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Boutchko 2012

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Journal of Applied Geophysics 76 (2012) 74–81

Contents lists available at SciVerse ScienceDirect

Journal of Applied Geophysics


journal homepage: www.elsevier.com/locate/jappgeo

Imaging and modeling of flow in porous media using clinical nuclear emission
tomography systems and computational fluid dynamics
Rostyslav Boutchko a,⁎, Vitaliy L. Rayz b, Nicholas T. Vandehey a, James P. O'Neil a, Thomas F. Budinger a,
Peter S. Nico c, Jennifer L. Druhan d, David A. Saloner b, Grant T. Gullberg a, William W. Moses a
a
Department of Radiotracer Development & Imaging Technology, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd, MS55R0121, Berkeley, CA 94720, USA
b
Department of Radiology & Biomedical Imaging, University of California, San Francisco, 505 Parnassus Avenue, M-391 San Francisco, CA 94143, USA
c
Geochemistry Department, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd, MS90R1116, Berkeley, CA 94720, USA
d
Department of Earth and Planetary Science, University of California Berkeley, 307 McCone Hall, Berkeley, CA 94710, USA

a r t i c l e i n f o a b s t r a c t

Article history: This paper presents experimental and modeling aspects of applying nuclear emission tomography to study
Received 23 May 2011 fluid flow in laboratory packed porous media columns of the type frequently used in geophysics, geochemistry
Accepted 8 October 2011 and hydrology research. Positron emission tomography (PET) and single photon emission computed tomography
Available online 17 October 2011
(SPECT) are used as non-invasive tools to obtain dynamic 3D images of radioactive tracer concentrations. Dynamic
sequences obtained using 18F-FDG PET are used to trace flow through a 5 cm diameter× 20 cm tall sand packed
Keywords:
Nuclear emission tomography
column with and without an impermeable obstacle. In addition, a custom-made rotating column setup placed
PET in a clinical two-headed SPECT camera is used to image 99mTc-DTPA tracer propagation in a through-
SPECT flowing column (10 cm diameter ×30 cm tall) packed with recovered aquifer sediments. A computational
Column flow fluid dynamics software package FLUENT is used to model the observed flow dynamics. Tracer distributions
Imaging obtained in the simulations in the smaller column uniformly packed with sand and in the column with an obstacle
are remarkably similar to the reconstructed images in the PET experiments. SPECT results demonstrate strongly
non-uniform flow patterns for the larger column slurry-packed with sub-surface sediment and slow upward
flow. In the numerical simulation of the SPECT study, two symmetric channels with increased permeability are
prescribed along the column walls, which result in the emergence of two well-defined preferential flow paths.
Methods and results of this work provide new opportunities in hydrologic and biogeochemical research. The
primary target application for developed technologies is non-destructive, non-perturbing, quantitative imag-
ing of flow dynamics within laboratory scale porous media systems.
Published by Elsevier B.V.

1. Introduction paths or 3D flow vector fields are all important and complex parameters
to constrain. In order to preserve the integrity of the on-going experiment,
Sediment columns are commonly used as experimental tools in non-invasive methods of evaluating these parameters are preferred, for
geochemistry, geophysics, hydrology and similar fields. The sediment which tomographic imaging (X-ray, optical, magnetic resonance, nuclear
is placed in a column and observed for an extended period of time emission) is well suited. A recent review of most non-invasive column
under controlled physical and chemical environment; column sizes imaging methods as well as systematically presented motivation for the
range from sub-centimeter diameter and a few centimeters length development of such methods is provided in Werth et al.(2010). In this
to tens of centimeters in diameter and a meter or more in length. In paper, we will focus on the nuclear emission tomography, which is not
a typical experiment, the column is held vertically with water directly discussed in Werth et al.(2010). Our hypothesis is that this
pumped upward through the column at rates that simulate ground- method can provide unique knowledge of the column medium parame-
water seepage flow. Adequate design, process control and interpretation ters and the tracer propagation geometry, which is not always accessible
of the results of such an experiment greatly benefit from having using other column imaging technologies.
knowledge of the internal configuration of the column material and Tomographic nuclear emission imaging methods include positron
compounds pumped through it. Porosity distribution, chemical proper- emission tomography (PET) and single photon emission computed
ties, content of contaminant-reducing materials, geometry of flow tomography (SPECT). Both methods have been actively used in medi-
cine and non-medical applications for several decades. As a result, the
equipment and expertise are both commercially available and already
⁎ Corresponding author. Tel.: + 1 510 4864858. exist at many research universities and institutions, opening a way to
E-mail address: rbuchko@lbl.gov (R. Boutchko). wide spread application of these techniques in the earth sciences. In

0926-9851/$ – see front matter. Published by Elsevier B.V.


doi:10.1016/j.jappgeo.2011.10.003
R. Boutchko et al. / Journal of Applied Geophysics 76 (2012) 74–81 75

both modalities, the three-dimensional distribution of radioactive trac- column research. Section 2 describes the column set-up and the imaging
er concentration within an object of interest is measured. Spatial resolu- experiments, Section 3 describes the computational modeling details,
tion of these techniques varies from 3 to 10 mm when scanning Section 4 presents the imaging and modeling results for flow in similar
patients to less than a millimeter in small animal imaging. In dynamic systems, and Section 5 discusses the advantages and limitations of the
PET or SPECT, a series of 3D distributions are obtained, forming a 4D presented methods for geosciences applications.
dataset of activity concentration as a function of position and time.
PET and SPECT differ by the types of radioisotopes used and by the ap- 2. Materials and methods
proach to data acquisition. The common features of the two techniques
are their non-invasive nature, robustness and extremely high sensitivi- 2.1. Nuclear emission tomography
ty: pico- and femtomolar concentrations of radioactive materials can
provide sufficient amounts of tracer activity to obtain useful imaging in- Below, we list some of the basic facts about nuclear emission
formation without altering the dominate geochemical conditions tomography necessary for understanding our work. A proper introduc-
within the experiment (Cherry et al., 2003; Wernick and Aarsvold, tion to the field is available in Wernick and Aarsvold(2004) and Cherry
2004). et al.(2003). Perret et al.(2000) also gives a simple description of SPECT
PET has been used to study sediment columns and similar objects technology.
since the 1990s. Degueldre et al.(1996) and Maguire et al.(1997)
applied PET to the study of rock samples, Hoff et al.(1996) – to • In both PET and SPECT, a radioactive tracer is injected into the studied
the study of the internal properties of construction materials, and specimen. Gamma-ray detectors of the scanner measure the intensity
Khalili et al.(1998) – to visualize flow in porous sediments. More re- of radiation emitted by radioactive decay or the tracer. The two
cently, a large body of PET research of the transport of water and salt so- modalities differ by the type of radioactivity and by the detection
lutions in geomaterials was presented by a group in Leipzig, Germany geometry. Basic principles of the scanning set-up and geometry
(Gründig et al., 2007; Kulenkampff et al., 2008; Richter et al., 2005). are shown in Fig. 1.
Since flow velocities studied in hydrogeological experiments are low, • The objective of nuclear emission tomography is to compute the
10− 4 cm/s or less, the flow residence time in a typical column is of image, an intensity distribution of radioactive decay; it is proportional
the order of hours to days. At these time scales, some of the common to the radiotracer concentration distribution v(x, y, z).
PET radioisotopes are not usable because of their short half-lives (15O: • Mathematically, nuclear emission tomography solves the inverse
t1/2 ≈2 min, 13N: t1/2 ≈10 min, 11C: t1/2 ≈20 min). Most of the studies problem of finding an unknown discrete vn from a set of measured
cited above use 18F (t1/2 ≈110 min), and some also use 64Cu (t1/ projections. Each projection Pm is a Poisson random variable, its
mean P~ m given by
124
2 ≈12.7 h) or I (t1/2 ≈4.2 days).
In comparison to positron emission tomography, SPECT imaging of
sediment columns is scarcely reported. One possible explanation for P~ m ¼ ∑ Smn vn ; ð1Þ
this fact is that neither PET nor SPECT geometries are convenient for n
the task of imaging columns. A standard arrangement for a column
is vertical, while the gantry bores of clinical SPECT and PET scanners where the system matrix Smn is calculated based on the imaging
are typically horizontal. Also, uninterrupted upward flow of water modality and configuration of the system. For a fixed m, the sum
or tracer solution is expected, while SPECT acquisition implies that (1) can usually be approximated by a weighted line integral of v.
the contrast distribution within the field of view does not change while • There are several well-studied algorithms of image reconstruction,
the gantry rotates around the imaged object to acquire the projection including analytical and iterative methods. In this work, we use
data. Perret et al.(2000) reconstructed tomographic images of soil statistical reconstruction methods that are proven to provide a
columns, but horizontal column positioning was used and the flow good model of the physics of image generation and acquisition.
was interrupted during image acquisition. Lear et al.(2010) studied
vertical columns using a SPECT camera as a simple gamma camera 2.2. Experiments A and B: small column studies using PET
acquiring only planar projection images rather than 3D distributions.
In addition, Lear used a redox-sensitive, non-conservative tracer In Experiments A and B, a 5 × 20 cm (diameter × length) glass column
designed to image redox conditions as opposed to flow dynamics. was studied using 18F-fluorodeoxyglucose (18F-FDG) PET.
Overall, application of true tomographic capabilities of SPECT to
study 3D flow fields and 4D contaminant distributions in soils and 2.2.1. Experimental set-up
sediments largely remains an unexplored field. The diagram of the setup is provided in Fig. 2. In Experiment A,
Given a 4D dataset, another major challenge in the practical approximately 75% of the length of the column was slurry-packed
implementation of the nuclear imaging methods to study flow in with lab-grade quartzite sand, the remaining portion occupied by
sediment columns is relating the 4D radiotracer distribution in the the column plumbing components. This arrangement assured minimal
column to the fluid flow field and sediment attributes such as porosity interaction between radiotracer and the column material, giving the
and permeability. In order to establish a connection between the radio- best experimental approximation to the uniform porous medium. In
tracer distribution data and the water flow, we construct a computational Experiment B, the column was re-packed with a 12.5 × 25 mm
fluid dynamics (CFD) model of the system based on the basic laws of fluid (diameter × height) solid nylon cylinder inserted in the center of
dynamics and a model of a sediment-filled column as a column of porous the column, in-line with the longitudinal axis, 10 cm from the
medium. Parameters describing the medium (sediment) such as entrance frit. The goal of this modification was to study the uniform
porosity, permeability and diffusivity can be adjusted to achieve the flow around an impermeable object. The column was rigidly
same tracer distribution for different time frames as observed experi- mounted in a vertical position in the center of the PET gantry. Tap
mentally. Radiotracer propagation can be simulated using “virtual water was pumped through the column at a constant flow rate of
ink”, a method of modeling non-reactive contrast agents previously 0.5 ml/min using a peristaltic pump through 1-mm inner diameter
applied to visualize blood flow in cerebral aneurysms (Rayz et al., 2010). tubing.
The goal of this paper is to describe a successful implementation of
nuclear emission imaging methods to the study of fluid flow in sediments, 2.2.2. Imaging
to compare the imaging experiments and CFD models of flow in porous The columns were imaged on a Siemens ECAT HR PET scanner. In
medium, and to outline how these methods can be applied in sediment Experiment A, concentrated activity, 2.6 mCi (96.2 MBq, 10 − 9 mol),
76 R. Boutchko et al. / Journal of Applied Geophysics 76 (2012) 74–81

(a) filtered backprojection (FBP) with corrections made for attenuation,


detector crystal parallel hole 2nd detector histogramed projections randoms, and scatter. For each dynamic frame, 47 slices with thickness
collimator for a single gantry angle
PMTs one projection of 3.13 mm were reconstructed with an in-plane pixel size of 2.2 mm.
element Pm Experiment B data were reconstructed using the ML-EM algorithm
parallel ray with the appropriate corrections.
collimation
decay
events
2.2.3. Velocity analysis
In order to estimate cross-sectional velocity distribution in the
column, the following analysis tool was applied to the dynamic
50 cm

image frames. Image intensity representing the tracer concentration


was denoted as f(x, y, z, t). Pixels of the column cross-section were
indexed, and then for each pixel n with coordinates (xn, yn) and for
one imaged
slice each time frame t, the instantaneous position of the tracer bolus was
gantry or other detectors and other rotationangles, defined as
specimen rotation usually, every 3-6° for each detector head

zn ðt Þ ¼ argmax f ðxn ; yn ; z; t Þ ð2Þ


(b) z

rings of detector elements detector ring, axial view


imaged object and
its axial slice + decay, The slope of zn(t) is proportional to the longitudinal component of
positrons the flow velocity at cross-sectional pixel n.
annihilate
emitting
a pair of 2.3. Experiment C: larger column studied using SPECT
511 keV
50 cm

photons
In Experiment C, a 10× 30 cm quartz glass column packed with re-
511 keV covered field materials was imaged using 99mTc-DTPA dynamic SPECT.
photons,
single coincidence
detector, detection 2.3.1. Experimental set-up
crystal+PMTs lines
The diagram of the setup is provided in Fig. 3. The column was
slurry-packed with sediment from the DOE Integrated Field Research
Fig. 1. General scheme of using (a) single photon emission computed tomography
(SPECT) and (b) positron emission tomography (PET) to image a column-shaped object. Site (IFRC) in Rifle, Colorado (Anderson et al., 2003; Williams et al.,
Radiation detectors consisting of scintillation crystals and photomultiplier tubes (PMTs) 2009) and mounted on a custom designed rotating stage in a vertical
measure γ-rays emitted either directly in SPECT or indirectly through positron recom- position. Vertical positioning, as opposed to horizontal, is expected to
bination in PET. reduce preferential flow channels and flow fingering and to allow
escape of any gases formed during reactive flow. The column was
placed between the detector heads of GE VG3 Millennium SPECT-
1 ml, was injected as a bolus at the column inlet, corresponding to a CT camera. The column was rotated about its vertical axis by a
delta-like input function (time-dependence of the activity concentration computer-controlled stepper motor. At the inlet (1 mm-diameter
at the inlet). In Experiment B, a step-function input function was used: tubing), the flow was somewhat dispersed through a star-shaped
the input was switched from water to 18F-FDG solution, 23.9 mCi pattern cut into the bottom inlet plate, which proved to provide bet-
(0.884 GBq, 10− 8 mol) in 270 ml, at a constant flow rate of 0.5 ml/min. ter dispersion than a dispersion frit. Anoxic artificial ground water
Dynamic image acquisition continued for 6 h. The acquisition frame mixed to reflect field conditions (Li et al., 2009) was pumped up
durations were the following: fifteen 20 s frames, five 60 s frames, and the column at 1.25 ml/min using a Waters 590 HPLC pump. 99mTc-
seventy 300 s frames. Experiment A data were reconstructed using 2D DTPA, 30 mCi (1.1 GBq, 60 pmol) diluted in 3 ml of groundwater,

(g)
(a)
(c)
5 cm
(d)
(b) (f)
(e)
(h)

Fig. 2. Small column PET experiment setup (Experiments A and B). Components: (a) column filled with hydrated sand, (b) insert used in Experiment B, (c) peristaltic pump,
(d) activity source, 1-ml syringe in Experiment A, 0.5 l in Experiment B, (e) three-way valve, (f) deionized tap-water tank, (g) column outlet, (h) PET gantry.
R. Boutchko et al. / Journal of Applied Geophysics 76 (2012) 74–81 77

Fig. 3. A diagram and a photograph of Experiment C. (a) Stepper-motor rotating the column, (b) stand, (c) glass column filled with Rifle site sediment, (d) outlet, (e) SPECT detector
heads, (f) sliding mounts, (g) activity delivery system with a syringe drive, (h) T-shaped connector, (i) HPLC-pump, (j) deoxygenated groundwater tank.

was delivered to the inlet line using a syringe drive at 0.1 ml/min. 3.1. Theory
During the 30-minute interval of activity delivery, the HPLC
pump rate was reduced to 1.15 ml/min, thus achieving a constant The physical variables and system parameters used to model fluid
flow rate at the inlet of 1.25 ml/min and a 30 min-wide rectangle- flow in the medium are:
shaped radiotracer input function. The testing and characterization
• U— velocity vector of the fluid;
of the 99mTc-DTPA as a conservative tracer is described elsewhere
• ρ— density of the fluid;
(Vandehey et al., submitted for publication).
• μ— viscosity of the fluid;
• γ— porosity of the medium 1;
2.3.2. Imaging
• K— permeability of the medium;
In order to obtain tomographic datasets, the column was rotated
• p— pressure (includes both applied pressure and gravity).
about its vertical axis while a dynamic planar image sequence was ac-
quired by the scanner. Image acquisition was synchronized with the step- These variables and parameters are sufficient to formulate the
per motor rotating the column so that an equivalent of a continuous- basic equations of fluid flow in the first level of approximation.
rotation sinogram was acquired. During each dynamic study, 120 projec- Second-level parameters to be considered in the future include tensor
tions (128×128 pixels, 4.42 mm pixel size) were acquired in 6 min as elements of the porosity (at this stage, we assume isotropic pores, so
the column rotated 360°. For each 6-minute acquisition, the projection γ is a scalar between 0 and 1), permeability, and chemical exchange
data acquired by both detector heads were combined, cropped and parameters. In order to describe the velocity field of the fluid, we
reshaped to form a single 28×88×120 sinogram. A total of 180 sino- use the flow continuity equation
grams were acquired every 8 min over a 24-hour period.
Each sinogram was reconstructed using 25-iterations of a standard ∇⋅ðγUÞ ¼ 0; ð3Þ
ML-EM algorithm. The ray-driven system matrix was calculated
including continuous rotation correction, divergent-ray geometric and Navier–Stokes equation for porous medium

∂ 
response correction, and attenuation correction. Since the water/
2 γμ
tracer flow was not stopped for the time of acquisition, a certain ργUÞ þ U⋅∇ ⋅ ργUÞ−μγ∇ U þ γ∇p ¼ − U: ð4Þ
∂t K
amount of motion blurring was introduced to the data. However, with
mean flow velocities (based on the flow rate) below 0.5 mm/min, the Setting γ = 1 turns the left hand side of Eq. (4) into the standard
motion blurring was expected to be within the image spatial resolution Navier–Stokes equation — the equivalent of equations of motion for
of 4.42 mm. fluid flow. The right hand side is the momentum sink term that is
Attenuation correction was realized in two stages. First, the projection responsible for the non-inertial nature of flow in porous medium.
data were adjusted to take into account attenuation by the stationary el- The density ρ is constant, assuming incompressible liquid. Generally,
ements of the column mounting setup, labelled as (f) in Fig. 2. Then, later both K and γ variables are location-dependent and coupled with
time frames of the activity distribution inside the column were recon- each other. However, since a few percent change in the porosity
structed without attenuation correction and used to build a virtual 3D can correspond to orders of magnitude change in the permeability,
column. Uniform attenuation coefficient of μ = 0.255 cm− 1 was we use K as the only variable parameter of the system at this stage.
assigned to every point inside the virtual column and used to re-
peat the reconstruction with the attenuation correction. The value 3.2. Flow modeling
of attenuation coefficient μ was measured independently by two
methods: a pre-study transmission CT scan and a measurement of the Numerical solution of Eqs. (3)−(4) is implemented using standard
attenuation of a uniform intensity 99mTc rod source. CFD software packages FLUENT and CFX (ANSYS, Inc., Canonsburg, PA,
USA). The spatial mesh for the solution is generated using Hypermesh
3. Computational modeling software (Altair Engineering, Troy, MI). Computational domains

This section explains computational fluid dynamics modeling of 1


γ denotes the area surface porosity represented as a tensor in anisotropic medium,
the water and tracer solution flow in a column. see (Neuman, 2005) for theoretical details.
78 R. Boutchko et al. / Journal of Applied Geophysics 76 (2012) 74–81

include pure fluid (inlet and outlet tubes) and porous medium (column). model of the system, hence all of the approximations are made only at
In Experiment B only, a solid domain representing an impermeable the parameter selection level.
object that partially obstructs the flow of liquid was added.
The boundary conditions for the Navier–Stokes equations were 3.4. Numerical simulations
no-slip (zero tangential and normal velocity) at the wall and uniform
velocity profile at the inlet. Initial conditions were zero velocity and Three studies were been performed to match the system and flow
pressure throughout the computational domain. A Cartesian coordinate parameters used in Experiments A, B, and C. In each of the simulations,
system was used in the CFD model (in the general case of non-uniform the width and length of the column matched that used in the experiments
permeability we could not use a symmetrical domain to reduce the described in the previous section. Inside the column, a porosity value of
computational cost). γ=0.5 and permeability value K=10− 8 m− 2 were used.

3.3. Tracer model


3.5. Experiment A: Uniform medium

A non-reacting tracer injection was simulated by using virtual ink: a


The simplest experiment was with uniform γ and K in a column
passive scalar function C assigned to each computational cell (Rayz
with no additional obstacles. This was aimed at computing the fluid
et al., 2010). The distribution of the tracer at each time step was calcu-
velocity, and the pressure distributions and characteristic tracer profile
lated by solving an advection–diffusion equation
for fluid flow in uniform porous medium. The single bolus input
function was modeled as a 4-second-wide rectangle function.
∂C 2
þ U ⋅∇C ¼ D∇ C; ð5Þ
∂t
3.6. Experiment B: Uniform medium with an obstacle
where D is the diffusion coefficient, C represents the local concentration
The goal of this experiment was to obtain the tracer propagation
of the tracer, and the steady flow velocities U are obtained from
profile for fluid flow around an impermeable object. The
Eqs. (3)−(4). Diffusion effects were neglected as being much slower
12.5 × 25 mm obstacle was modeled by modifying the computational
than the advection by setting D = 0 throughout the domain. This
mesh of the numerical study A to include a solid domain in the center
pure advection equation is identical to the level-set equation, which is
of the column. A step-function input-function was used.
widely used in numerical simulations to track the interface between
different materials (liquid–solid, liquid–gas, and liquid–liquid). Initially,
the concentration of the tracer was uniformly zero throughout the 3.7. Experiment C
domain. The value of the scalar at the inlet was set to 1 during the
injection of the tracer and zero otherwise. The time intervals of the 3.7.1. Non-uniform medium
tracer injection (input function) matched the time intervals used in The goal of this experiment was to model flow propagation in the
the experiments. As the tracer was advected through the media, the medium with non-uniform permeability and porosity. Two preferential
regions where the scalar value was 1 were filled with tracer, while flow paths were modeled by setting the permeability to K = 10− 4 m− 2
the regions where its value was zero were tracer-free. Due to the inside a 1 cm-wide region along two opposing walls of the column and
Eulerian nature (which represents the concentration C as the volume along the bottom 1 cm-wide slice of the column. The regions of
average over the control volume) of this method and a certain amount increased permeability extended along the column length with
of numerical diffusion, the value of the scalar obtained in the numerical an angular span of 0.1 rad (5.7°). A 30-minute rectangle input
solution is not always 0 or 1 but can assume values in between. The flow function was used. Nine hours of the tracer propagation were simulated.
regions with the scalar value above a certain threshold can be readily vi- A vertical cross-section image was saved to the system every 10 min of
sualized with a color coding scheme. There is a one-way coupling be- model time.
tween the Navier–Stokes and advection–diffusion equations, so the
distribution of the tracer at each time step will be computed after the 4. Results
velocity field solution is obtained, thus tracer concentration has no effect
on the velocity field. The described approach is somewhat different from Below, three imaging experiments described in Section 2 are
a more common approach to modeling flow in geophysics using Darcy's compared to the results of the corresponding numerical studies described
law. Navier–Stokes and continuity equations describe the exact physical in Section 3.

(a) 5 cm (c) 5 cm

(d)
(b)

0 0.2 0.4 0.6 0.8 1


intensity fraction (unitless)
Fig. 4. Time-ordered (left to right) longitudinal sections through the sand-filled 16 × 5 cm portion of the column in (a) imaging Experiment A, (b) numerical study A, (c) imaging
Experiment B, (d) numerical study B. Approximately the lower 80% of the column is shown in both (c) and (d). PET images are decay-corrected so the image intensity is propor-
tional to the tracer concentration. The time variables for the individual frames were selected to visually match the propagation of the tracer edge in PET and simulation image se-
quences. Since quantitative information of tracer concentration is not available at this time, proportional color scheme was selected with brightness and contrast adjusted for best
visibility of the tracer bolus.
R. Boutchko et al. / Journal of Applied Geophysics 76 (2012) 74–81 79

(a) 10 cm 4.3. Experiment C


1
2 Fig. 5 shows vertical longitudinal sections through dynamic SPECT
images and numerical simulations of flow in a medium with non-
uniform porosity. Since the preferential flow-channel positions were
selected arbitrarily prior to the study, the two image series show
significant differences. Most notably, while both preferential flow
(b) paths in the CFD simulation images are within the imaging plane,
the main flow path in the real system moves out of the imaging
plane near the bottom of the column and reenters the imaging
plane first at about 2/3 of the column length and then immediately
before the outlet. In addition, rather than the two flow paths being
identical, the flow path on the left side of the cross section in the
0 0.2 0.4 0.6 0.8 1 real system is less pronounced. Despite the fact that the system
intensity fraction (unitless) that was modeled was a highly simplified version of what is likely to
exist, it still shows many qualitative similarities to the real system.
Fig. 5. Tracer propagation in inhomogeneous medium: (a) Experiment C, longitudinal We list several essential features of tracer behavior in non-uniform
cross-sectional slices of the 10 × 30 cm column, reconstructed every 36 min. medium that are common for both image sets below:
(b) Numerical study C results, sampling times adjusted to synchronize the simulated
and experimental images. Proportional color scale adjusted for best visual comparison
between the datasets. SPECT images were decay corrected so that the image intensity
• The flow behavior near the bottom of the column is likely driven by
is proportional to the tracer concentration. Arrow 1 shows the point where the main the higher-velocity inlet jet, first creating a semi-spherical shape of
flow path enters the cross-section plane. Arrow 2 indicates a minor preferential flow the tracer distribution, and then the same-shape dark spot, as the
path. tracer input (rectangle function) is followed by tracerless water.
• A significant difference between the image series in Fig. 5 is the
visibility of the trailing edge of the contrast bolus: it is clearly visible
4.1. Experiment A
in the simulation but hardly visible in the SPECT results. The exact
nature of this effect is unclear, although it is unlikely that it is caused
Fig. 4 shows a series of intensity profiles of tracer distribution both
by chemical absorption of 99mTc-DTPA, which is shown to be a
in the PET-imaged (a) and numerically simulated (b) columns with
conservative tracer for Rifle sediments in Vandehey et al.(submitted
uniform porosity. The two image series exhibit significant similarity
for publication).
between the experimental and the simulated tracer flow in medium
• Most of the tracer transport occurs through the preferential flow
of uniform porosity porous medium, notably the inverted “V”-like
paths.
shape of the tracer distribution formed by the diverging flow geom-
• A body of the activity outside of these flow paths propagates up the
etry near the inlet, then propagated across the column with minor
column at a relatively slow rate.
deformations.
• A significant amount of flow dispersion in a visible blurring of the
image intensity (proportional to the tracer concentration), especial-
ly outside of the main flow paths.
4.2. Experiment B

Fig. 4 shows the tracer propagation profiles for PET-imaged (c)


and CFD-simulated (d) fluid flow around an impermeable object 4.4. Visualization
with a step-function tracer input function. Visual comparison of the
simulated and the measured profiles shows significant similarity, In addition to the cross-sectional slices, several other display
especially at the early time frames, before the tracer front reaches methods can be used to visualize flow paths in the column. Fig. 6
the obstacle. As the front flows around the obstacle, it develops a shows four dynamic time frames of the tracer propagation using
somewhat asymmetric shape and decreased contrast, most likely cross-sectional planes and isosurfaces. The main flow path and
caused by the asymmetric placement of the impermeable insert in the minor flow paths are clearly visible, as are the effects of tracer mixing
experimental column. with the activity-free water.

1
intensity fraction (unitless)

0.8

0.6

0.4

0.2

Fig. 6. Visualization of the tracer propagation in Experiment C, at four time points, 10 min, 1 h, 2 h and 5 h after injection. Each time frame is shown both on four cross-sectional
planes and as an isosurface computed at 1/3 of the color axis maximum.
80 R. Boutchko et al. / Journal of Applied Geophysics 76 (2012) 74–81

Intensity Maxima Coordinates for 32 Flow Lines Good qualitative agreement between the numerical studies and
distance from the bottom of the column (cm)

Experiments A and B and lack of such agreement in Experiment C


18
demonstrate the limits of computational approach based on an
16 exact model within fluid dynamics. While modeling flow in a
homogeneous medium can be used to develop and validate methods
14 of extracting material parameters of the medium from dynamic
image sequences, modeling flow in a heterogeneous system with
12 unknown medium parameter distributions (which is commonly
found in real sediment columns) is a much more complex task.
10
Exact CFD simulations are computationally intensive and time consuming
8 even for the uniform medium; introduction of non-uniform porosity and
permeability further increases the complexity of the problem and often
6 leads to instabilities in the numerical solution of the Navier–Stokes
equation. We will continue to build numerical models of flow through
4
inhomogeneous medium both using the method presented in Section 3
2 and simpler models of solute transport in medium, such as Darcy's
flow. A working flow model will allow us to calculate local porosity
0 and permeability distributions in columns from the dynamic sets of
0 50 100 150 200
PET or SPECT images.
time (min)
The most novel aspect of the presented research is the application
Fig. 7. Tracer bolus propagation lines in Experiment A calculated using Eq. (2). Parallel of SPECT to obtain 3D tracer distributions in a large vertical column
lines indicate cross-sectionally uniform velocity distribution. Converging lines at times with continuous fluid flow. This method allows continuous monitoring
less than 20 min and more than 180 min correspond to divergent flow near the inlet of technetium distribution within a column in a non-invasive manner,
and converging flow near the outlet. Insert in the lower right corner of the plot
shows arbitrarily chosen cross-sectional positions of the 32 flow lines matched against
without the need to take physical samples of the fluid or sediment
the longitudinal projection of the column intensity distribution 2.5 h after the bolus material. As mentioned in the introduction, the method is highly sensitive
injection. and allows imaging with trace amounts of the radioisotope. The total
injected technetium in Experiment C is about 60 pmol, at a concentration
of 1.5 pmol/ml. The contrast resolution in Fig. 5 is at least 2–3 nCi/pixel,
4.5. Velocity analysis which translates to the ability to resolve differences in concentration of
10− 15 mol/l at sub-centimeter length scales.
In the process of calculating the flow fields during the CFD simulation, Our future research in the area of sediment column imaging will
FLUENT software computes the velocities inside the porous domain. In focus both on improving the methodology of image acquisition and
the uniform medium case (Experiment A), the velocity field is uniform analysis, and on applying this technique to specific problems in
everywhere except for relatively small regions near the inlet and the geochemistry, geophysics, hydrology and similar fields. The most
outlet. This is a distinct feature of flow in the medium, since velocities immediate practical application of technetium imaging is to study
in the free flowing fluid in a pipe generally vary depending on the problems related to subsurface transport properties and immobilization
distance to the pipe walls. In Fig. 7 we show a plot of the maximum strategies for technetium(VII), a prevalent radioactive contaminant
intensity lines for several points within the column cross-section (Burke et al., 2005; Lear et al., 2010; Plymale et al., 2011). In particular,
for Experiment A calculated using Eq. (2). The slope of each of the column described in Experiment C is currently used in an extended
these curves corresponds to the axial (z) velocity component at a imaging study with both an active technetium(VII) tracer and a
fixed (x, y). The fact that the curves are parallel straight lines through chemically conservative tracer applied to see the effects of anoxic
most of their lengths confirms that velocity is cross-sectionally and environments and bacterial activity on technetium immobilization,
longitudinally uniform in most of the column. The value of velocity distribution of biogenic divalent iron and flow path variability.
evaluated from the plot is approximately 6.7×10− 2 cm/min. Multiplying
this value by the column cross-sectional area 2.52πcm2, we obtain flow 6. Conclusions
rate of 1.3γ ml/min, where γ is the porosity of the medium. The mea-
sured flow rate in the column is 0.5 ml/min, which gives us γ∼0.4, a re- A highly-sensitive non-invasive method of imaging sediment
alistic estimate of porosity for sand. columns using clinical PET and SPECT cameras has been developed
and compared to computer simulations of fluid flow in a porous
5. Discussion medium obtained using FLUENT software. 18F-FDG PET was used
to image small columns filled with homogeneous material. Dynamic
Experiments A and B demonstrate successful application of PET to 3D image sequences acquired using PET exhibit significant qualitative
imaging vertical columns with column sizes comparable to those similarities to simulated tracer distribution images computed for the
already reported in the literature. In nuclear emission tomography, flow in a medium with uniform porosity and permeability. A
it is generally considered that in order to obtain good images, the custom-designed experimental arrangement allowed acquisition of
width of the imaged object should correspond to five attenuation tomographic SPECT images in a vertical column with continuously
lengths or less. An attenuation length is the thickness of material upward flow of the tracer solution. Dynamic 3D sequences of 99mTc-
that reduces the intensity of the penetrating radiation by the factor DTPA distributions in the column were acquired and reconstructed,
of 1/e. For the 511 keV γ-ray, this distance of five attenuation revealing the inhomogeneous nature of the sediment. Numerical
lengths corresponds to about 50 cm for water and biological tissues simulations of tracer flow in medium with non-uniform porosity
and 25 cm for soils and sediments, implying that column diameters and permeability exhibit the same essential features of the flow as
as large as 25 cm can be imaged by PET. Thus, PET with 18F presents observed in the tomographic images. However, the significant and
a convenient method of measuring 3D distributions of tracer as it important differences between the imaged flow patterns within
propagates through the column at water seepage flow rates of even this relatively simple system using actual field materials and
10 − 2 cm/sec. Similar or slower flow rates can be studied using the modeled flow dynamics emphasize the need for non-invasive
other long half-life PET isotopes, such as 76Br, 64Cu or 124I. flow quantification in the interpretation of packed sediment column
R. Boutchko et al. / Journal of Applied Geophysics 76 (2012) 74–81 81

experiments. Such measurements allow more accurate data inter- Khalili, A., Basu, A., Pietrzyk, U., 1998. Flow visualization in porous media via Positron
Emission Tomography. Physics of Fluids 10, 1031–1033.
pretation and significantly improve the overall utility of these Kulenkampff, J., Gründig, M., Richter, M., Enzmann, F., 2008. Evaluation of positron-
types of experiments. Routine use of nuclear emission tomographic emission-tomography for visualisation of migration processes in geomaterials. MI-
techniques could address this problem and serve an important role GRATION 2007, 11th International Conference on the Chemistry and Migration Be-
haviour of Actinides and Fission Products in the Geosphere: Physics and Chemistry
within the earth sciences community. The current work presented of the Earth, Parts A/B/C, 33, pp. 937–942.
new tracer options and new column imaging apparatus in order to Lear, G., McBeth, J.M., Boothman, C., Gunning, D.J., Ellis, B.L., Lawson, R.S., Morris, K.,
help bring about that routine application. Burke, I.T., Bryan, N.D., Brown, A.P., Livens, F.R., Lloyd, J.R., 2010. Probing the bio-
geochemical behavior of technetium using a novel nuclear imaging approach. En-
vironmental Science & Technology 44, 156–162.
Acknowledgment Li, L., Steefel, C.I., Williams, K.H., Wilkins, M.J., Hubbard, S.S., 2009. Mineral transforma-
tion and biomass accumulation associated with uranium bioremediation at Rifle,
Colorado. Environmental Science & Technology 43, 5429–5435.
This work was supported by the Director, Office of Science, Office Maguire, R., Missimer, J., Emert, F., Townsend, D., Dollinger, H., Leenders, K., 1997. Pos-
of Biological and Environmental Research, Biological Systems Science itron emission tomography of large rock samples using a multiring PET instrument.
and Climate and Environmental Science Divisions of the U.S. Department IEEE Transactions on Nuclear Science 44, 26–30.
Neuman, S.P., 2005. On the tensorial nature of advective porosity. Advances in Water
of Energy under contract no. DE-AC02-05CH11231, “Radiotracer Im- Resources 28, 149–159 (Erratum to the paper is published on p. 884, same volume
aging Technologies for Plant, Microbial, and Environmental Systems" of the journal).
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flow in intact soil columns measured by SPECT scanning. Soil Science Society Of
and by National Institutes of Health grant no. K25NS059891. America Journal 64, 469–477.
Plymale, A.E., Fredrickson, J.K., Zachara, J.M., Dohnalkova, A.C., Heald, S.M., Moore, D.A.,
Kennedy, D.W., Marshall, M.J., Wang, C., Resch, C.T., Nachimuthu, P., 2011. Com-
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