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    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.
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    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.
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    Evaluation of the bonding properties between low-value plastic fibers treated with microbially-induced calcium carbonate precipitation and cement mortar
    (Elsevier BV, 2022-11) Espinal, Michael; Kane, Seth; Ryan, Cecily; Phillips, Adrienne J.; Heveran, Chelsea
    Plastic fiber reinforced cementitious materials offer the potential to increase the reusability of plastic waste and create lower-CO2 cementitious composites. However, the bonding properties of many plastic types with ordinary Portland cement (OPC) are largely unknown. This work employs single fiber pullout (SFPO) tests to quantify the interfacial bonding properties of polyvinyl chloride, low-density polyethylene, polypropylene, polystyrene, and acrylonitrile butadiene styrene embedded in OPC mortar. The interfacial bonding properties were compared for fibers either treated with microbially-induced calcium carbonate precipitation (MICP) or left untreated. SFPO tests revealed that plastic type had a large influence over bonding properties. Specifically, the fiber surface energy, as estimated from water contact angle measurements, was found to be the driving factor of bond strength. ABS had the highest surface energy and demonstrated the strongest bonding out of all plastic types studied. However, MICP treatment of fibers did not increase the interfacial bond strength for any of the plastics studied. The thick and inconsistent coverage of biomineral over the fiber surface from MICP is likely attributed to preventing an increase in bond strength. These results contribute to the design and application of plastic-reinforced mortars by comparing bonding properties for a range of typically low-value, unrecycled plastic types.
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    In Situ Enhancement and Isotopic Labeling of Biogenic Coalbed Methane
    (American Chemical Society, 2022-02) Barnhart, Elliott P.; Ruppert, Leslie; Hiebert, Randy; Smith, Heidi J.; Schweitzer, Hannah D.; Clark, Arthur C.; Weeks, Edwin P.; Orem, William H.; Varonka, Matthew S.; Platt, George; Shelton, Jenna L.; Davis, Katherine J.; Hyatt, Robert J.; McIntosh, Jennifer C.; Ashley, Kilian; Ono, Shuhei; Martini, Anna M.; Hackley, Keith C.; Gerlach, Robin; Spangler, Lee; Phillips, Adrienne J.; Barry, Mark; Cunningham, Alfred B.; Fields, Matthew W.
    Subsurface microbial (biogenic) methane production is an important part of the global carbon cycle that has resulted in natural gas accumulations in many coal beds worldwide. Laboratory studies suggest that complex carbon-containing nutrients (e.g., yeast or algae extract) can stimulate methane production, yet the effectiveness of these nutrients within coal beds is unknown. Here, we use downhole monitoring methods in combination with deuterated water (D2O) and a 200-liter injection of 0.1% yeast extract (YE) to stimulate and isotopically label newly generated methane. A total dissolved gas pressure sensor enabled real time gas measurements (641 days preinjection and for 478 days postinjection). Downhole samples, collected with subsurface environmental samplers, indicate that methane increased 132% above preinjection levels based on isotopic labeling from D2O, 108% based on pressure readings, and 183% based on methane measurements 266 days postinjection. Demonstrating that YE enhances biogenic coalbed methane production in situ using multiple novel measurement methods has immediate implications for other field-scale biogenic methane investigations, including in situ methods to detect and track microbial activities related to the methanogenic turnover of recalcitrant carbon in the subsurface.
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    A Numerical Model for Enzymatically Induced Calcium Carbonate Precipitation
    (MDPI, 2020-06) Hommel, Johannes; Akyel, Arda; Frieling, Zachary; Phillips, Adrienne J.; Gerlach, Robin; Cunningham, Alfred B.; Class, Holger
    Enzymatically induced calcium carbonate precipitation (EICP) is an emerging engineered mineralization method similar to others such as microbially induced calcium carbonate precipitation (MICP). EICP is advantageous compared to MICP as the enzyme is still active at conditions where microbes, e.g., Sporosarcina pasteurii, commonly used for MICP, cannot grow. Especially, EICP expands the applicability of ureolysis-induced calcium carbonate mineral precipitation to higher temperatures, enabling its use in leakage mitigation deeper in the subsurface than previously thought to be possible with MICP. A new conceptual and numerical model for EICP is presented. The model was calibrated and validated using quasi-1D column experiments designed to provide the necessary data for model calibration and can now be used to assess the potential of EICP applications for leakage mitigation and other subsurface modifications.
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    Temperature‐dependent inactivation and catalysis rates of plant‐based ureases for engineered biomineralization
    (Wiley, 2020-11) Feder, Marnie J.; Akyel, Arda; Morasko, Vincent J.; Gerlach, Robin; Phillips, Adrienne J.
    Engineered (bio)mineralization uses the enzyme urease to catalyze the hydrolysis of urea to promote carbonate mineral precipitation. The current study investigates the influence of temperature on ureolysis rate and degree of inactivation of plant-sourced ureases over a range of environmentally relevant temperatures. Batch experiments at 30◦C demonstrated that jack bean meal (JBM) has a 1.7 to 56 times higher activity (844 μmol urea hydrolyzed g−1 JBM min−1) than the other tested plant-sourced ureases (soybean, pigeon pea and cottonseed). Hence, ureolysis and enzyme inactivation rates were evaluated for JBM at temperatures between 20◦C and 80◦C. A combined first-order urea hydrolysis and first-order enzyme inactivation model described the inactivation of urease over the investigated range of temperatures. The temperature-dependent rate coefficients (kurea) increased with temperature and ranged from 0.0018 at 20◦C to 0.0249 L g−1 JBM min−1 at 80◦C; JBM urease became ≥50% inactivated in as little as 5.2 minutes at 80◦C and in as long as 2238 minutes at 50◦C. The combined urea hydrolysis kinetics and enzyme inactivation model provides a mathematical relationship useful for the design of biomineralization technologies and can be incorporated into reactive transport models
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    Biomineralization of Plastic Waste to Improve the Strength of Plastic-Reinforced Cement Mortar
    (2021-04) Kane, Seth; Thane, Abby; Espinal, Michael; Lunday, Kendra; Armagan, Hakan; Phillips, Adrienne J.; Heveran, Chelsea M.; Ryan, Cecily A.
    The development of methods to reuse large volumes of plastic waste is essential to curb the environmental impact of plastic pollution. Plastic-reinforced cementitious materials (PRCs), such as plastic-reinforced mortar (PRM), may be potential avenues to productively use large quantities of low-value plastic waste. However, poor bonding between the plastic and cement matrix reduces the strength of PRCs, limiting its viable applications. In this study, calcium carbonate biomineralization techniques were applied to coat plastic waste and improved the compressive strength of PRM. Two biomineralization treatments were examined: enzymatically induced calcium carbonate precipitation (EICP) and microbially induced calcium carbonate precipitation (MICP). MICP treatment of polyethylene terephthalate (PET) resulted in PRMs with compressive strengths similar to that of plastic-free mortar and higher than the compressive strengths of PRMs with untreated or EICP-treated PET. Based on the results of this study, MICP was used to treat hard-to-recycle types 3–7 plastic waste. No plastics investigated in this study inhibited the MICP process. PRM samples with 5% MICP-treated polyvinyl chloride (PVC) and mixed type 3–7 plastic had compressive strengths similar to plastic-free mortar. These results indicate that MICP treatment can improve PRM strength and that MICP-treated PRM shows promise as a method to reuse plastic waste.
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