Colloid and colloid-facilitated transport modeling using HPx

Transcription

1 Colloid and colloid-facilitated transport modeling using HPx D. Jacques 1, D. Zhou 2, J. Makselon 3, I. Engelhardt 2, and S. Thiele-Bruh 4 1 SCK-CEN, 2 TU Berlin, 3 Forschungszentrum Jülich GmbH, 4 University of Trier (djacques@sckcen.be) 5th International Hydrus Conference Hydrus software applications to subsurface flow and contaminant transport problems March , Prague

2 Slide title HPx codes : Overview & recent developments Applications: Colloidal and colloidal-facilitated transport

3 BioGeoChemical Processes + Leterme et al., 2014 Battle-Aguilar et al., 2011

4 Transport phenomena =

5 Reactive transport K = adsorbed U (mol/l) / aqueous U (mol / l) 1x10 4 1x10 3 1x10 2 1x10 1 Atmospheric Steady-state ph 25 cm depth 5 cm depth

6 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)

7 Simulating water flow, transport and bio-geochemical reactions in environmental soil quality problems A Coupled Numerical Code for Variably Saturated Water Flow, Solute Transport and BioGeoChemistry in Soil Systems Flow and transport model HYDRUS-1D 4.0 HYDRUS (2D/3D) 2.x Biogeochemical model PHREEQC-3

8 International cooperation Rien van Genuchten Dirk Mallants Diederik Jacques Jirka Simunek Mirek Senja

9 Governing Equations Flow and Transport

10 Governing Equations Equilibrium

11 Governing Equations Kinetics

12 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 A E Bh1 Bh2 Bh/C C1 C2 depth (cm) D/2D/3D geometry Coupling transport properties to geochemical state variables

13 Water flow and solute transport models Uniform flow and transport model Solid phase Porosity ε s θ a θ w Γ wa Γ ws S r,w S r,s,i S c,i Three phase system Aqueous, solid and gas phase Transport Water flow Heat transport Advection-dispersion in aqueous phase Diffusion in gas phase Homogeneous sink/source terms S Root water uptake S r,w Solute root uptake S r,s,i Degradation/decay/transformation S c,i Heterogeneous mass exchange Γ Aqueous solid phase Γ ws Aqueous air phase Γ wa Gas phase Aqueous phase 13

14 Water flow and solute transport models Uniform flow and MIM transport model Mobile Immobile Three phase system Aqueous, solid and gas phase Solid phase ε s θ a θ w Γ ws,m Γ ws,im Two domains Mobile / Immobile Transport Water flow Heat transport Advection-dispersion in aqueous phase Diffusion in gas phase Solute exchange Γ i Porosity Γ wa S r,w S r,s,i S c,i Γ i Homogeneous sink/source terms S Root water uptake S r,w Solute root uptake S r,s,i Degradation/decay/transformation S c,i Heterogeneous mass exchange Γ Aqueous solid phase Γ ws : in both mobile and immobile domain Aqueous air phase Γ wa Gas phase Aqueous phase 14

15 Water flow and solute transport models Dual-porosity model water flow and solute transport Mobile Immobile Three phase system Aqueous, solid and gas phase Solid phase ε s θ a θ w Γ ws,m Γ i Γ ws,im Two domains Mobile / Immobile Transport Water flow Heat transport Advection-dispersion in aqueous phase Diffusion in gas phase Water exchange Γ w Solute exchange Γ i Porosity Γ wa S r,w S r,s,i S c,i Γ w Homogeneous sink/source terms S Root water uptake S r,w Solute root uptake S r,s,i Degradation/decay/transformation S c,i Heterogeneous mass exchange Γ Aqueous solid phase Γ ws : in both mobile and immobile domain Aqueous air phase Γ wa Gas phase Aqueous phase 15

16 Numerical Tool - GUI Geometry and physical processes Geochemical processes and coupling Processing of output

17 Diffusion in the gas phase Processes not in the standard HYDRUS Mayer et al. (2015)

18 Processes not in the standard HYDRUS Update of physical, hydrological and transport parameters Porosity Xie et al. (2015) Tortuosity factor λ (mm/y0.5) λ (mm/y0.5)

19 Phreeqc-3 OPEN-MP Scripting

20 Include different SOM degradation models Geochemistry H 2 O = OH - + H + CO H + = HCO 3 - CO H + = CO 2 + H 2 O CO 2(g) = CO 2(aq)

21 Accounting for environmental variables result in a spatialtemporal pattern

22 Adding a mobile component

23 Introducing bioturbation mixing of SOM between different layers

24 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 Output GNUPLOT templates Profiles Time series 2D plots generated using the GUI Viewing with HPxOutput

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26 Protection

27 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:

28 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

29 Step 2 Antibiotic transport model AD equation with Langmuir competitive adsorption kinetic Zhou, D., et al., 2016 Second-order kinetic adsorption and competition, first-order desorption SMOX highest retardation (sorption driven by the sulfonamide R-substituents -> hydrophobicity & polarity)

30 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

31 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

32 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):

33 Model Approach AD accounting for colloid filtration at SW and SA interface Influence of change in water Makselon et al. (2017).

34 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).

35 Model Approach Lower IS Makselon et al. (2017). Higher maximum energy barrier Smaller secondary minimum So : decrease in attachment efficiency

36 Model Approach Makselon et al. (2017).

37 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!