Browsing by Author "Seymour, Joseph D."

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Anomalous fluid transport in porous media induced by biofilm growth
(2004-11) Seymour, Joseph D.; Gage, Justin P.; Codd, Sarah L.; Gerlach, Robin
Magnetic resonance measurements of the transition from normal to anomalous hydrodynamic dispersion in porous media due to biological activity are presented. Fractional advection-diffusion equations are shown to provide models for the measured impact of biofilm growth on porous media transport dynamics.
Anomalous preasymptotic colloid transport by hydrodynamic dispersion in microfluidic capillary flow
(2014-07) Fridjonsson, E. O.; Seymour, Joseph D.; Codd, Sarah L.
The anomalous preasymptotic transport of colloids in a microfluidic capillary flow due to hydrodynamic dispersion is measured by noninvasive nuclear magnetic resonance (NMR). The data indicate a reduced scaling of mean squared displacement with time from the âŒ©z(t)^{2}âŒª_{c}âˆ¼t^{3} behavior for the interaction of a normal diffusion process with a simple shear flow. This nonequilibrium steady-state system is shown to be modeled by a continuous time random walk (CTRW) on a moving fluid. The full propagator of the motion is measured by NMR, providing verification of the assumption of Gaussian jump length distributions in the CTRW model. The connection of the data to microrheology measurements by NMR, in which every particle in a suspension contributes information, is established.
Application of PFG-NMR to study the impact of colloidal deposition on hydrodynamic dispersion in a porous medium
(2014-05) Fridjonsson, E. O.; Codd, Sarah L.; Seymour, Joseph D.
Colloidal particulate deposition affects the performance of industrial equipment, reverse osmosis membranes and sub-surface contaminant transport. Nuclear magnetic resonance (NMR) techniques, i.e. diffusion, diffraction and velocity imaging, are used to study the effect deposited colloidal particulate have on the fluid dynamics of water inside a model porous medium. Specially prepared oil-filled hard-sphere particles allow monitoring of particulate accumulation via NMR spectroscopy. Evidence of preferential spatial deposition is observed after the initial colloidal particulate deposition. Loss of spatial homogeneity is observed through NMR diffraction, while observations of the probability distributions of displacement (propagators) indicate the formation of back-bone type flow. This paper presents unique dynamic NMR data for the non-invasive non-destructive investigation of fluid transport in opaque porous media experiencing colloidal deposition.
Beyond the Surface: Non-Invasive Low-Field NMR Analysis of Microbially-Induced Calcium Carbonate Precipitation in Shale Fractures
(Springer Science and Business Media LLC, 2024-07) Willett, Matthew R.; Bedey, Kayla; Crandall, Dustin; Seymour, Joseph D.; Rutqvist, Jonny; Cunningham, Alfred B.; Phillips, Adrienne J.; Kirkland, Catherine M.
Microbially-induced calcium carbonate precipitation (MICP) is a biological process in which microbially-produced urease enzymes convert urea and calcium into solid calcium carbonate (CaCO3) deposits. MICP has been demonstrated to reduce permeability in shale fractures under elevated pressures, raising the possibility of applying this technology to enhance shale reservoir storage safety. For this and other applications to become a reality, non-invasive tools are needed to determine how effectively MICP seals shale fractures at subsurface temperatures. In this study, two different MICP strategies were tested on 2.54 cm diameter and 5.08 cm long shale cores with a single fracture at 60 ℃. Flow-through, pulsed-flow MICP-treatment was repeatedly applied to Marcellus shale fractures with and without sand (“proppant”) until reaching approximately four orders of magnitude reduction in apparent permeability, while a single application of polymer-based “immersion” MICP-treatment was applied to an Eagle Ford shale fracture with proppant. Low-field nuclear magnetic resonance (LF-NMR) and X-Ray computed microtomography (micro-CT) techniques were used to assess the degree of biomineralization. With the flow-through approach, these tools revealed that while CaCO3 precipitation occurred throughout the fracture, there was preferential precipitation around proppant. Without proppant, the same approach led to premature sealing at the inlet side of the core. In contrast, immersion MICP-treatment sealed off the fracture edges and showed less mineral precipitation overall. This study highlights the use of LF-NMR relaxometry in characterizing fracture sealing and can help guide NMR logging tools in subsurface remediation efforts.
Beyond the Surface: Non-Invasive Low-Field NMR Analysis of Microbially-Induced Calcium Carbonate Precipitation in Shale Fractures
(Springer Science and Business Media LLC, 2024-07) Willet, Matthew R.; Bedey, Kayla; Crandall, Dustin; Seymour, Joseph D.; Rutqvist, Jonny; Cunningham, Alfred B.; Phillips, Adrienne J.; Kirkland, Catherine M.
Microbially-induced calcium carbonate precipitation (MICP) is a biological process in which microbially-produced urease enzymes convert urea and calcium into solid calcium carbonate (CaCO3) deposits. MICP has been demonstrated to reduce permeability in shale fractures under elevated pressures, raising the possibility of applying this technology to enhance shale reservoir storage safety. For this and other applications to become a reality, non-invasive tools are needed to determine how effectively MICP seals shale fractures at subsurface temperatures. In this study, two different MICP strategies were tested on 2.54 cm diameter and 5.08 cm long shale cores with a single fracture at 60 ℃. Flow-through, pulsed-flow MICP-treatment was repeatedly applied to Marcellus shale fractures with and without sand (“proppant”) until reaching approximately four orders of magnitude reduction in apparent permeability, while a single application of polymer-based “immersion” MICP-treatment was applied to an Eagle Ford shale fracture with proppant. Low-field nuclear magnetic resonance (LF-NMR) and X-Ray computed microtomography (micro-CT) techniques were used to assess the degree of biomineralization. With the flow-through approach, these tools revealed that while CaCO3 precipitation occurred throughout the fracture, there was preferential precipitation around proppant. Without proppant, the same approach led to premature sealing at the inlet side of the core. In contrast, immersion MICP-treatment sealed off the fracture edges and showed less mineral precipitation overall. This study highlights the use of LF-NMR relaxometry in characterizing fracture sealing and can help guide NMR logging tools in subsurface remediation efforts.
Biofilm detection in a model well-bore environment using low-field magnetic resonance
(2015-09) Kirkland, Catherine M.; Hiebert, Dwight Randall; Phillips, Adrienne J.; Grunewald, Elliot; Walsh, David O.; Seymour, Joseph D.; Codd, Sarah L.
This research addresses the challenges of the lack of non-invasive methods and poor spatiotemporal resolution associated with monitoring biogeochemical activity central to bioremediation of subsurface contaminants. Remediation efforts often include growth of biofilm to contain or degrade chemical contaminants, such as nitrates, hydrocarbons, heavy metals, and some chlorinated solvents. Previous research indicates that nuclear magnetic resonance (NMR) is sensitive to the biogeochemical processes of biofilm accumulation. The current research focuses on developing methods to use low-cost NMR technology to support in situ monitoring of biofilm growth and geochemical remediation processes in the subsurface. Biofilm was grown in a lab-scale radial flow bioreactor designed to model the near wellbore subsurface environment. The Vista Clara Javelin NMR logging device, a slim down-the-borehole probe, collected NMR measurements over the course of eight days while biofilm was cultivated in the sand-packed reactor. Measured NMR mean log T2 relaxation times decreased from approximately 710 to 389 ms, indicating that the pore environment and bulk fluid properties were changing due to biofilm growth. Destructive sampling employing drop plate microbial population analysis and scanning electron and stereoscopic microscopy confirmed biofilm formation. Our findings demonstrate that the NMR logging tool can detect small to moderate changes in T2 distribution associated with environmentally relevant quantities of biofilm in quartz sand.
Biopolymer and water dynamics in microbial biofilm extracellular polymeric substance
(2008-09) Hornemann, Jennifer A.; Lysova, Anna A.; Codd, Sarah L.; Seymour, Joseph D.; Busse, S.; Stewart, Philip S.; Brown, Jennifer R.
Nuclear magnetic resonance (NMR) is a noninvasive and nondestructive tool able to access several observable quantities in biofilms such as chemical composition, diffusion, and macroscale structure and transport. Pulsed gradient spin echo (PGSE) NMR techniques were used to measure spectrally resolved biomacromolecular diffusion in biofilm biomass, extending previous research on spectrally resolved diffusion in biofilms. The dominant free water signal was nulled using an inversion recovery modification of the traditional PGSE technique in which the signal from free water is minimized in order to view the spectra of components such as the rotationally mobile carbohydrates, DNA, and proteins. Diffusion data for the major constituents obtained from each of these spectral peaks demonstrate that the biomass of the biofilm contains both a fast and slow diffusion component. The dependence of diffusion on antimicrobial and environmental challenges suggests the polymer molecular dynamics measured by NMR are a sensitive indicator of biofilm function.
Characterization and quantification of structure and flow in multichannel polymer membranes by MRI
(2019-01) Schuhmann, S.; Simkins, Jeffrey W.; Schork, N.; Codd, Sarah L.; Seymour, Joseph D.; Heijnen, M.; Saravia, F.; Horn, H.; Nirschl, H.; Guthausen, G.
Polymeric multichannel hollow fiber membranes were developed to reduce fiber breakage and to increase the volume-to-membrane-surface ratio and consequently the efficiency of filtration processes. These membranes are commonly used in ultrafiltration and are operated in in-out dead-end mode. However, some of the filtration details are unknown. The filtration efficiency and flow in the multichannel membranes depend on filtration time and are expected to vary along spatial coordinates. In the current work, in-situ magnetic resonance imaging was used to answer these questions. Velocities were quantified in the feed channels to obtain a detailed understanding of the filtration process. Flow and deposits were measured in each of the seven channels during filtration of sodium alginate, which is a model substance for extracellular polymeric substances occurring in water treatment. Volume flow and flow profiles were calculated from phase contrast flow images. The flow in z-direction in the center channel was higher than in the surrounding channels. Flow profiles variate depending on the concentration of Ca2+, which changes the filtration mechanism of aqueous solutions of sodium alginate from concentration polarization to gel layer filtration.
Characterization of velocity fluctuations and the transition from transient to steady state shear banding with and without pre-shear in a wormlike micelle solution under shear startup by Rheo-NMR
(2020-04) Al-kaby, Rehab N.; Codd, Sarah L.; Seymour, Joseph D.; Brown, Jennifer R.
Rheo-NMR velocimetry was used to study shear banding of a 6 wt.% cetylpyridinium chloride (CPCl) worm-like micelle solution under shear startup conditions with and without pre-shear. 1D velocity profiles across the fluid gap of a concentric cylinder Couette shear cell were measured every 1 s following shear startup for four different applied shear rates within the stress plateau. Fitting of the velocity profiles allowed calculation of the shear banding characteristics (shear rates in the high and low shear band, the interface position and apparent slip at the inner rotating wall) as the flow transitioned from transient to steady state regimes. Characteristic timescales to reach steady state were obtained and found to be similar for all shear banding characteristics. Timescales decreased with increasing applied shear rate. Large temporal fluctuations with time were also observed and Fourier transform of the time and velocity autocorrelation functions quantified the fluctuation frequencies. Frequencies corresponded to the elastically driven hydrodynamic instabilities, i.e. vortices, that are known to occur in the unstable high shear band and were dependent upon both applied shear rate and the pre-shear protocol.
Characterizing the structure of aerobic granular sludge using ultra-high field magnetic resonance
(IWA Publishing, 2020-08) Kirkland, Catherine M.; Krug, Julia R.; Vergeldt, Frank J.; van den Berg, Lenno; Velders, Aldrik H.; Seymour, Joseph D.; Codd, Sarah L.; Van As, Henk; de Kreuk, Merle K.
Despite aerobic granular sludge wastewater treatment plants operating around the world, our understanding of internal granule structure and its relation to treatment efficiency remains limited. This can be attributed in part to the drawbacks of time-consuming, labor-intensive, and invasive microscopy protocols which effectively restrict samples sizes and may introduce artefacts. Timedomain nuclear magnetic resonance (NMR) allows non-invasive measurements which describe internal structural features of opaque, complex materials like biofilms. NMR was used to image aerobic granules collected from five full-scale wastewater treatment plants in the Netherlands and United States, as well as laboratory granules and control beads. T1 and T2 relaxation-weighted images reveal heterogeneous structures that include high- and low-density biofilm regions, waterlike voids, and solid-like inclusions. Channels larger than approximately 50 μm and connected to the bulk fluid were not visible. Both cluster and ring-like structures were observed with each granule source having a characteristic structural type. These structures, and their NMR relaxation behavior, were stable over several months of storage. These observations reveal the complex structures within aerobic granules from a range of sources and highlight the need for non-invasive characterization methods like NMR to be applied in the ongoing effort to correlate structure and function.
Colloid particle transport in a microcapillary: NMR study of particle and suspending fluid dynamics
(2016-10) Fridjonsson, E. O.; Seymour, Joseph D.
Precise manipulation of the hydrodynamic interaction between particles is particularly important for operation of microfluidic devices. Shear-induced migration gives rise to dynamical patterns within the flow that have been observed in a range of systems. In this work NMR ‘active’ colloidal particles (a=1.25 µm) at volume fraction of 22% in an aqueous phase are flowed through a µ-capillary (R=126 µm) and the transport dynamics of the particle and suspending fluid phases are studied using dynamic NMR techniques. Simultaneous interrogation of shear rheology of the suspending fluid and particle phases of colloidal suspensions is presented. The dynamic behavior of the suspending fluid is shown to carry within it information about the structure of the colloidal particle ensembles on the time scales investigated (Δ=25 ms→250 ms) providing rich experimental data for further investigation and model verification. The importance of determining the particle concentration profile within μ-capillaries is explicitly demonstrated as shear induced migration causes significant concentration gradients to occur at strong flow conditions (i.e. Pep=270).
Detection of biological uranium reduction using magnetic resonance
(2012-04) Vogt, Sarah J.; Stewart, B. D.; Seymour, Joseph D.; Peyton, Brent M.; Codd, Sarah L.
The conversion of soluble uranyl ions (UO22+) by bacterial reduction to sparingly soluble uraninite (UO2(s)) is being studied as a way of immobilizing subsurface uranium contamination. Under anaerobic conditions, several known types of bacteria including iron and sulfate reducing bacteria have been shown to reduce U (VI) to U (IV). Experiments using a suspension of uraninite (UO2(s)) particles produced by Shewanella putrefaciens CN32 bacteria show a dependence of both longitudinal (T1) and transverse (T2) magnetic resonance (MR) relaxation times on the oxidation state and solubility of the uranium. Gradient echo and spin echo MR images were compared to quantify the effect caused by the magnetic field fluctuations (T*2 ) of the uraninite particles and soluble uranyl ions. Since the precipitate studied was suspended in liquid water, the effects of concentration and particle aggregation were explored. A suspension of uraninite particles was injected into a polysaccharide gel, which simulates the precipitation environment of uraninite in the extracellular biofilm matrix. A reduction in the T2 of the gel surrounding the particles was observed. Tests done in situ using three bioreactors under different mixing conditions, continuously stirred, intermittently stirred, and not stirred, showed a quantifiable T2 magnetic relaxation effect over the extent of the reaction.
Direct numerical simulation of pore-scale flow in a bead pack: Comparison with magnetic resonance imaging observations
(2013-04) Yang, Xinmin; Scheibe, T. D.; Richmond, M. C.; Perkins, W. A.; Vogt, Sarah J.; Codd, Sarah L.; Seymour, Joseph D.; McKinley, M. I.
A significant body of current research is aimed at developing methods for numerical simulation of flow and transport in porous media that explicitly resolve complex pore and solid geometries, and at utilizing such models to study the relationships between fundamental pore-scale processes and macroscopic manifestations at larger (i.e., Darcy) scales. A number of different numerical methods for pore-scale simulation have been developed, and have been extensively tested and validated for simplified geometries. However, validation of pore-scale simulations of fluid velocity for complex, three-dimensional (3D) pore geometries that are representative of natural porous media is challenging due to our limited ability to measure pore-scale velocity in such systems. Recent advances in magnetic resonance imaging (MRI) offer the opportunity to measure not only the pore geometry, but also local fluid velocities under steady-state flow conditions in 3D and with high spatial resolution. In this paper, we present a 3D velocity field measured at sub-pore resolution (tens of micrometers) over a centimeter-scale 3D domain using MRI methods. We have utilized the measured pore geometry to perform 3D simulations of Navierâ€“Stokes flow over the same domain using direct numerical simulation techniques. We present a comparison of the numerical simulation results with the measured velocity field. It is shown that the numerical results match the observed velocity patterns well overall except for a variance and small systematic scaling which can be attributed to the known experimental uncertainty in the MRI measurements. The comparisons presented here provide strong validation of the pore-scale simulation methods and new insights for interpretation of uncertainty in MRI measurements of pore-scale velocity. This study also provides a potential benchmark for future comparison of other pore-scale simulation methods. Â© 2012 Elsevier Science. All rights reserved.
Electroosmotic flow and dispersion in open and closed porous media
(2016-05) Maier, Robert S.; Nybo, Elmira; Seymour, Joseph D.; Codd, Sarah L.
Electroosmotic flow and dispersion in open and closed packed beds were investigated using Nuclear Magnetic Resonance (NMR) spectroscopy and pore-scale simulation. A series of NMR spectroscopy experiments were conducted to measure the effect of electroosmotic pressure on dispersion in packed spheres as a function of diameter and electric field strength. The experiments confirm earlier observations by others of superdiffusive transport in closed media. However, superdiffusive behavior is observed even at small pore sizes, contrary to earlier results and simulations in fixed sphere packs, and is conjectured to result from pressure-induced rearrangement of the particles. Simulations also support the existence of pore size-independent velocity distributions in closed media. The distribution of reverse velocities is also similar, apart from a difference in sign, to pressure-driven flow in open porous media.
Glass Dynamics and Domain Size in a Solvent-Polymer Weak Gel Measured by Multidimensional Magnetic Resonance Relaxometry and Diffusometry
(2019-02) Williamson, Nathan H.; Dower, April M.; Codd, Sarah L.; Broadbent, Amber L.; Gross, Dieter; Seymour, Joseph D.
Nuclear magnetic resonance measurements of rotational and translational molecular dynamics are applied to characterize the nanoscale dynamic heterogeneity of a physically cross-linked solvent-polymer system above and below the glass transition temperature. Measured rotational dynamics identify domains associated with regions of solidlike and liquidlike dynamics. Translational dynamics provide quantitative length and timescales of nanoscale heterogeneity due to polymer network cross-link density. Mean squared displacement measurements of the solvent provide microrheological characterization of the system and indicate glasslike caging dynamics both above and below the glass transition temperature.
Heterogeneous diffusion in aerobic granular sludge
(Wiley, 2020-08) van den Berg, Lenno; Kirkland, Catherine M.; Seymour, Joseph D.; Codd, Sarah L.; Van Loosdrecht, Mark C. M.; de Kreuk, Merle K.
Aerobic granular sludge (AGS) technology allows simultaneous nitrogen, phosphorus, and carbon removal in compact wastewater treatment processes. To operate, design, and model AGS reactors, it is essential to properly understand the diffusive transport within the granules. In this study, diffusive mass transfer within full‐scale and lab‐scale AGS was characterized with nuclear magnetic resonance (NMR) methods. Self‐diffusion coefficients of water inside the granules were determined with pulsed‐field gradient NMR, while the granule structure was visualized with NMR imaging. A reaction‐diffusion granule‐scale model was set up to evaluate the impact of heterogeneous diffusion on granule performance. The self‐diffusion coefficient of water in AGS was ∼70% of the self‐diffusion coefficient of free water. There was no significant difference between self‐diffusion in AGS from full‐scale treatment plants and from lab‐scale reactors. The results of the model showed that diffusional heterogeneity did not lead to a major change of flux into the granule (<1%). This study shows that differences between granular sludges and heterogeneity within granules have little impact on the kinetic properties of AGS. Thus, a relatively simple approach is sufficient to describe mass transport by diffusion into the granules.
Impact of Mineral Precipitation on Flow and Mixing in Porous Media Determined by Microcomputed Tomography and MRI
(2017-02) Bray, Joshua A.; Lauchnor, Ellen G.; Redden, George D.; Fujita, Yoshiko; Codd, Sarah L.; Seymour, Joseph D.
Precipitation reactions influence transport properties in porous media and can be coupled to advective and dispersive transport. For example, in subsurface environments, mixing of groundwater and injected solutions can induce mineral supersaturation of constituents and drive precipitation reactions. Magnetic resonance imaging (MRI) and microcomputed tomography (μ-CT) were employed as complementary techniques to evaluate advection, dispersion, and formation of precipitate in a 3D porous media flow cell. Two parallel fluids were flowed concentrically through packed glass beads under two relative flow rates with Na2CO3 and CaCl2 in the inner and outer fluids, respectively. CaCO3 became supersaturated and formed a precipitate at the mixing interface between the two solutions. Spatial maps of changing local velocity fields and dispersion in the flow cell were generated from MRI, while high resolution μ-CT imaging visualized the precipitate formed in the porous media. Formation of a precipitate minimized dispersive and advective transport between the two fluids and the shape of the precipitation front was influenced by the relative flow rates. This work demonstrates that the combined use of MRI and μ-CT can be highly complementary in the study of reactive transport processes in porous media.
Impact of Xylose on Dynamics of Water Diffusion in Mesoporous Zeolites Measured by NMR
(2021-09) Nelson, Madison L.; Romo, Joelle E.; Wettstein, Stephanie G.; Seymour, Joseph D.
Zeolites are known to be effective catalysts in biomass converting processes. Understanding the mesoporous structure and dynamics within it during such reactions is important in effectively utilizing them. Nuclear magnetic resonance (NMR) T2 relaxation and diffusion measurements, using a high-power radio frequency probe, are shown to characterize the dynamics of water in mesoporous commercially made 5A zeolite beads before and after the introduction of xylose. Xylose is the starting point in the dehydration into furfural. The results indicate xylose slightly enhances rotational mobility while it decreases translational motion through altering the permeability, K, throughout the porous structure. The measurements show xylose inhibits pure water from relocating into larger pores within the zeolite beads where it eventually is expelled from the bead itself.
Magnetic resonance analysis of capillary formation reaction front dynamics in alginate gels
(2011-09) Maneval, James E.; Bernin, D.; Fabich, H. T.; Seymour, Joseph D.; Codd, Sarah L.
The formation of heterogeneous structures in biopolymer gels is of current interest for biomedical applications and is of fundamental interest to understanding the molecular level origins of structures generated from disordered solutions by reactions. The cation-mediated physical gelation of alginate by calcium and copper is analyzed using magnetic resonance measurements of spatially resolved molecular dynamics during gel front propagation. Relaxation time and pulse-field gradient methods are applied to determine the impact of ion front motion on molecular translational dynamics. The formation of capillaries in alginate copper gels is correlated to changes in translational dynamics.
Magnetic resonance measurement of fluid dynamics and transport in tube flow of a near-critical fluid
(2014-07) Bray, J. M.; Rassi, Erik M.; Seymour, Joseph D.; Codd, Sarah L.
An ability to predict fluid dynamics and transport in supercritical fluids is essential for optimization of applications such as carbon sequestration, enhanced oil recovery, â€œgreenâ€ solvents, and supercritical coolant systems. While much has been done to model supercritical velocity distributions, experimental characterization is sparse, owing in part to a high sensitivity to perturbation by measurement probes. Magnetic resonance (MR) techniques, however, detect signal noninvasively from the fluid molecules and thereby overcome this obstacle to measurement. MR velocity maps and propagators (i.e., probability density functions of displacement) were acquired of a flowing fluid in several regimes about the critical point, providing quantitative data on the transport and fluid dynamics in the system. Hexafluoroethane (C2F6) was pumped at 0.5 ml/min in a cylindrical tube through an MR system, and propagators as well as velocity maps were measured at temperatures and pressures below, near, and above the critical values. It was observed that flow of C2F6 with thermodynamic properties far above or below the critical point had the Poiseuille flow distribution of an incompressible Newtonian fluid. Flows with thermodynamic properties near the critical point exhibit complex flow distributions impacted by buoyancy and viscous forces. The approach to steady state was also observed and found to take the longest near the critical point, but once it was reached, the dynamics were stable and reproducible. These data provide insight into the interplay between the critical phase transition thermodynamics and the fluid dynamics, which control transport processes.