Boutchko 2012
Boutchko 2012
Boutchko 2012
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
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
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
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.
(a) 5 cm (c) 5 cm
(d)
(b)
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. 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).
and “Subsurface Science Sustainable Systems" Scientific Focus areas, Perret, J., Prasher, S., Kantzas, A., Hamilton, K., Langford, C., 2000. Preferential solute
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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