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This work focuses on a generalized assessment of source zone natural attenuation (SZNA) at chlorinated aliphatic hydrocarbon (CAH) impacted sites. Given the numbers of sites and technical challenges for cleanup there is a need for a SZNA method at CAH impacted sites. The method anticipates that decision makers will be interested in the following questions: 1-Is SZNA occurring and what processes contribute? 2-What are the current SZNA rates? 3-What are the longer-term implications? The approach is macroscopic and uses multiple lines-of-evidence. An in-depth application of the generalized non-site specific method over multiple site events, with sampling refinement approaches applied for improving SZNA estimates, at three CAH impacted sites is presented with a focus on discharge rates for four events over approximately three years (Site 1:2.9, 8.4, 4.9, 2.8kg/yr as PCE, Site 2:1.6, 2.2, 1.7, 1.1kg/y as PCE, Site 3:570, 590, 250, 240kg/y as TCE). When applying the generalized CAH-SZNA method, it is likely that different practitioners will not sample a site similarly, especially regarding sampling density on a groundwater transect. Calculation of SZNA rates is affected by contaminant spatial variability with reference to transect sampling intervals and density with variations in either resulting in different mass discharge estimates. The effects on discharge estimates from varied sampling densities and spacings were examined to develop heuristic sampling guidelines with practical site sampling densities; the guidelines aim to reduce the variability in discharge estimates due to different sampling approaches and to improve confidence in SZNA rates allowing decision-makers to place the rates in perspective and determine a course of action based on remedial goals. Finally bench scale testing was used to address longer term questions; specifically the nature and extent of source architecture. A rapid in-situ disturbance method was developed using a bench-scale apparatus. The approach allows for rapid identification of the presence of DNAPL using several common pilot scale technologies (ISCO, air-sparging, water-injection) and can identify relevant source architectural features (ganglia, pools, dissolved source). Understanding of source architecture and identification of DNAPL containing regions greatly enhances site conceptualization models, improving estimated time frames for SZNA, and possibly improving design of remedial systems.
ContributorsEkre, Ryan (Author) / Johnson, Paul Carr (Thesis advisor) / Rittmann, Bruce (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Arizona State University (Publisher)
Created2013
Description
Biofuel from microbial biomass is a viable alternative to current energy production practices that could mitigate greenhouse gas levels and reduce dependency on fossil fuels. Sustainable production of microbial biomass requires efficient utilization of nutrients like phosphorus (P). P is a limited resource which is vital for global food security. This paper seeks to understand the fate of P through biofuel production and proposes a proof-of-concept process to recover P from microbial biomass. The photosynthetic cyanobacterium Synechocystis sp. PCC 6803 is found to contain 1.4% P by dry weight. After the crude lipids are extracted for biofuel processing, 92% of the intercellular P is found within the residual biomass. Most intercellular P is associated with nucleic acids which remain within the cell after lipids are extracted. Phospholipids comprise a small percentage of cellular P. A wet chemical advanced oxidation process of adding 30% hydrogen peroxide followed by 10 min of microwave heating converts 92% of the total cellular P from organic-P and polyphosphate into orthophosphate. P was then isolated and concentrated from the complex digested matrix by use of resins. An anion exchange resin impregnated with iron nanoparticles demonstrates high affinity for P by sorbing 98% of the influent P through 20 bed volumes, but only was able to release 23% of it when regenerated. A strong base anion exchange resin sorbed 87% of the influent P through 20 bed volumes then released 50% of it upon regeneration. The overall P recovery process was able to recover 48% of the starting intercellular P into a pure and concentrated nutrient solution available for reuse. Further optimization of elution could improve P recovery, but this provides a proof-of-concept for converting residual biomass after lipid extraction to a beneficial P source.
ContributorsGifford, James McKay (Author) / Westerhoff, Paul (Thesis advisor) / Rittmann, Bruce (Committee member) / Vannela, Ravindhar (Committee member) / Arizona State University (Publisher)
Created2012
Improving cyanobacterial hydrogen production through bioprospecting of natural microbial communities
Description
Some cyanobacteria can generate hydrogen (H2) under certain physiological conditions and are considered potential agents for biohydrogen production. However, they also present low amounts of H2 production, a reaction reversal towards H2 consumption, and O2 sensitivity. Most attempts to improve H2 production have involved genetic or metabolic engineering approaches. I used a bio-prospecting approach instead to find novel strains that are naturally more apt for biohydrogen production. A set of 36, phylogenetically diverse strains isolated from terrestrial, freshwater and marine environments were probed for their potential to produce H2 from excess reductant. Two distinct patterns in H2 production were detected. Strains displaying Pattern 1, as previously known from Synechocystis sp. PCC 6803, produced H2 only temporarily, reverting to H2 consumption within a short time and after reaching only moderately high H2 concentrations. By contrast, Pattern 2 cyanobacteria, in the genera Lyngbya and Microcoleus, displayed high production rates, did not reverse the direction of the reaction and reached much higher steady-state H2 concentrations. L. aestuarii BL J, an isolate from marine intertidal mats, had the fastest production rates and reached the highest steady-state concentrations, 15-fold higher than that observed in Synechocystis sp. PCC 6803. Because all Pattern 2 strains originated in intertidal microbial mats that become anoxic in dark, it was hypothesized that their strong hydrogenogenic capacity may have evolved to aid in fermentation of the photosynthate. When forced to ferment, these cyanobacteria display similarly desirable characteristics of physiological H2 production. Again, L. aestuarii BL J had the fastest specific rates and attained the highest H2 concentrations during fermentation, which proceeded via a mixed-acid pathway to yield acetate, ethanol, lactate, H2, CO2 and pyruvate. The genome of L. aestuarii BL J was sequenced and bioinformatically compared to other cyanobacterial genomes to ascertain any potential genetic or structural basis for powerful H2 production. The association hcp exclusively in Pattern 2 strains suggests its possible role in increased H2 production. This study demonstrates the value of bioprospecting approaches to biotechnology, pointing to the strain L. aestuarii BL J as a source of useful genetic information or as a potential platform for biohydrogen production.
ContributorsKothari, Ankita (Author) / Garcia-Pichel, Ferran (Thesis advisor) / Vermaas, Willem F J (Committee member) / Rittmann, Bruce (Committee member) / Torres, Cesar (Committee member) / Arizona State University (Publisher)
Created2013
Description
As engineered nanomaterials (NMs) become used in industry and commerce their loading to sewage will increase. However, the fate of widely used NMs in wastewater treatment plants (WWTPs) remains poorly understood. In this research, sequencing batch reactors (SBRs) were operated with hydraulic (HRT) and sludge (SRT) retention times representative of full-scale biological WWTPs for several weeks. NM loadings at the higher range of expected environmental concentrations were selected. To achieve the pseudo-equilibrium state concentration of NMs in biomass, SBR experiments needed to operate for more than three times the SRT value, approximately 18 days. Under the conditions tested, NMs had negligible effects on ability of the wastewater bacteria to biodegrade organic material, as measured by chemical oxygen demand (COD). NM mass balance closure was achieved by measuring NMs in liquid effluent and waste biosolids. All NMs were well removed at the typical biomass concentration (1~2 gSS/L). However, carboxy-terminated polymer coated silver nanoparticles (fn-Ag) were removed less effectively (88% removal) than hydroxylated fullerenes (fullerols; >90% removal), nano TiO2 (>95% removal) or aqueous fullerenes (nC60; >95% removal). Although most NMs did not settle out of the feed solution without bacteria present, approximately 65% of the titanium dioxide was removed even in the absence of biomass simply due to self-aggregation and settling. Experiments conducted over 4 months with daily loadings of nC60 showed that nC60 removal from solution depends on the biomass concentration. Under conditions representative of most suspended growth biological WWTPs (e.g., activated sludge), most of the NMs will accumulate in biosolids rather than in liquid effluent discharged to surface waters. Significant fractions of fn-Ag were associated with colloidal material which suggests that efficient particle separation processes (sedimentation or filtration) could further improve removal of NM from effluent. As most NMs appear to accumulate in biosolids, future research should examine the fate of NMs during disposal of WWTP biosolids, which may occur through composting or anaerobic digestion and/or land application, incineration, or landfill disposal.
ContributorsWang, Yifei (Author) / Westerhoff, Paul (Thesis advisor) / Krajmalnik-Brown, Rosa (Committee member) / Rittmann, Bruce (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2012
Description
Population growth and fresh water depletion challenge drinking water utilities. Surface water quality is impacted significantly by climate variability, human activities, and extreme events like natural disasters. Dissolved organic carbon (DOC) is an important water quality index and the precursor of disinfection by-products (DBPs) that varies with both hydrologic and anthropogenic factors. Granular activated carbon (GAC) is a best available technology for utilities to meet Stage 2 D/DBP rule compliance and to remove contaminants of emerging concern (CECs) (e.g., pharmaceutical, personal care products (PCPs), etc.). Utilities can operate GAC with more efficient and flexible strategies with the understanding of organic occurrence in source water and a model capable predicting DOC occurrence. In this dissertation, it was found that DOC loading significantly correlated with spring runoff and was intensified by dry-duration antecedent to first flush. Dynamic modeling based on reservoir management (e.g., pump-back operation) was established to simulate the DOC transport in the reservoir system. Additionally, summer water recreational activities were found to raise the level of PCPs, especially skin-applied products, in raw waters. GAC was examined in this dissertation for both carbonaceous and emerging nitrogenous DBP (N-DBP) precursors (i.e., dissolved organic nitrogen (DON)) removal. Based on the experimental findings, GAC preferentially removes UV254-absorbing material, and DOC is preferentially removed over DON which may be composed primarily of hydrophilic organic and results in the low affinity for adsorption by GAC. The presence of organic nitrogen can elevate the toxicity of DBPs by forming N-DBPs, and this could be a major drawback for facilities considering installation of a GAC adsorber owing to the poor removal efficiency of DON by GAC. A modeling approach was established for predicting DOC and DON breakthrough during GAC operation. However, installation of GAC adsorber is a burden for utilities with respect to operational and maintenance cost. It is common for utilities to regenerate saturated GAC in order to save the cost of purchasing fresh GAC. The traditional thermal regeneration technology for saturated GAC is an energy intensive process requiring high temperature of incineration. Additionally, small water treatment sites usually ship saturated GAC to specialized facilities for regeneration increasing the already significant carbon footprint of thermal regeneration. An innovative GAC regeneration technique was investigated in this dissertation for the feasibility as on-site water treatment process. Virgin GAC was first saturated by organic contaminant then regenerated in-situ by iron oxide nanocatalysts mixed with hydrogen peroxide. At least 70 % of adsorption capacity of GAC can be regenerated repeatedly for experiments using modeling compound (phenol) or natural organic matter (Suwannee River humic acid). The regeneration efficiency increases with increasing adsorbate concentration. Used-iron nanocatalysts can be recovered repeatedly without significant loss of catalytic ability. This in-situ regeneration technique provides cost and energy efficient solution for water utilities considering GAC installation. Overall, patterns were found for DOC and CEC variations in drinking water sources. Increasing concentrations of bulk (DOC and DON) and/or trace organics challenge GAC operation in utilities that have limited numbers of bed-volume treated before regeneration is required. In-situ regeneration using iron nanocatalysts and hydrogen peroxide provides utilities an alternative energy-efficient operation mode when considering installation of GAC adsorber.
ContributorsChiu, Chao-An (Author) / Westerhoff, Paul (Thesis advisor) / Rittmann, Bruce (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2012
Description
Endocrine-disrupting chemicals (EDCs) are substances that disrupt the function of the endocrine system by blocking or mimicking hormones. Over the years, these substances have been identified as responsible for producing adverse reproductive effects in freshwater vertebrate populations. Freshwater vertebrates include reptiles, amphibians, and fish living in bodies of water such as lakes or streams and are exposed when concentrations of EDCs enter their habitats. With over 800 known or potential EDCs identified, ample studies can be conducted on the effects of EDCs on freshwater vertebrates; however, studies can be costly. Since studies are costly, I have developed a methodology to prioritize EDC studies. I analyzed ten EDCs to determine their impact on freshwater vertebrates. I specified four criteria and EDCs that passed all four criteria were considered significant. The four criteria I utilized were population decreases, routes of exposure, adverse reproductive effects, and environmental persistence. I analyzed research studies as evidence for the pass or fail of each criterion, where I considered the EDC "ambiguous" if there was not enough information to make a judgment. I then assessed the research available for each EDC. Only one EDC had adequate information to pass or fail each criterion. The one with adequate information passed all criteria. Two EDCs lacked adequate information for three of the four criteria, three EDCs lacked adequate information for two of the four criteria, and four EDCs lacked adequate information for one of the four criteria. I assessed the EDCs based on whether there was adequate information available in each criterion in order to provide researchers direction for future research endeavors. The results indicate either there is much research that remains to be conducted or that researchers are not making existing results of studies available. Companies producing EDCs that are released into the environment can use the information in this report as a basis for determining strategies to minimize the impacts of EDCs on freshwater vertebrates.
ContributorsCooper, Samantha Lynn (Author) / Rittmann, Bruce (Thesis director) / Valentine, Teresa A. (Committee member) / Civil, Environmental and Sustainable Engineering Programs (Contributor) / Barrett, The Honors College (Contributor)
Created2015-05
Description
With global warming becoming a more serious problem and mankind's alarming dependency on fossil fuels, the need for a sustainable and environmentally friendly fuel source is becoming more important. Biofuels produced from photosynthetic microorganisms like algae or cyanobacteria offer a carbon neutral replacement for petroleum fuel sources; however, with the technology and information available today, the amount of biomass that would need to be produced is not economically feasible. In this work, I examined a possible factor impacting the growth of a model cyanobacterium, Synechocystis sp. PCC6803, which is heterotrophic bacteria communities accompanying the cyanobacteria. I experimented with three variables: the type of heterotrophic bacteria strain, the initial concentration of heterotrophic bacteria, and the addition of a carbon source (glucose) to the culture. With experimental information, I identified if given conditions would increase Synechocystis growth and thus increase the yield of biomass. I found that under non-limiting growth conditions, heterotrophic bacteria do not significantly affect the growth of Synechocystis or the corresponding biomass yield. The initial concentration of heterotrophic bacteria and the added glucose also did not affect the growth of Synechocystis. I did see some nutrient recycling from the heterotrophic bacteria as the phosphate levels in the growth medium were depleted, which was apparent from prolonged growth phase and higher levels of reactive phosphate in the media.
ContributorsCahill, Brendan Robert (Author) / Rittmann, Bruce (Thesis director) / Krajmalnik-Brown, Rosa (Committee member) / W. P. Carey School of Business (Contributor) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2015-12
Description
Microalgae-derived lipids are good sources of biofuel, but extracting them involves high cost, energy
expenditure, and environmental risk. Surfactant treatment to disrupt Scenedesmus biomass was evaluated
as a means to make solvent extraction more efficient. Surfactant treatment increased the recovery of fatty
acid methyl ester (FAME) by as much as 16-fold vs. untreated biomass using isopropanol extraction, and
nearly 100% FAME recovery was possible without any Folch solvent, which is toxic and expensive. Surfactant
treatment caused cell disruption and morphological changes to the cell membrane, as documented by
transmission electron microscopy and flow cytometry. Surfactant treatment made it possible to extract wet
biomass at room temperature, which avoids the expense and energy cost associated with heating
and drying of biomass during the extraction process. The best FAME recovery was obtained from highlipid
biomass treated with Myristyltrimethylammonium bromide (MTAB)- and 3-(decyldimethylammonio)-
propanesulfonate inner salt (3_DAPS)-surfactants using a mixed solvent (hexane : isopropanol = 1 : 1, v/v)
vortexed for just 1 min; this was as much as 160-fold higher than untreated biomass. The critical micelle
concentration of the surfactants played a major role in dictating extraction performance, but the growth
stage of the biomass had an even larger impact on how well the surfactants disrupted the cells and
improved lipid extraction. Surfactant treatment had minimal impact on extracted-FAME profiles and,
consequently, fuel-feedstock quality. This work shows that surfactant treatment is a promising strategy for
more efficient, sustainable, and economical extraction of fuel feedstock from microalgae.
expenditure, and environmental risk. Surfactant treatment to disrupt Scenedesmus biomass was evaluated
as a means to make solvent extraction more efficient. Surfactant treatment increased the recovery of fatty
acid methyl ester (FAME) by as much as 16-fold vs. untreated biomass using isopropanol extraction, and
nearly 100% FAME recovery was possible without any Folch solvent, which is toxic and expensive. Surfactant
treatment caused cell disruption and morphological changes to the cell membrane, as documented by
transmission electron microscopy and flow cytometry. Surfactant treatment made it possible to extract wet
biomass at room temperature, which avoids the expense and energy cost associated with heating
and drying of biomass during the extraction process. The best FAME recovery was obtained from highlipid
biomass treated with Myristyltrimethylammonium bromide (MTAB)- and 3-(decyldimethylammonio)-
propanesulfonate inner salt (3_DAPS)-surfactants using a mixed solvent (hexane : isopropanol = 1 : 1, v/v)
vortexed for just 1 min; this was as much as 160-fold higher than untreated biomass. The critical micelle
concentration of the surfactants played a major role in dictating extraction performance, but the growth
stage of the biomass had an even larger impact on how well the surfactants disrupted the cells and
improved lipid extraction. Surfactant treatment had minimal impact on extracted-FAME profiles and,
consequently, fuel-feedstock quality. This work shows that surfactant treatment is a promising strategy for
more efficient, sustainable, and economical extraction of fuel feedstock from microalgae.
ContributorsLai, Yenjung Sean (Author) / De Francesco, Federica (Author) / Aguinaga, Alyssa (Author) / Parameswaran, Prathap (Author) / Rittmann, Bruce (Author) / Biodesign Institute (Contributor) / Swette Center for Environmental Biotechnology (Contributor)
Created2015-10-20
Description
Using a CH[subscript 4]-based membrane biofilm reactor (MBfR), we studied perchlorate (ClO[subscript 4]–) reduction by a biofilm performing anaerobic methane oxidation coupled to denitrification (ANMO-D). We focused on the effects of nitrate (NO[subscript 3]–) and nitrite (NO[subscript 2]–) surface loadings on ClO[subscript 4]– reduction and on the biofilm community’s mechanism for ClO[subscript 4]– reduction. The ANMO-D biofilm reduced up to 5 mg/L of ClO[subscript 4]– to a nondetectable level using CH[subscript 4] as the only electron donor and carbon source when CH[subscript 4] delivery was not limiting; NO[subscript 3]– was completely reduced as well when its surface loading was ≤0.32 g N/m[superscript 2]-d. When CH[subscript 4] delivery was limiting, NO[subscript 3]– inhibited ClO[subscript 4]– reduction by competing for the scarce electron donor. NO[subscript 2]– inhibited ClO[subscript 4]– reduction when its surface loading was ≥0.10 g N/m[superscript 2]-d, probably because of cellular toxicity. Although Archaea were present through all stages, Bacteria dominated the ClO[subscript 4]–-reducing ANMO-D biofilm, and gene copies of the particulate methane mono-oxygenase (pMMO) correlated to the increase of respiratory gene copies. These pieces of evidence support that ClO[subscript 4]– reduction by the MBfR biofilm involved chlorite (ClO[subscript 2]–) dismutation to generate the O[subscript 2] needed as a cosubstrate for the mono-oxygenation of CH[subscript 4].
ContributorsLuo, Yi-Hao (Author) / Chen, Ran (Author) / Wen, Li-Lian (Author) / Meng, Fan (Author) / Zhang, Yin (Author) / Lai, Chun-Yu (Author) / Rittmann, Bruce (Author) / Zhao, He-Ping (Author) / Zheng, Ping (Author) / Biodesign Institute (Contributor) / Swette Center for Environmental Biotechnology (Contributor)
Created2015-02-17
Description
UV photolysis was used to relieve inhibition of biomass growth by sulfadiazine (SD), a broad-spectrum anti-microbial. To investigate the effects of SD on biomass growth, three substrates—glucose alone (G), glucose plus sulfadiazine (G+SD), and glucose plus photolyzed SD (G+PSD)—were used to culture the bacteria acclimated to glucose. The biomass was strongly inhibited when SD was added into the glucose solution, but inhibition was relieved to a significant degree when the SD was treated with UV irradiation as a pretreatment. The biomass growth kinetics were described well by the Monod model when glucose was used as a substrate alone, but the kinetics followed a hybrid Aiba model for non-competitive inhibition when SD was added to the solution. When photolyzed SD was added to glucose solution to replace original SD, the growth still followed Aiba inhibition, but inhibition was significantly relieved: the maximum specific growth rate (μ[subscript max]) increased by 17 %, and the Aiba inhibition concentration increased by 60 %. Aniline, a major product of UV photolysis, supported the growth of the glucose-biodegrading bacteria. Thus, UV photolysis of SD significantly relieved inhibition by lowering the SD concentration and by generating a biodegradable product.
ContributorsPan, Shihui (Author) / Yan, Ning (Author) / Zhang, Yongming (Author) / Rittmann, Bruce (Author) / Biodesign Institute (Contributor) / Swette Center for Environmental Biotechnology (Contributor)
Created2015-05-01