192: 118-128.
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Step 1 – DOC transport model
AD equation with CFT
CFT is applicable Non-equilibrium sorption of colloids F – highest retardation (highest aromaticity and hydrophobicity)
Zhou, D., et al., 2016
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Step 2 – Antibiotic transport model
AD equation with Langmuir competitive adsorption kinetic
Second-order kinetic adsorption and competition, first-order desorption SMOX – highest retardation (sorption driven by the sulfonamide R-substituents -> hydrophobicity & polarity)
Zhou, D., et al., 2016
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Step 3 – Colloidal-affected transport
AD equation with kinetic sorption on mobile and immobile colloids and competitive kinetic sorption
AD equation of DOM-S with kinetic sorption/desorption Immobile DOM-S with kinetic sorption/desorption
SDZ, SMPD – retardation Immobile DOM gives additional sorption Independent of DOM type
Zhou, D., et al., 2016
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Step 3 – Colloidal-affected transport
AD equation with kinetic sorption on mobile and immobile colloids and competitive kinetic sorption
AD equation of DOM-S with kinetic sorption/desorption Immobile DOM-S with kinetic sorption/desorption
SMOX – depending on DOM type For F-type, mobility was enhanced because increased competition for adsorption on surface
Zhou, D., et al., 2016
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Transport of AgNP under variable flow and ionic strenght
Makselon, J., D. Zhou, I. Engelhardt, D. Jacques and E. Klumpp (2017). "Experimental and Numerical Investigations of Silver Nanoparticle Transport under Variable Flow and Ionic Strength in Soil." Environmental Science & Technology 51(4): 2096-2104.
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Model Approach
AD accounting for colloid filtration at SW and SA interface
Influence of change in water
Makselon et al. (2017).
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Model Approach
AD accounting for colloid filtration at SW and SA interface
Influence of ionic strength / geochemical composition
Influence of ionic strength / geochemical composition “attachment efficiency” calculated via the DVLO theory
Makselon et al. (2017).
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Model Approach
Makselon et al. (2017).
Lower IS Higher maximum energy barrier Smaller secondary minimum So : decrease in attachment efficiency
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Model Approach
Makselon et al. (2017).
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End
HPx combines the best of two worlds
We work towards large flexibility but trying also to facilitate input and post-processing
Learning curve could be significant
A well defined idea of the conceptual geochemical model is required
We welcome applications of HPx for various systems!