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    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.
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    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.
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    Peclet number dependent superdiffusive hydrodynamic dispersion in a site percolation porous media measured by NMR
    (2017-04) Seymour, Joseph D.; Codd, Sarah L.; Kimmich, Rainer
    The displacement time dependent hydrodynamic dispersion in a model 2D site percolation structure is measured using PGSE NMR. The data indicate superdiffusive scaling of the mean squared displacement at high Peclet numbers, where advective transport dominates, consistent with classic percolation scaling concepts. The time scaling of the mean squared displacement is shown to vary with the Peclet number demonstrating a dependence on the changing dynamics.
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    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.
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    Detecting Microbially Induced Calcite Precipitation in a Model Well-Bore Using Downhole Low-Field NMR
    (2017-02) Kirkland, Catherine M.; Zanetti, Sam; Grunewald, Elliot; Walsh, David O.; Codd, Sarah L.; Phillips, Adrienne J.
    Microbially induced calcite precipitation (MICP) has been widely researched recently due to its relevance for subsurface engineering applications including sealing leakage pathways and permeability modification. These applications of MICP are inherently difficult to monitor nondestructively in time and space. Nuclear magnetic resonance (NMR) can characterize the pore size distributions, porosity, and permeability of subsurface formations. This investigation used a low-field NMR well-logging probe to monitor MICP in a sand-filled bioreactor, measuring NMR signal amplitude and T2 relaxation over an 8 day experimental period. Following inoculation with the ureolytic bacteria, Sporosarcina pasteurii, and pulsed injections of urea and calcium substrate, the NMR measured water content in the reactor decreased to 76% of its initial value. T2 relaxation distributions bifurcated from a single mode centered about approximately 650 ms into a fast decaying population (T2 less than 10 ms) and a larger population with T2 greater than 1000 ms. The combination of changes in pore volume and surface minerology accounts for the changes in the T2 distributions. Destructive sampling confirmed final porosity was approximately 88% of the original value. These results indicate the low-field NMR well-logging probe is sensitive to the physical and chemical changes caused by MICP in a laboratory bioreactor.
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