Subsurface Flow and Transport

Remediation strategies have been developed for a variety of contaminants by integrating theory, experiment and numerical simulation prior to field-scale studies. Researchers can conduct experiments at various scales, and compare experimental and numerical results to address the nation's most challenging problems in the subsurface related to contaminant transport, carbon cycling, enhanced oil recovery and carbon dioxide sequestration.

Resources and Techniques

  • Users have access to all the tools—flow cells, simulation programs and analytical instruments from chromatographs to spectrometers—necessary for designing and conducting a subsurface flow and transport experiments.
  • Designing experiments—Simulators such as STOMP (Subsurface Transport Over Multiple Phases) are used to define the boundary and initial conditions of the experiment.
  • Conducting experiments—Micro- to intermediate-flow cells are used with analytical tools to generate data about how contaminants move through the soil.
  • A full suite of analytical tools are available to generate data about samples.

Additional Information:

Description

Capability Details

  • Intermediate-scale columns and flow cells
  • Pore-scale microfluidic and imaging capabilities
  • High-pressure/temperature cells for research at reservoir conditions
  • Dual energy gamma radiation system
  • Integrated hydraulic properties apparatus
  • Relative permeability apparatus
  • Analytical tools including ion, liquid and gas chromatographs, inductively coupled plasma-mass spectrometry and carbon analysis tools

Instruments

EMSL's Subsurface Flow and Transport Experimental Laboratory offers several meter-scale flow cells and columns for research in saturated and...
Custodian(s): Tom Wietsma, Mart Oostrom
The Agilent 4500 Series inductively coupled plasma mass spectrometer (ICP-MS) is available for all research areas requiring analysis of trace metals...
Custodian(s): Tom Wietsma
This ion chromatography capability comprises two Dionex DX-500 modular chromatography systems that can be configured to conduct fully automated...
Custodian(s): Tom Wietsma
The Agilent 1100 Series liquid chromatography system is used for all research areas that require quantitative determination of nonvolatile and...
Custodian(s): Tom Wietsma
The pore-scale micromodel flow and transport lab is part of EMSL's Subsurface Flow and Transport Laboratory (SFTL) with a focus on coupled (...
Custodian(s): Mart Oostrom

Publications

This paper presents the results of a comprehensive model-based analysis of a uranium tracer test conducted at the U.S Department of Energy Hanford...
Zero-valent iron particles are an effective remediation technology for groundwater contaminated with halogenated organic compounds. In particular,...
The adsorption and speciation of U(VI) was investigated on contaminated, fine grained sediment materials from the Hanford 300 area (SPP1 GWF) in...
The outer membrane decaheme c-type cytochromes (c-Cyt) MtrC and OmcA of Shewanella oneidensis MR-1(MR-1) play critical roles in extracellular...
The microbial reduction of Fe(III) and U(VI) were investigated in shallow aquifer sediments collected from subsurface Pleistocene flood deposits near...

Science Highlights

Posted: July 11, 2014
The Science The physical and chemical processes that occur at the scale of individual soil particles dictate the way fluids flow underground over...
Posted: April 21, 2014
A multidisciplinary team of scientists at Pacific Northwest National Laboratory using EMSL resources developed a new approach to simulate water...
Posted: March 19, 2013
One of the most noteworthy concerns for the U.S. Department of Energy is controlling atmospheric carbon dioxide to mitigate its effects on global...
Posted: June 13, 2012
Using EMSL capabilities,  scientists at Pacific Northwest National Laboratory determined the wettability—the preference of a rock or other surface...

Remediation strategies have been developed for a variety of contaminants by integrating theory, experiment and numerical simulation prior to field-scale studies. Researchers can conduct experiments at various scales, and compare experimental and numerical results to address the nation's most challenging problems in the subsurface related to contaminant transport, carbon cycling, enhanced oil recovery and carbon dioxide sequestration.

Resources and Techniques

  • Users have access to all the tools—flow cells, simulation programs and analytical instruments from chromatographs to spectrometers—necessary for designing and conducting a subsurface flow and transport experiments.
  • Designing experiments—Simulators such as STOMP (Subsurface Transport Over Multiple Phases) are used to define the boundary and initial conditions of the experiment.
  • Conducting experiments—Micro- to intermediate-flow cells are used with analytical tools to generate data about how contaminants move through the soil.
  • A full suite of analytical tools are available to generate data about samples.

Additional Information:

Assessment of Controlling Processes for Field-Scale Uranium Reactive Transport under Highly Transient Flow Conditions.

Abstract: 

This paper presents the results of a comprehensive model-based analysis of a uranium tracer test conducted at the U.S Department of Energy Hanford 300 Area (300A) IFRC site. A three-dimensional multi-component reactive transport model was employed to assess the key factors and processes that control the field-scale uranium reactive transport. Taking into consideration of relevant physical and chemical processes, the selected conceptual/numerical model replicates the spatial and temporal variations of the observed U(VI) concentrations reasonably well in spite of the highly complex field conditions. A sensitivity analysis was performed to interrogate the relative importance of various processes and factors for reactive transport of U(VI) at the field-scale. The results indicate that multi-rate U(VI) sorption/desorption, U(VI) surface complexation reactions, and initial U(VI) concentrations were the most important processes and factors controlling U(VI) migration. On the other hand, cation exchange reactions, the choice of the surface complexation model, and dual-domain mass transfer processes, which were previously identified to be important in laboratory experiments, played less important roles under the field-scale experimental condition at the 300A site. However, the model simulations also revealed that the groundwater chemistry was relatively stable during the uranium tracer experiment and therefore presumably not dynamic enough to appropriately assess the effects of ion exchange reaction and the choice of surface complexation models on U(VI) sorption and desorption. Furthermore, it also showed that the field experimental duration (16 days) was not sufficiently long to precisely assess the role of a majority of the sorption sites that were accessed by slow kinetic processes within the dual domain model. The sensitivity analysis revealed the crucial role of the intraborehole flow that occurred within the long-screened monitoring wells and thus significantly affected both field-scale measurements and simulated U(VI) concentrations as a combined effect of aquifer heterogeneity and highly dynamic flow conditions. Overall, this study, which provides one of the few detailed and highly data-constrained uranium transport simulations, highlights the difference in controlling processes between laboratory and field scale that prevent a simple direct upscaling of laboratory-scale models.

Citation: 
Ma R, C Zheng, C Liu, J Greskowiak, H Prommer, and JM Zachara.2014."Assessment of Controlling Processes for Field-Scale Uranium Reactive Transport under Highly Transient Flow Conditions."Water Resources Research 50(2):1006-1024. doi:10.1002/2013WR013835
Authors: 
Ma R
C Zheng
C Liu
J Greskowiak
H Prommer
JM Zachara
Instruments: 
Volume: 
50
Issue: 
2
Pages: 
1006-1024
Publication year: 
2014

Determination of water saturation using gas phase partitioning tracers and time-lapse electrical conductivity measurements.

Abstract: 

Water saturation is an important indicator of contaminant distribution and plays a governing role in contaminant transport within the vadose zone. Understanding the water saturation distribution is critical for both remediation and contaminant flux monitoring in unsaturated environments. In this work we propose and demonstrate a method of remotely determining water saturation levels using gas phase partitioning tracers and time-lapse bulk electrical conductivity measurements. The theoretical development includes the partitioning chemistry for the tracers we demonstrate (ammonia and carbon dioxide), as well as a review of the petrophysical relationship governing how these tracers influence bulk conductivity. We also investigate methods of utilizing secondary information provided by electrical conductivity breakthrough magnitudes induced by the tracers. We test the method on clean, well characterized, intermediate-scale sand columns under controlled conditions. Results demonstrate the capability to predict partitioning coefficients and accurately monitor gas breakthrough curves along the length of the column according to the corresponding electrical conductivity response, leading to accurate water saturation estimates. This work is motivated by the need to develop effective characterization and monitoring techniques for contaminated deep vadose zone environments, and provides a proof-of-concept toward uniquely characterizing and monitoring water saturation levels at the field scale and in three-dimensions using electrical resistivity tomography.

Citation: 
Johnson TC, M Oostrom, MJ Truex, JN Thomle, and TW Wietsma.2013."Determination of water saturation using gas phase partitioning tracers and time-lapse electrical conductivity measurements."Vadose Zone Journal 12(2):, doi:10.2136/vzj2012.0142
Authors: 
TC Johnson
M Oostrom
MJ Truex
JN Thomle
TW Wietsma
Instruments: 
Volume: 
Issue: 
Pages: 
Publication year: 
2013

Development of a Proteoliposome Model to Probe Transmembrane Electron-Transfer Reactions.

Abstract: 

The mineral respiring bacterium Shewanella oneidensis uses a protein complex, MtrCAB, composed of two decaheme cytochromes brought together inside a transmembrane porin to transport electrons across the outer membrane to a variety of mineral-based electron acceptors. A proteoliposome system has been developed that contains methyl viologen (MV) as an internalised electron acceptor and valinomycin (V) as a membrane associated cation exchanger. These proteoliposomes can be used as a model system to investigate MtrCAB function.

Citation: 
White GF, Z Shi, L Shi, A Dohnalkova, JK Fredrickson, JM Zachara, JN Butt, DJ Richardson, and T Clarke.2012."Development of a Proteoliposome Model to Probe Transmembrane Electron-Transfer Reactions."Biochemical Society: Transactions 40(6):1257-1260. doi:10.1042/BST20120116
Authors: 
GF White
Z Shi
L Shi
A Dohnalkova
JK Fredrickson
JM Zachara
JN Butt
DJ Richardson
T Clarke
Volume: 
40
Issue: 
6
Pages: 
1257-1260
Publication year: 
2012

Microbial Reductive Transformation of Phyllosilicate Fe(III) and U(VI) in Fluvial Subsurface Sediments.

Abstract: 

The microbial reduction of Fe(III) and U(VI) were investigated in shallow aquifer sediments collected from subsurface Pleistocene flood deposits near the Hanford Reach of the Columbia River in Washington State. Increases in 0.5 N HCl-extractable Fe(II) were observed in incubated sediments and 57Fe Mössbauer spectroscopy revealed that Fe(III) associated with phyllosilicates and pyroxene was reduced to Fe(II). Aqueous uranium(VI) concentrations decreased in incubated Hanford sediments with the rate and extent being greater in sediment amended with organic carbon. X-ray absorption spectroscopy of bioreduced sediments indicated that 67-77% of the U signal was U(VI), probably as an adsorbed species associated with a new or modified reactive mineral phase. Phylotypes within the Deltaproteobacteria were more common in Hanford sediments incubated with U(VI) than without and in U(VI)-free incubations, members of the Clostridiales were dominant with sulfate-reducing phylotypes more common in the sulfate-amended sediments. These results demonstrate the potential for anaerobic reduction phyllosilicate Fe(III) and sulfate in Hanford unconfined aquifer sediments and biotransformations involving reduction and adsorption leading to decreased aqueous U concentrations.

Citation: 
Lee JH, JK Fredrickson, RK Kukkadapu, MI Boyanov, KM Kemner, X Lin, DW Kennedy, BN Bjornstad, A Konopka, DA Moore, CT Resch, and JL Phillips.2012."Microbial Reductive Transformation of Phyllosilicate Fe(III) and U(VI) in Fluvial Subsurface Sediments."Environmental Science & Technology 46(7):3721–3730. doi:10.1021/es204528m
Authors: 
JH Lee
JK Fredrickson
RK Kukkadapu
MI Boyanov
KM Kemner
X Lin
DW Kennedy
BN Bjornstad
A Konopka
DA Moore
CT Resch
JL Phillips
Volume: 
Issue: 
Pages: 
Publication year: 
2012

Identification and Characterization of UndA-HRCR-6, an Outer Membrane Endecaheme c-Type Cytochrome of Shewanella sp. Strain HRCR

Abstract: 

The outer membrane decaheme c-type cytochromes (c-Cyt) MtrC and OmcA of Shewanella oneidensis MR-1(MR-1) play critical roles in extracellular reduction of iron [Fe(III)] oxides and uranium [ U(VI)]. To identify and characterize the outer membrane c-Cyts found in the metal-reducing Shewanella strains isolated from the Hanford Reach of the Columbia River (HRCR), 7 HRCR isolates were tested for the presence of mtrC, omcA and undA1 (a gene encoding a putative 11-heme c-Cyt) homologues in their genomes. All 7 tested strains possessed an mtrC homologue, while 3 strains had an omcA homologue and the remaining 4 strains contained an undA1 homologue. The coding region of an undA1 homologue from HRCR isolate 6 was cloned and sequenced. Because it was 93% identical to the UndA of S. baltica OS223, the protein product encoded by this sequenced gene was named as UndA-HRCR6. In MR-1, UndA-HRCR6 (i) restored an MR-1 mutant’s ability to reduce solid phase ferrihydrite at 40% of that for MR-1 wild type, (ii) increased extracellular formation of UO2 associated with the outer membrane and extracellular polymeric substances in a U(VI) reduction assay and (iii) was secreted to the extracellular environment by bacterial type II secretion system. UndA-HRCR6 was purified from the membrane fraction following its overexpression in MR-1 cells. Purified UndA-HRCR6 possessed 11 heme-Fe and reduced ferric complexes. Collectively, these results show that UndA-HRCR6 is an outer membrane endecaheme c-Cyt and can serve an extracellular metal reductase with functions similar to that of MR-1 MtrC and OmcA.

Citation: 
Shi L, SM Belchik, Z Wang, DW Kennedy, A Dohnalkova, MJ Marshall, JM Zachara, and JK Fredrickson.2011."Identification and Characterization of UndA-HRCR-6, an Outer Membrane Endecaheme c-Type Cytochrome of Shewanella sp. Strain HRCR-6 ."Applied and Environmental Microbiology 77(15):5521-5523. doi:10.1128/AEM.00614-11
Authors: 
L Shi
SM Belchik
Z Wang
DW Kennedy
A Dohnalkova
MJ Marshall
JM Zachara
JK Fredrickson
Volume: 
77
Issue: 
15
Pages: 
5521-5523
Publication year: 
2011

Determining Individual Mineral Contributions To U(VI) Adsorption In A Contaminated Aquifer Sediment: A Fluorescence Spectroscopy

Abstract: 

The adsorption and speciation of U(VI) was investigated on contaminated, fine grained sediment materials from the Hanford 300 area (SPP1 GWF) in simulated groundwater using cryogenic laser-induced U(VI) fluorescence spectroscopy combined with chemometric analysis. A series of reference minerals (montmorillonite, illite, Michigan chlorite, North Carolina chlorite, California clinochlore, quartz and synthetic 6-line ferrihydrite) was used for comparison that represents the mineralogical constituents of SPP1 GWF. Surface area-normalized Kd values were measured at U(VI) concentrations of 5x10-7 mol L-1 and 5x10-6 mol L-1, respectively, that displayed the following affinity series: 6-line-ferrihydrite > North Carolina chlorite ≈ California clinochlore > Michigan chlorite ≈ quartz > montmorillonite ≈ illite ≈ SPP1 GWF. Both time-resolved spectra and asynchronous two-dimensional (2D) correlation analysis of SPP1 GWF at different delay times indicated that two major adsorbed U(VI) species were present in the sediment that resembled U(VI) adsorbed on quartz and phyllosilicates. Simulations of the normalized fluorescence spectra confirmed that the speciation of SPP1 GWF was best represented by a linear combination of U(VI) adsorbed on quartz (90%) and phyllosilicates (10%). However, the fluorescence quantum yield for U(VI) adsorbed on phyllosilicates was lower than quartz and, consequently, its fractional contribution to speciation may be underestimated. Spectral comparison with literature data suggested that U(VI) exists primarily as inner-sphere U(VI) complexes with surface silanol groups on quartz while U(VI) on phyllosilicates was consistent with the formation of surface U(VI) tricarbonate complexes.

Citation: 
Wang Z, JM Zachara, JF Boily, Y Xia, CT Resch, DA Moore, and C Liu.2011."Determining Individual Mineral Contributions To U(VI) Adsorption In A Contaminated Aquifer Sediment: A Fluorescence Spectroscopy Study."Geochimica et Cosmochimica Acta 75(10):2965–2979.
Authors: 
Z Wang
JM Zachara
JF Boily
Y Xia
CT Resch
DA Moore
C Liu
Volume: 
Issue: 
Pages: 
Publication year: 
2011

Zero Valent Iron: Impact of Anions Present during Synthesis on Subsequent Nanoparticle Reactivity.

Abstract: 

Zero-valent iron particles are an effective remediation technology for groundwater contaminated with halogenated organic compounds. In particular, nano-scale zero-valent iron is a promising material for remediation due to its high specific surface area, which results in faster rate constants and more effective use of the iron. An aspect of iron nanoparticle reactivity that has not been explored is the impact of anions present during iron metal nanoparticle synthesis. Solutions containing chloride, phosphate, sulfate, and nitrate anions and ferric ions were used to generate iron oxide nanoparticles. The resulting materials were dialyzed to remove dissolved byproducts and then dried and reduced by hydrogen gas at high temperature. The reactivity of the resulting zero valent iron nanoparticles was quantified by monitoring the kinetics as well as products of carbon tetrachloride reduction, and significant differences in reactivity and chloroform yield were observed. The reactivity of nanoparticles prepared in the presence of sulfate and phosphate demonstrated the highest reactivity and chloroform yield. Furthermore, substantial variations in the solid-state products of oxidation (magnetite, iron sulfide, and goethite, among others) were also observed.

Citation: 
Moore K, B Forsberg, DR Baer, WA Arnold, and RL Penn.2011."Zero Valent Iron: Impact of Anions Present during Synthesis on Subsequent Nanoparticle Reactivity."Journal of Environmental Engineering (ASCE) 137(10):889-896. doi:10.1061/(ASCE)EE.1943-7870.0000407
Authors: 
K Moore
B Forsberg
DR Baer
WA Arnold
RL Penn
Volume: 
137
Issue: 
10
Pages: 
889-896
Publication year: 
2011

Petal Thicknesses and Shape Transformations in Blooming Lilies.

Abstract: 

During blooming, flower petals undergo significant shape changes. For lilies, various different mechanisms responsible for the change have been suggested [1,2]. One is that cell growth along the edge of a petal, or, more generally, a tepal, drives a transition from a cup shape (within a bud) to a saddle shape (within a bloom). This mechanism has been previously considered for tepals modeled as shallow elliptical shells whose thickness from the center, t, falls off at least as fast as t = t0 (1 - x2/a2 - y2/b2 ) [1]. Here t0 is the maximum thickness of the shell, a and b are the semimajor and semiminoraxes, x and y are the coordinates along the longitudinal and lateral axes. By measuring tepal thicknesses from images collected by x-ray tomography of intact buds and by photography of microtomed buds, we find that this condition is indeed met for both Lilium casablanca and Lilium lancifolium. [1] Liang and Mahadevan. Growth, geometry, and mechanics of a blooming lily.

Citation: 
Portet T, PN Holmes, ME Bowden, SA Stephens, T Varga, and SL Keller.2013."Petal Thicknesses and Shape Transformations in Blooming Lilies."Biophysical Journal 104(2 Supplement 1):493A-493A. doi:10.1016/j.bpj.2012.11.2717
Authors: 
T Portet
PN Holmes
ME Bowden
SA Stephens
T Varga
SL Keller
Publication year: 
2013

Influence of Mg2+ on CaCO3 precipitation during subsurface reactive transport in a homogeneous silicon-etched pore network.

Abstract: 

Calcium carbonate (CaCO3) geochemical reactions exert a fundamental control on the evolution of porosity and permeability in shallow-to-deep subsurface siliciclastic and limestone rock reservoirs. As a result, these carbonate water-rock interactions play a critically important role in research on groundwater remediation, geological carbon sequestration, and hydrocarbon exploration. A study was undertaken to determine the effects of Mg2+ concentration on CaCO3 crystal morphology, precipitation rate, and porosity occlusion under flow and mixing conditions similar to those in subsurface aquifers.

Citation: 
Boyd V, H Yoon, C Zhang, M Oostrom, NJ Hess, BW Fouke, AJ Valocchi, and CJ Werth.2014."Influence of Mg2+ on CaCO3 precipitation during subsurface reactive transport in a homogeneous silicon-etched pore network."Geochimica et Cosmochimica Acta 135:321-335. doi:10.1016/j.gca.2014.03.018
Authors: 
V Boyd
H Yoon
C Zhang
M Oostrom
NJ Hess
BW Fouke
AJ Valocchi
CJ Werth
Publication year: 
2014

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