© 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 (djacques@sckcen.be)

5th International Hydrus Conference ‘Hydrus software applications to subsurface flow and contaminant transport problems’ March 30-32 2017, Prague

© 2017 SCK•CEN

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

14

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

15

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.

© 2017 SCK•CEN

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).

© 2017 SCK•CEN

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!