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. See a complete list of Subsurface Flow and Transport instruments.

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.

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

The carbon analyzer is used to analyze total carbon (TC), inorganic carbon (IC), total organic carbon (TOC), purgeable organic carbon (POC), and non...
Custodian(s): Tom Wietsma
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 instrument is housed in EMSL.  More details about this instrument will be available soon.
Custodian(s): Tom Wietsma, Mart Oostrom
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

Publications

The altered layer (i.e., amorphous hydrated surface layer and crystalline reaction products)represents a complex region, both physically and...
Bacterial species in the Enterobacteriaceae typically contain multiple paralogues of a small domain of unknown function (DUF1471) from a family of...
The occurrence of plutonium dioxide (PuO2) either from direct deposition or from the precipitation of plutonium-bearing solutions in contaminated...
Implantation with 1 MeV N ions was performed at room temperature in n-type 4H-SiC(0001) to four implantation fluences (or doses in dpa (displacements...
An in-situ study is reported on the structural evolution in nanocluster films under He+ ion irradiation using an advanced helium ion microscope. The...

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. See a complete list of Subsurface Flow and Transport instruments.

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.

Structural and Functional Characterization of DUF1471 Domains of Salmonella Proteins SrfN, YdgH/SssB, and YahO.

Abstract: 

Bacterial species in the Enterobacteriaceae typically contain multiple paralogues of a small domain of unknown function (DUF1471) from a family of conserved proteins also known as YhcN or BhsA/McbA. Proteins containing DUF1471 may have a
single or three copies of this domain. Representatives of this family have been demonstrated to play roles in several cellular processes including stress response, biofilm formation, and pathogenesis. We have conducted NMR and X-ray crystallographic studies of four DUF1471 domains from Salmonella representing three different paralogous DUF1471 subfamilies: SrfN, YahO, and SssB/YdgH (two of its three DUF1471 domains: the N-terminal domain I (residues 21–91), and the C-terminal domain III (residues 244–314)). Notably, SrfN has been shown to have a role in intracellular infection by Salmonella Typhimurium. These domains share less than 35% pairwise sequence identity. Structures of all four domains show a mixed a+b fold that is most similar to that of bacterial lipoprotein RcsF. However, all four DUF1471 sequences lack the redox sensitive cysteine residues essential for RcsF activity in a phospho-relay pathway, suggesting that DUF1471 domains perform a different function(s). SrfN forms a dimer in contrast to YahO and SssB domains I and III, which are monomers in solution. A putative binding site for oxyanions such as phosphate and sulfate was identified in SrfN, and an interaction between the SrfN dimer and sulfated polysaccharides was demonstrated, suggesting a direct role for this DUF1471 domain at the host-pathogen interface.

Citation: 
Eletsky A, K Michalska, S Houliston, Q Zhang, MD Daily, X Xu, H Cui, A Yee, A Lemak, B Wu, M Garcia, MC Burnet, KM Meyer, UK Aryal, O Sanchez, C Ansong, R Xiao, T Acton, JN Adkins, G Montelione, A Joachimiak, CH Arrowsmith, A Savchenko, T Szyperski, and JR Cort.2014."Structural and Functional Characterization of DUF1471 Domains of Salmonella Proteins SrfN, YdgH/SssB, and YahO."PLoS One 9(7):Article No. e101787. doi:10.1371/journal.pone.0101787
Authors: 
A Eletsky
K Michalska
S Houliston
Q Zhang
MD Daily
X Xu
H Cui
A Yee
A Lemak
B Wu
M Garcia
MC Burnet
KM Meyer
UK Aryal
O Sanchez
C Ansong
R Xiao
T Acton
JN Adkins
G Montelione
A Joachimiak
CH Arrowsmith
A Savchenko
T Szyperski
JR Cort
Facility: 
Volume: 
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Publication year: 
2014

Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations.

Abstract: 

The altered layer (i.e., amorphous hydrated surface layer and crystalline reaction products)represents a complex region, both physically and chemically, sandwiched between two distinct boundaries - pristine glass surface at the inner most interface and aqueous solution at the outer most. The physico-chemical processes that control the development of this region have a significant impact on the long-term glass-water reaction. Computational models, spanning different length and time-scales, are currently being developed to improve our understanding of this complex and dynamic process with the goal of accurately describing the pore-scale changes that occur as the system evolves. These modeling approaches include Geochemical Reaction Path simulations, Glass Reactivity in Allowance for Alteration Layer simulations, Monte Carlo simulations, and Molecular Dynamics methods. Discussed in this manuscript are the advances and limitations of each modeling approach placed in the context of the glass water reaction and how collectively these approaches provide insights into the mechanisms that control the formation and evolution of altered layers; thus providing the fundamental data needed to develop pore-scale equations that enable more accurate predictions of nuclear waste glass corrosion in a geologic repository.

Citation: 
Pierce EM, P Frugier, LJ Criscenti, KD Kwon, and SN Kerisit.2014."Modeling Interfacial Glass-Water Reactions: Recent Advances and Current Limitations."International Journal of Applied Glass Science 5(4):421-435. doi:10.1111/ijag.12077
Authors: 
EM Pierce
P Frugier
LJ Criscenti
KD Kwon
SN Kerisit
Volume: 
5
Issue: 
4
Pages: 
421-435
Publication year: 
2014

In-situ Study of Nanostructure and Electrical Resistance of Nanocluster Films Irradiated with Ion Beams.

Abstract: 

An in-situ study is reported on the structural evolution in nanocluster films under He+ ion irradiation using an advanced helium ion microscope. The films consist of loosely interconnected nanoclusters of magnetite or iron-magnetite (Fe-Fe3O4) core-shells. The nanostructure is observed to undergo dramatic changes under ion-beam irradiation, featuring grain growth, phase transition, particle aggregation, and formation of nanowire-like network and nano-pores. Studies based on ion irradiation, thermal annealing and election irradiation have indicated that the major structural evolution is activated by elastic nuclear collisions, while both electronic and thermal processes can play a significant role once the evolution starts. The electrical resistance of the Fe-Fe3O4 films measured in situ exhibits a super-exponential decay with dose. The behavior suggests that the nanocluster films possess an intrinsic merit for development of an advanced online monitor for neutron radiation with both high detection sensitivity and long-term applicability, which can enhance safety measures in many nuclear operations.

Citation: 
Jiang W, JA Sundararajan, T Varga, ME Bowden, Y Qiang, JS McCloy, CH Henager, Jr, and RO Montgomery.2014."In-situ Study of Nanostructure and Electrical Resistance of Nanocluster Films Irradiated with Ion Beams."Advanced Functional Materials 24(39):6210-6218. doi:10.1002/adfm.201400553
Authors: 
W Jiang
JA Sundararajan
T Varga
ME Bowden
Y Qiang
JS McCloy
CH Henager
Jr
RO Montgomery
Instruments: 
Volume: 
24
Issue: 
39
Pages: 
6210-6218
Publication year: 
2014

Characterization of Defects in N-type 4H-SiC After High-Energy N Ion Implantation by RBS-Channeling and Raman Spectroscopy.

Abstract: 

Implantation with 1 MeV N ions was performed at room temperature in n-type 4H-SiC(0001) to four implantation fluences (or doses in dpa (displacements per atom) at the damage peak) of 1.5×1013(0.0034), 7.8×1013(0.018), 1.5×1014(0.034), and 7.8×1014(0.18) ions/cm2, respectively. The evolution of disorder was studied using Rutherford backscattering spectrometry in channeling mode (RBS-C) and Raman spectroscopy. The disorder in the Si sub-lattice was found to be less than 10% for the dpa of 0.0034 and 0.0178 and increased to 40% and 60% for the dpa of 0.034 and 0.178 respectively. Raman Spectroscopy was performed using a green laser of wavelength 532 nm as excitation source. The normalized Raman Intensity, In shows disorder of 41%, 69%, 77% and 100% for the dpa of 0.0034, 0.017, 0.034 and 0.178 respectively. In this paper, the characterizations of the defects produced due to the Nitrogen implantation in 4H-SiC are presented and the results are discussed.

Citation: 
Kummari VC, T Reinert, W Jiang, FD McDaniel, and B Rout.2014."Characterization of Defects in N-type 4H-SiC After High-Energy N Ion Implantation by RBS-Channeling and Raman Spectroscopy."Nuclear Instruments and Methods in Physics Research. Section B, Beam Interactions with Materials and Atoms 332:28-32. doi:10.1016/j.nimb.2014.02.023
Authors: 
VC Kummari
T Reinert
W Jiang
FD McDaniel
B Rout
Instruments: 
Volume: 
Issue: 
Pages: 
Publication year: 
2014

Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site.

Abstract: 

The occurrence of plutonium dioxide (PuO2) either from direct deposition or from the precipitation of plutonium-bearing solutions in contaminated soils and sediments has been well described, particularly for the Hanford site in Washington State. However, past research has suggested that plutonium may exist in environmental samples at the Hanford site in chemical forms in addition to large size PuO2 particles and that these previously unidentified nano-sized particles maybe more reactive and thus more likely to influence the environmental mobility of Pu. Here we present evidence for the formation of nano-sized plutonium iron phosphate hydroxide structurally related to the rhabdophane group nanoparticles in 216-Z9 crib sediments from Hanford using transmission electron microscopy (TEM). The distribution and nature of these nanoparticles varied depending on the adjacent phases present. Fine electron probes were used to obtain electron diffraction and electron energy-loss spectra from specific phase regions of the 216-Z9 cribs specimens from fine-grained plutonium oxide and phosphate phases. Energy-loss spectra were used to evaluate the plutonium N4,5 (4d → 5f ) and iron L2,3 absorption edges. The iron plutonium phosphate formation may depend on the local micro-environment in the sediments, availability of phosphate, and hence the distribution of these minerals may control long-term migration of Pu in the soil. This study also points to the utility of using electron beam methods for determining the identity of actinide phases and their association with other sediment phases.

Citation: 
Buck EC, DA Moore, KR Czerwinski, SD Conradson, O Batuk, and AR Felmy.2014."Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site."Radiochimica Acta 102(12):1059-1068. doi:10.1515/ract-2013-2103
Authors: 
EC Buck
DA Moore
KR Czerwinski
SD Conradson
O Batuk
AR Felmy
Volume: 
102
Issue: 
12
Pages: 
1059-1068
Publication year: 
2014

An Electrically Switchable Metal-Organic Framework.

Abstract: 

Crystalline metal organic framework (MOF) materials containing interconnected porosity can be chemically modified to promote stimulus-driven (light, magnetic or electric fields) structural transformations that can be used in a number of devices. Innovative research strategies are now focused on understanding the role of chemical bond manipulation to reversibly alter the free volume in such structures of critical importance for electro-catalysis, molecular electronics, energy storage technologies, sensor devices and smart membranes. In this letter, we study the mechanism for which an electrically switchable MOF composed of Cu(TCNQ) (TCNQ 5 7,7,8,8-tetracyanoquinodimethane) transitions from a high-resistance state to a conducting state in a reversible fashion by an applied potential. The actual mechanism for this reversible electrical switching is still not understood even though a number of reports are available describing the application of electric-field-induced switching of Cu(TCNQ) in device fabrication.

Citation: 
Fernandez CA, PF Martin, HT Schaef, ME Bowden, PK Thallapally, LX Dang, W Xu, X Chen, and BP McGrail.2014."An Electrically Switchable Metal-Organic Framework."Scientific Reports 12(3):Article No. 6114 . doi:10.1038/srep06114
Authors: 
CA Fernez
PF Martin
HT Schaef
ME Bowden
PK Thallapally
LX Dang
W Xu
X Chen
BP McGrail
Facility: 
Volume: 
Issue: 
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Publication year: 
2014

Remedial Amendment Delivery near the Water Table Using Shear Thinning Fluids: Experiments and Numerical Simulations.

Abstract: 

The use of shear thinning fluids (STFs) containing xanthan is a potential enhancement for emplacing a solute amendment near the water table and within the capillary fringe. Most research to date related to STF behavior has involved saturated and confined conditions. A series of flow cell experiments were conducted to investigate STF emplacement in variable saturated homogeneous and layered heterogeneous systems. Besides flow visualization using dyes, amendment concentrations and pressure data were obtained at several locations. The experiments showed that injection of STFs considerably improved the subsurface distribution near the water table by mitigating preferential flow through higher permeability zones compared to no-polymer injections. The phosphate amendment migrated with the xanthan SFT without retardation. Despite the high viscosity of the STF, no excessive mounding or preferential flow were observed in the unsaturated zone. The STOMP simulator was able to predict the experimentally observed fluid displacement and amendment concentrations reasonably well. Cross flow between layers could be interpreted as the main mechanism to transport STFs into lower permeability layers based on the observed pressure gradient and concentration data in layers of differing hydraulic conductivity.

Citation: 
Oostrom M, MJ Truex, VR Vermeul, L Zhong, GD Tartakovsky, and TW Wietsma.2014."Remedial Amendment Delivery near the Water Table Using Shear Thinning Fluids: Experiments and Numerical Simulations."Environmental Processes 1(4):331-351. doi:10.1007/s40710-014-0031-9
Authors: 
M Oostrom
MJ Truex
VR Vermeul
L Zhong
GD Tartakovsky
TW Wietsma
Instruments: 
Volume: 
1
Issue: 
4
Pages: 
331-351
Publication year: 
2014

Investigation of U(VI) Adsorption in Quartz-Chlorite Mineral Mixtures.

Abstract: 

A batch and cryogenic laser-induced time-resolved fluorescence spectroscopy investigation of U(VI) adsorbed on quartz-chlorite mixtures with variable mass ratios have been performed under field-relevant uranium concentrations (5x10-7 M and 5x10-6 M) in pH 8.1 synthetic groundwater. The U(VI) adsorption Kd values steadily increased as the mass fraction of chlorite increased, indicating preferential sorption to chlorite. For all mineral mixtures, U(VI) adsorption Kd values were lower than that calculated from the assumption of component additivity; The largest deviation occurred when the mass fractions of the two minerals were equal. U(VI) adsorbed on quartz and chlorite displayed characteristic individual fluorescence spectra that were not affected by mineral mixing. The spectra of U(VI) adsorbed within the mixtures could be simulated by one surface U(VI) species on quartz and two on chlorite. The fluorescence intensity decreased in a nonlinear manner as the adsorbed U(VI) concentration increased with increasing chlorite mass fraction – likely due to ill-defined fluorescence quenching by both structural Fe/Cr in chlorite, and trace amounts of solubilized and re-precipitated Fe/Cr in the aqueous phase. However, the fractional spectral intensities of U(VI) adsorbed on quartz and chlorite followed the same trend of fractional adsorbed U(VI) concentration in each mineral phase; approximate linear correlations in the quartz:chlorite mass ratio ranges of 0.0 - 0.2 and 0.2 - 1.0, offering a method to estimate of U(VI) concentration distribution between the mineral components.

Citation: 
Wang Z, JM Zachara, J Shang, C Jeon, J Liu, and C Liu.2014."Investigation of U(VI) Adsorption in Quartz-Chlorite Mineral Mixtures."Environmental Science & Technology 48(14):7766-7773. doi:10.1021/es500537g
Authors: 
Z Wang
JM Zachara
J Shang
C Jeon
J Liu
C Liu
Volume: 
48
Issue: 
14
Pages: 
7766-7773
Publication year: 
2014

Low-temperature lithium diffusion in simulated high-level boroaluminosilicate nuclear waste glasses.

Abstract: 

Ion exchange is recognized as an integral, if underrepresented, mechanism influencing glass corrosion. However, due to the formation of various alteration layers in the presence of water, it is difficult to conclusively deconvolute the mechanisms of ion exchange from other processes occurring simultaneously during corrosion. In this work, an operationally inert non-aqueous solution was used as an alkali source material to isolate ion exchange and study the solid-state diffusion of lithium. Specifically, the experiments involved contacting glass coupons relevant to the immobilization of high-level nuclear waste, SON68 and CJ-6, which contained Li in natural isotope abundance, with a non-aqueous solution of 6LiCl dissolved in dimethyl sulfoxide at 90 °C for various time periods. The depth profiles of major elements in the glass coupons were measured using time-of-flight secondary ion mass spectrometry (ToF-SIMS). Lithium interdiffusion coefficients, DLi, were then calculated based on the measured depth profiles. The results indicate that the penetration of 6Li is rapid in both glasses with the simplified CJ-6 glass (D6Li ≈ 4.0-8.0 × 10-21 m2/s) exhibiting faster exchange than the more complex SON68 glass (D6Li ≈ 2.0-4.0 × 10-21 m2/s). Additionally, sodium ions present in the glass were observed to participate in ion exchange reactions; however, different diffusion coefficients were necessary to fit the diffusion profiles of the two alkali ions. Implications of the diffusion coefficients obtained in the absence of alteration layers to the long-term performance of nuclear waste glasses in a geological repository system are also discussed.

Citation: 
Neeway JJ, SN Kerisit, S Gin, Z Wang, Z Zhu, and JV Ryan.2014."Low-temperature lithium diffusion in simulated high-level boroaluminosilicate nuclear waste glasses."Journal of Non-crystalline Solids 405:83-90. doi:10.1016/j.jnoncrysol.2014.08.053
Authors: 
JJ Neeway
SN Kerisit
S Gin
Z Wang
Z Zhu
JV Ryan
Volume: 
Issue: 
Pages: 
Publication year: 
2014

Measuring Spatial Variability of Vapor Flux to Characterize Vadose-zone VOC Sources: Flow-cell Experiments.

Abstract: 

A method termed vapor-phase tomography has recently been proposed to characterize the distribution of volatile organic contaminant mass in vadose-zone source areas, and to measure associated three-dimensional distributions of local contaminant mass discharge. The method is based on measuring the spatial variability of vapor flux, and thus inherent to its effectiveness is the premise that the magnitudes and temporal variability of vapor concentrations measured at different monitoring points within the interrogated area will be a function of the geospatial positions of the points relative to the source location. A series of flow-cell experiments was conducted to evaluate this premise. A well-defined source zone was created by injection and extraction of a non-reactive gas (SF6). Spatial and temporal concentration distributions obtained from the tests were compared to simulations produced with a mathematical model describing advective and diffusive transport. Tests were conducted to characterize both areal and vertical components of the application. Decreases in concentration over time were observed for monitoring points located on the opposite side of the source zone from the local–extraction point, whereas increases were observed for monitoring points located between the local–extraction point and the source zone. The results illustrate that comparison of temporal concentration profiles obtained at various monitoring points gives a general indication of the source location with respect to the extraction and monitoring points.

Citation: 
Mainhagu J, C Morrison, MJ Truex, M Oostrom, and M Brusseau.2014."Measuring Spatial Variability of Vapor Flux to Characterize Vadose-zone VOC Sources: Flow-cell Experiments."Journal of Contaminant Hydrology 167:32-43. doi:10.1016/j.jconhyd.2014.07.007
Authors: 
J Mainhagu
C Morrison
MJ Truex
M Oostrom
M Brusseau
Volume: 
Issue: 
Pages: 
Publication year: 
2014

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