Matching Items (5)
Description
The use of petroleum for liquid-transportation fuels has strained the environment and caused the global crude oil reserves to diminish. Therefore, there exists a need to replace petroleum as the primary fuel derivative. Butanol is a four-carbon alcohol that can be used to effectively replace gasoline without changing the current automotive infrastructure. Additionally, butanol offers the same environmentally friendly effects as ethanol, but possess a 23% higher energy density. Clostridium acetobutylicum is an anaerobic bacterium that can ferment renewable biomass-derived sugars into butanol. However, this fermentation becomes limited by relatively low butanol concentrations (1.3% w/v), making this process uneconomical. To economically produce butanol, the in-situ product removal (ISPR) strategy is employed to the butanol fermentation. ISPR entails the removal of butanol as it is produced, effectively avoiding the toxicity limit and allowing for increased overall butanol production. This thesis explores the application of ISPR through integration of expanded-bed adsorption (EBA) with the C. acetobutylicum butanol fermentations. The goal is to enhance volumetric productivity and to develop a semi-continuous biofuel production process. The hydrophobic polymer resin adsorbent Dowex Optipore L-493 was characterized in cell-free studies to determine the impact of adsorbent mass and circulation rate on butanol loading capacity and removal rate. Additionally, the EBA column was optimized to use a superficial velocity of 9.5 cm/min and a resin fraction of 50 g/L. When EBA was applied to a fed-batch butanol fermentation performed under optimal operating conditions, a total of 25.5 g butanol was produced in 120 h, corresponding to an average yield on glucose of 18.6%. At this level, integration of EBA for in situ butanol recovered enabled the production of 33% more butanol than the control fermentation. These results are very promising for the production of butanol as a biofuel. Future work will entail the optimization of the fed-batch process for higher glucose utilization and development of a reliable butanol recovery system from the resin.
ContributorsWiehn, Michael (Author) / Nielsen, David (Thesis advisor) / Lin, Jerry (Committee member) / Lind, Mary Laura (Committee member) / Arizona State University (Publisher)
Created2013
Description
Emergent environmental issues, ever-shrinking petroleum reserves, and rising fossil fuel costs continue to spur interest in the development of sustainable biofuels from renewable feed-stocks. Meanwhile, however, the development and viability of biofuel fermentations remain limited by numerous factors such as feedback inhibition and inefficient and generally energy intensive product recovery processes. To circumvent both feedback inhibition and recovery issues, researchers have turned their attention to incorporating energy efficient separation techniques such as adsorption in in situ product recovery (ISPR) approaches. This thesis focused on the characterization of two novel adsorbents for the recovery of alcohol biofuels from model aqueous solutions. First, a hydrophobic silica aerogel was evaluated as a biofuel adsorbent through characterization of equilibrium behavior for conventional second generation biofuels (e.g., ethanol and n-butanol). Longer chain and accordingly more hydrophobic alcohols (i.e., n-butanol and 2-pentanol) were more effectively adsorbed than shorter chain alcohols (i.e., ethanol and i-propanol), suggesting a mechanism of hydrophobic adsorption. Still, the adsorbed alcohol capacity at biologically relevant conditions were low relative to other `model' biofuel adsorbents as a result of poor interfacial contact between the aqueous and sorbent. However, sorbent wettability and adsorption is greatly enhanced at high concentrations of alcohol in the aqueous. Consequently, the sorbent exhibits Type IV adsorption isotherms for all biofuels studied, which results from significant multilayer adsorption at elevated alcohol concentrations in the aqueous. Additionally, sorbent wettability significantly affects the dynamic binding efficiency within a packed adsorption column. Second, mesoporous carbons were evaluated as biofuel adsorbents through characterization of equilibrium and kinetic behavior. Variations in synthetic conditions enabled tuning of specific surface area and pore morphology of adsorbents. The adsorbed alcohol capacity increased with elevated specific surface area of the adsorbents. While their adsorption capacity is comparable to polymeric adsorbents of similar surface area, pore morphology and structure of mesoporous carbons greatly influenced adsorption rates. Multiple cycles of adsorbent regeneration rendered no impact on adsorption equilibrium or kinetics. The high chemical and thermal stability of mesoporous carbons provide potential significant advantages over other commonly examined biofuel adsorbents. Correspondingly, mesoporous carbons should be further studied for biofuel ISPR applications.
ContributorsLevario, Thomas (Author) / Nielsen, David R (Thesis advisor) / Vogt, Bryan D (Committee member) / Lind, Mary L (Committee member) / Arizona State University (Publisher)
Created2011
Description
The R-specific alcohol dehydrogenase (RADH or LVIS_0347) from Lactobacillus brevis LB19 was found to possess activity on several short chain aldehydes and ketones. This broad substrate specificity was previously uncharacterized. To demonstrate its relevance to the biofuels industry as well as its broader utility for chiral reductions, a detailed characterization was performed to further investigate the activity and function of RADH.
ContributorsHalloum, Ibrahim (Co-author) / Pugh, Shawn (Co-author) / Nielsen, David R. (Thesis director) / Rege, Kaushal (Committee member) / Barrett, The Honors College (Contributor) / Chemical Engineering Program (Contributor)
Created2015-05
Description
This document outlines the research work done by Shona Becwar in the process design and refinement for the production of sustainable butanol from Clostridium, along with the required background knowledge on the subject. The process that the microbiological organisms go through to produce butanol must be an oxygen free environment for up to 21 days with multiple perforations made into the environment in this period. There was not previously a cost effective method to do this, even in small scale. It was determined that using a butyl rubber septa would allow for the environment to be sustained during the growth process. The pervaporation process was losing butanol product at a rate of approximately 60%, changing the tubing from silicon to stainless steel allowed for a mere 7% loss during the separation process, greatly increasing the prospective of upscaling this process. These improvements to the sustainable butanol production process will allow for a more efficient, therefore more economically competitive product which can be used as a drop in equivalent to the current butanol market.
ContributorsBecwar, Shona Marie (Author) / Nielsen, David R. (Thesis director) / Staggs, Kyle (Committee member) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2016-05
Description
Chlorinated ethenes are among the most prevalent legacy contaminants affecting groundwater quality. A common treatment for chlorinated ethenes in the subsurface is in situ anaerobic bioremediation where the organohalide-respiring bacteria, Dehalococcoides mccartyi, convert the contaminants to non-toxic ethene via hydrogen (H2) dependent reductive dehalogenation. Typically, D. mccartyi obtain H2 through the fermentation of organic substrates by fermentative bacteria. However, stimulation of H2 competing processes causing production of methane (a potent greenhouse gas), rapid substrate consumption of simple substrates, and well/pore clogging by viscous complex substrates often challenge bioremediation, leading to slow rates of dehalogenation or stalls at chlorinated intermediates.This dissertation details the potential of microbial chain elongation as a technology for bioremediation of chlorinated ethenes. In chain elongation, bacteria reliably produce H2 and carboxylates (e.g., butyrate (C4)) using simple compounds (e.g., ethanol (C2) and acetate (C2)) as substrates. Under certain conditions, production of alcohols (e.g., butanol (C4)) can also occur. Here, chain elongation was demonstrated to drive reductive dehalogenation of trichloroethene via direct rapid-release H2 and slow-release H2 during fermentation of elongated products. Results showed chain elongation suppressed methanogenesis, supporting chain elongation as a potential solution for bioremediation when typical fermentable substrates do not meet treatment goals. Next, the potential for chain elongation was evaluated using groundwater and soil from a Superfund site experiencing challenges with bioremediation. Soils from the site were found to contain chain elongating bacteria, while groundwater not previously stimulated with ethanol and acetate was steered to chain elongate with bioaugmentation. Additional chain elongation substrate combinations relevant to bioremediation were identified. Results are being used to inform the design of a pilot study at the site. Lastly, this research identified and demonstrated higher ethanol concentrations, higher total pressures, and higher H2 partial pressure improves chain elongation activity and production of butanol, an important biofuel. These results aid in efforts to make chain elongation relevant as a bioprocess in a circular economy and bioremediation. Cumulatively, this dissertation research demonstrated the potential of chain elongation in bioremediation of chlorinated ethenes, indicating it should be considered when evaluating solutions for contaminated sites.
ContributorsRobles, Aide (Author) / Delgado, Anca G. (Thesis advisor) / Torres, Cesar I. (Committee member) / Bennett, Peter J. (Committee member) / Arizona State University (Publisher)
Created2023