Browsing by Author "Criddle, Craig S."

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Assessment of models for anaerobic biodegradation of a model bioplastic: Poly(hydroxybutyrate-co-hydroxyvalerate)
(2017-03) Ryan, Cecily A.; Billington, Sarah L.; Criddle, Craig S.
Kinetic models of anaerobic digestion (AD) are widely applied to soluble and particulate substrates, but have not been systematically evaluated for bioplastics. Here, five models are evaluated to determine their suitability for modeling of anaerobic biodegradation of the bioplastic poly(hydroxybutyrate-co-hydroxyvalerate) (PHBV): (1) first-order kinetics with and without a lag phase, (2) two-step first-order, (3) Monod (4) Contois, and (5) Gompertz. Three models that couple biomass growth with substrate hydrolysis (Monod, Contois, and Gompertz) gave the best overall fits for the data , with reasonable estimates of ultimate CH4 production. The particle size limits of these models were then evaluated. Below a particle size of 0.8 mm, rates of hydrolysis and acetogenesis exceeded rates of methanogenesis with accumulation of intermediates leading to a temporary inhibition of CH4 production. Based on model fit and simplicity, the Gompertz model is recommended for applications in which particle size is greater than 0.8 mm.
Bacterial community succession during in situ uranium bioremediation: spatial similarities along controlled flow paths
(2009-01) Hwang, Chiachi; Wu, Wei-Min; Gentry, Terry J.; Carley, Jack; Corbin, Gail A.; Carroll, Sue L.; Watson, David B.; Jardine, Phil M.; Zhou, Jizhong; Criddle, Craig S.; Fields, Matthew W.
Bacterial community succession was investigated in a field-scale subsurface reactor formed by a series of wells that received weekly ethanol additions to re-circulating groundwater. Ethanol additions stimulated denitrification, metal reduction, sulfate reduction and U(VI) reduction to sparingly soluble U(IV). Clone libraries of SSU rRNA gene sequences from groundwater samples enabled tracking of spatial and temporal changes over a 1.5-year period. Analyses showed that the communities changed in a manner consistent with geochemical variations that occurred along temporal and spatial scales. Canonical correspondence analysis revealed that the levels of nitrate, uranium, sulfide, sulfate and ethanol were strongly correlated with particular bacterial populations. As sulfate and U(VI) levels declined, sequences representative of sulfate reducers and metal reducers were detected at high levels. Ultimately, sequences associated with sulfate-reducing populations predominated, and sulfate levels declined as U(VI) remained at low levels. When engineering controls were compared with the population variation through canonical ordination, changes could be related to dissolved oxygen control and ethanol addition. The data also indicated that the indigenous populations responded differently to stimulation for bioreduction; however, the two biostimulated communities became more similar after different transitions in an idiosyncratic manner. The strong associations between particular environmental variables and certain populations provide insight into the establishment of practical and successful remediation strategies in radionuclide-contaminated environments with respect to engineering controls and microbial ecology.
Bacterial community succession during in situ uranium bioremediation: spatial similarities along controlled flow paths
(2009-01) Hwang, Chiachi; Wu, Wei-Min; Gentry, Terry J.; Carley, Jack; Corbin, Gail A.; Carroll, Sue L.; Watson, David B.; Jardine, Phil M.; Zhou, Jizhong; Criddle, Craig S.; Fields, Matthew W.
Bacterial community succession was investigated in a field-scale subsurface reactor formed by a series of wells that received weekly ethanol additions to re-circulating groundwater. Ethanol additions stimulated denitrification, metal reduction, sulfate reduction and U(VI) reduction to sparingly soluble U(IV). Clone libraries of SSU rRNA gene sequences from groundwater samples enabled tracking of spatial and temporal changes over a 1.5-year period. Analyses showed that the communities changed in a manner consistent with geochemical variations that occurred along temporal and spatial scales. Canonical correspondence analysis revealed that the levels of nitrate, uranium, sulfide, sulfate and ethanol were strongly correlated with particular bacterial populations. As sulfate and U(VI) levels declined, sequences representative of sulfate reducers and metal reducers were detected at high levels. Ultimately, sequences associated with sulfate-reducing populations predominated, and sulfate levels declined as U(VI) remained at low levels. When engineering controls were compared with the population variation through canonical ordination, changes could be related to dissolved oxygen control and ethanol addition. The data also indicated that the indigenous populations responded differently to stimulation for bioreduction; however, the two biostimulated communities became more similar after different transitions in an idiosyncratic manner. The strong associations between particular environmental variables and certain populations provide insight into the establishment of practical and successful remediation strategies in radionuclide-contaminated environments with respect to engineering controls and microbial ecology.
Biocomposite Fiber-Matrix Treatments that Enhance In-Service Performance Can Also Accelerate End-of-Life Fragmentation and Anaerobic Biodegradation to Methane
(2017-07) Ryan, Cecily A.; Billington, Sarah L.; Criddle, Craig S.
Biodegradable resins can enhance the environmental sustainability of wood-plastic composites (WPCs) by enabling methane (CH4) recovery via anaerobic digestion (AD). An under appreciated step in biocomposite AD is the role of cracking and fragmentation due to moisture uptake by the wood fiber (WF) fraction. Here, we use batch microcosms to simulate AD at end-of-life and to assess the effects of fiber-matrix treatments used to retard in-service moisture uptake. The composites evaluated were injection molded poly(hydroxybutyrate-co-hydroxyvalerate) (PHBV) with WF (0, 20%) using two fiber-matrix compatibilization treatments: (1) hydrophobic silane treatment of the wood fiber and (2) grafting of hydrophilic maleic anhydride groups to the PHBV matrix. Both treatments accelerated rates of mass loss and CH4 production by a factor of 1.2-2.3 compared to neat PHBV. The fragmentation rate, as measured by mass loss, increased significantly for treated samples compared to untreated samples. A ranking of test samples from lowest to highest rates of mass loss gave the following sequence: neat PHBV ~ maleated PHBV < PHBV plus untreated WF < maleated PHBV plus untreated WF < PHBV plus silane-treated WF. Compared to the untreated samples, maleic anhydride treatment increased the mass loss rate by 30%, and silane treatment increased the mass loss rate by 92%. Onset of cracking in silane-treated composites was observed at 2 weeks (using X-ray micro-computed tomography). At the same time, solid mass loss and CH4 production peaked, implicating cracking and physical disintegration as the rate-limiting step for accelerated anaerobic degradation. When modified to account for bioplastic matrix degradation, a previously derived moisture-induced damage model could predict the onset of composite fragmentation at end-of-life. These results are significant for design of bio-WPCs and demonstrate that treatments designed to improve in-service performance can also improve end-of-life options.
High-quality draft genome sequence of Desulfovibrio carbinoliphilus FW-101-2B, an organic acid-oxidizing sulfate-reducing bacterium isolated from uranium(VI)-contaminated groundwater
(2015-03) Ramsay, Bradley D.; Hwang, Chiachi; Woo, Hannah L.; Carroll, Sue L.; Lucas, Susan; Han, Jie; Lapidus, Alla; Cheng, J. F.; Goodwin, L. A.; Pitluck, S.; Peters, L.; Chertkov, Olga; Held, B; Detter, John C.; Han, C.; Tapia, R.; Land, M. L.; Hauser, Loren; Kyrpides, Nikos; Ivanova, N. N.; Mikhailova, Natalia; Pagani, I.; Woyke, Tanja; Arkin, Adam P.; Dehal, P.; Chivian, D.; Criddle, Craig S.; Wu, Wei-Min; Chakraborty, R.; Hazen, Terry C.; Fields, Matthew W.
Desulfovibrio carbinoliphilus subsp. oakridgensis FW-101-2B is an anaerobic, organic acid/alcohol-oxidizing, sulfate-reducing d-proteobacterium. FW-101-2B was isolated from contaminated groundwater at The Field Research Center at Oak Ridge National Lab after in situ stimulation for heavy metal-reducing conditions. The genome will help elucidate the metabolic potential of sulfate-reducing bacteria during uranium reduction.
In situ bioreduction of uranium (VI) in situ and stability of immobilized uranium: Impact of dissolved oxygen
(2007-08) Wu, Wei-Min; Carley, Jack; Luo, Jian; Ginder-Vogel, Matthew A.; Cardenas, Erick; Leigh, Mary Beth; Hwang, Chiachi; Kelly, Shelly D.; Ruan, Chuanmin; Wu, Liyou; Nostrand, Joy V.; Gentry, Terry J.; Lowe, K. A.; Mehlhorn, T. L.; Carroll, Sue L.; Luo, Wensui; Fields, Matthew W.; Gu, Baohua; Watson, David B.; Kemner, K. M.; Marsh, Terence; Tiedje, J. M.; Zhou, Jizhong; Fendorf, Scott; Kitanidis, Peter K.; Jardine, Phil M.; Criddle, Craig S.
Groundwater within Area 3 of the U.S. Department of Energy (DOE) Environmental Remediation Sciences Program (ERSP) Field Research Center at Oak Ridge, TN (ORFRC) contains up to 135 microM uranium as U(VI). Through a series of experiments at a pilot scale test facility, we explored the lower limits of groundwater U(VI) that can be achieved by in-situ biostimulation and the effects of dissolved oxygen on immobilized uranium. Weekly 2-day additions of ethanol over a 2-year period stimulated growth of denitrifying, Fe(III)-reducing, and sulfate-reducing bacteria, and immobilization of uranium as U(IV), with dissolved uranium concentrations decreasing to low levels. Following sulfite addition to remove dissolved oxygen, aqueous U(VI) concentrations fell below the U.S. Environmental Protection Agengy maximum contaminant limit (MCL) for drinking water (< 30/microg L(-1) or 0.126 microM). Under anaerobic conditions, these low concentrations were stable, even in the absence of added ethanol. However, when sulfite additions stopped, and dissolved oxygen (4.0-5.5 mg L(-1)) entered the injection well, spatially variable changes in aqueous U(VI) occurred over a 60 day period, with concentrations increasing rapidly from < 0.13 to 2.0 microM at a multilevel sampling (MLS) well located close to the injection well, but changing little at an MLS well located further away. Resumption of ethanol addition restored reduction of Fe(III), sulfate, and U(VI) within 36 h. After 2 years of ethanol addition, X-ray absorption near-edge structure spectroscopy (XANES) analyses indicated that U(IV) comprised 60-80% of the total uranium in sediment samples. Atthe completion of the project (day 1260), U concentrations in MLS wells were less than 0.1 microM. The microbial community at MLS wells with low U(VI) contained bacteria that are known to reduce uranium, including Desulfovibrio spp. and Geobacter spp., in both sediment and groundwater. The dominant Fe(III)-reducing species were Geothrix spp.
Methodology to assess end-of-life anaerobic biodegradation kinetics and methane production potential for composite materials
(2017-04) Ryan, Cecily A.; Billington, Sarah L.; Criddle, Craig S.
Composites made with bio-based resins are promising candidates for replacement of conventional plastic composites made with petroleum-based resins in many applications (e.g., decking, paneling, furniture, molded automotive parts). For any such applications, end-of-life management needs consideration. Here, we describe a methodology to assess end-of-life anaerobic degradation to methane (CH4) within landfills or anaerobic digestion (AD) facilities in batch anaerobic microcosms. The core methodology combines stoichiometric considerations, chemical oxygen demand (COD) analysis, a CH4 production assay, and modeling. Additional analyses, such as thermogravimetric analysis (TGA), can complement this core set of analyses. We apply the methodology to injection molded poly(hydroxybutyrate-co-hydroxyvalerate) (PHBV) composites with wood fiber (WF) (0%, 20%, 40%) and two fiber-matrix compatibilization treatments that enhance in-service performance: (1) hydrophobic silane treatment of the WF and (2) grafting of hydrophilic maleic anhydride groups to the PHBV matrix. The methodology successfully quantifies process kinetics, ultimate CH4 production capacity, and biodegradability, and allows comparison to reference materials (positive controls).