Matching Items (43)
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Description
Zeolite thin films and membranes are currently a promising technology for pervaporation, gas separation and water purification. The main drawback with these technologies is that the synthesis is not consistent leading to varied and unreproducible results. The Langmuir-Blodgett technique is a robust method for transferring monolayers of molecules or crystals

Zeolite thin films and membranes are currently a promising technology for pervaporation, gas separation and water purification. The main drawback with these technologies is that the synthesis is not consistent leading to varied and unreproducible results. The Langmuir-Blodgett technique is a robust method for transferring monolayers of molecules or crystals to a solid substrate. By measuring the surface pressure and controlling the area, reliable results can be achieved by transferring monolayers to different solid substrates. It has been shown previously that various types of zeolites can be functionalized and dispersed on the top of water. This is done by using an alcohol to form a hydrophobic coating on the surface of zeolite. The Langmuir-Blodgett can be used to create thin, compact films of zeolites for synthesizing and growing zeolite films. For the first reported time, cubic LTA Zeolites monolayers have been assembled with the Langmuir-Blodgett technique with multiple solvents and different sizes of zeolites. These films were characterized with Scanning Electron Microscopy and Pressure-Area Isotherms generated from the Langmuir-Blodgett. It was found that linoleic acid is a required addition to the zeolite dispersions to protect the mechanical stability during agitation. Without this addition, the LTA zeolites are broken apart and lose their characteristic cubic structure. This effect is discussed and a theory is presented that the interparticle interactions of the long alkane chain of the linoleic acid help reduce the shear stress on the individual zeolite particles, thus preventing them from being broken. The effect of size of the zeolites on the monolayer formation was also discussed. There seemed to be little correlation between the monolayer quality and formation as size was changed. However, to optimize the process, different concentrations and target pressures are needed. Lastly, the effect of the solvent was explored and it was found that there is a different between monolayer formations for different solvents likely due to differing interparticle interactions. Overall, LTA zeolites were successfully fabricated and the important factors to consider are the zeolite size, the solvent, and the amount of surfactant stabilizer added.
ContributorsDopilka, Andrew Michael (Author) / Lind, Mary Laura (Thesis director) / Cay, Pinar (Committee member) / Materials Science and Engineering Program (Contributor) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2016-12
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Description
Even though access to purified water has improved, there are still many people and locations that do not have this convenience. Approximately 1.2 billion people lack access to safe drinking water and 2.6 billion people have little or no sanitation. Furthermore, breakthroughs in water purification technology are essential to combat

Even though access to purified water has improved, there are still many people and locations that do not have this convenience. Approximately 1.2 billion people lack access to safe drinking water and 2.6 billion people have little or no sanitation. Furthermore, breakthroughs in water purification technology are essential to combat these issues. While there are several approaches to water purification, membrane processes are widely used based on their numerous advantages, including high operating temperature and low energy input. In essence, membranes do not require chemical additives, thermal inputs, or regeneration of spent media. The spin coating procedure was used to make a total of 94 membrane samples by adjusting the following variables: membrane support, membrane wetting, solvent, polyacrylonitrile (PAN) content, water contant, Linde Type A (LTA) zeolite content, and the rotations per minute (RPM) of the spin coater. Parameters that were held constant include PAN for the permeable dispersion layer, LTA zeolites as the inorganic filler material, and a spin time of 30 seconds for the spin coater. There were key findings in both the preliminary and core data sets. From the preliminary membrane samples 1 \u2014 40, a baseline was established to use for the core data: polysulfone (PSf) support, 1 \u2014 3% PAN content, and 1 \u2014 3% LTA zeolite content. Flux analysis revealed many inconsistencies in groups 1 \u2014 13 such as unreasonably high error bars (+50%), flow rates that were near zero or extremely high (+15,000 L hr-1 m-2), and lack of a clear trend for membrane specifications. Membranes with a high degree of polymer \u2014 zeolite aggregation on the surface had very low flux values. A higher flux of 4,700 L hr-1 m-2 was correlated to gap and hole formation on the membrane surface. It was shown in group 7 that an increasing degree of surface defects corresponded to an increasing flux of 17,000 L hr-1 m-2. Although the target flux for a defect \u2014 free membrane lies between 500 \u2014 4,000 L hr-1 m-2, there were not any groups with flux values in this range. Attenuated total reflectance Fourier transform infrared (ATR-FTIR) analysis revealed that the observed group similarities could not be attributed to individual membrane specifications. However, this data showed chemical fingerprint overlap across all groups, which were synthesized with varying quantities of the same chemicals. Analysis of flux data, SEM images, and ATR-FTIR data all suggest that the spin coating procedure leads to inconsistent results. Although the spin coater provides flexibility in user control, its advantages are outweighed by the limited control of surface uniformity, zeolite dispersion, and defect formation. It has been shown that the spin coating process is not compatible with the formation of a uniform polymer \u2014 zeolite layer in these experiments.
ContributorsMaltagliati, Alexander Justin (Author) / Lind, Mary Laura (Thesis director) / Durgun, Pinar Cay (Committee member) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2016-12
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Description
This dissertation focuses on the biosynthetic production of aromatic fine chemicals in engineered Escherichia coli from renewable resources. The discussed metabolic pathways take advantage of key metabolites in the shikimic acid pathway, which is responsible for the production of the aromatic amino acids phenylalanine, tyrosine, and tryptophan. For the first

This dissertation focuses on the biosynthetic production of aromatic fine chemicals in engineered Escherichia coli from renewable resources. The discussed metabolic pathways take advantage of key metabolites in the shikimic acid pathway, which is responsible for the production of the aromatic amino acids phenylalanine, tyrosine, and tryptophan. For the first time, the renewable production of benzaldehyde and benzyl alcohol has been achieved in recombinant E. coli with a maximum titer of 114 mg/L of benzyl alcohol. Further strain development to knockout endogenous alcohol dehydrogenase has reduced the in vivo degradation of benzaldehyde by 9-fold, representing an improved host for the future production of benzaldehyde as a sole product. In addition, a novel alternative pathway for the production of protocatechuate (PCA) and catechol from the endogenous metabolite chorismate is demonstrated. Titers for PCA and catechol were achieved at 454 mg/L and 630 mg/L, respectively. To explore potential routes for improved aromatic product yields, an in silico model using elementary mode analysis was developed. From the model, stoichiometric optimums maximizing both product-to-substrate and biomass-to-substrate yields were discovered in a co-fed model using glycerol and D-xylose as the carbon substrates for the biosynthetic production of catechol. Overall, the work presented in this dissertation highlights contributions to the field of metabolic engineering through novel pathway design for the biosynthesis of industrially relevant aromatic fine chemicals and the use of in silico modelling to identify novel approaches to increasing aromatic product yields.
ContributorsPugh, Shawn (Author) / Nielsen, David (Thesis advisor) / Dai, Lenore (Committee member) / Torres, Cesar (Committee member) / Lind, Mary Laura (Committee member) / Wang, Xuan (Committee member) / Arizona State University (Publisher)
Created2016
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Description
Environmentally responsive hydrogels are one interesting class of soft materials. Due to their remarkable responsiveness to stimuli such as temperature, pH, or light, they have attracted widespread attention in many fields. However, certain functionality of these materials alone is often limited in comparison to other materials such as silicon; thus,

Environmentally responsive hydrogels are one interesting class of soft materials. Due to their remarkable responsiveness to stimuli such as temperature, pH, or light, they have attracted widespread attention in many fields. However, certain functionality of these materials alone is often limited in comparison to other materials such as silicon; thus, there is a need to integrate soft and hard materials for the advancement of environmental-ly responsive materials.

Conventional hydrogels lack good mechanical properties and have inherently slow response time, important characteristics which must be improved before the hydrogels can be integrated with silicon. In the present dissertation work, both these important attrib-utes of a temperature responsive hydrogel, poly(N-isopropylacrylamide) (PNIPAAm), were improved by adopting a low temperature polymerization process and adding a sili-cate compound, tetramethyl orthosilicate. Furthermore, the transition temperature was modulated by adjusting the media quality in which the hydrogels were equilibrated, e.g. by adding a co-solvent (methanol) or an anionic surfactant (sodium dodecyl sulfate). In-terestingly, the results revealed that, based on the hydrogels’ porosity, there were appre-ciable differences when the PNIPAAm hydrogels interacted with the media molecules.

Next, an adhesion mechanism was developed in order to transfer silicon thin film onto the hydrogel surface. This integration provided a means of mechanical buckling of the thin silicon film due to changes in environmental stimuli (e.g., temperature, pH). We also investigated how novel transfer printing techniques could be used to generate pat-terned deformation of silicon thin film when integrated on a planar hydrogel substrate. Furthermore, we explore multilayer hybrid hydrogel structures formed by the integration of different types of hydrogels that have tunable curvatures under the influence of differ-ent stimuli. Silicon thin film integration on such tunable curvature substrates reveal char-acteristic reversible buckling of the thin film in the presence of multiple stimuli.

Finally, different approaches of incorporating visible light response in PNIPAAm are discussed. Specifically, a chemical chromophore- spirobenzopyran was synthesized and integrated through chemical cross-linking into the PNIPAAm hydrogels. Further, methods of improving the light response and mechanical properties were also demonstrat-ed. Interestingly, such a system was shown to have potential application as light modulated topography altering system
ContributorsChatterjee, Prithwish (Author) / Dai, Lenore L. (Thesis advisor) / Jiang, Hanqing (Thesis advisor) / Lind, Mary Laura (Committee member) / Yu, Hongyu (Committee member) / Yu, Hongbin (Committee member) / Arizona State University (Publisher)
Created2015
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Description
In the United States, 95% of the industrially produced hydrogen is from natural gas reforming. Membrane-based techniques offer great potential for energy efficient hydrogen separations. Pd77Ag23 is the bench-mark metallic membrane material for hydrogen separation at high temperatures. However, the high cost of palladium limits widespread application. Amorphous metals with

In the United States, 95% of the industrially produced hydrogen is from natural gas reforming. Membrane-based techniques offer great potential for energy efficient hydrogen separations. Pd77Ag23 is the bench-mark metallic membrane material for hydrogen separation at high temperatures. However, the high cost of palladium limits widespread application. Amorphous metals with lower cost elements are one alternative to replace palladium-based membranes. The overall aim of this thesis is to investigate the potential of binary and ternary amorphous metallic membranes for hydrogen separation. First, as a benchmark, the influence of surface state of Pd77Ag23 crystalline metallic membranes on the hydrogen permeability was investigated. Second, the hydrogen permeability, thermal stability and mechanical properties of Cu-Zr and Ni60Nb35M5 (M=Sn, Ti and Zr) amorphous metallic membranes was evaluated.

Different heat treatments were applied to commercial Pd77Ag23 membranes to promote surface segregation. X-ray photoelectron spectroscopy (XPS) analysis indicates that the membrane surface composition changed after heat treatment. The surface area of all membranes increased after heat treatment. The higher the surface Pd/(Pd+Ag) ratio, the higher the hydrogen permeability. Surface carbon removal and surface area increase cannot explain the observed permeability differences.

Previous computational modeling predicted that Cu54Zr46 would have high hydrogen permeability. Amorphous metallic Cu-Zr (Zr=37, 54, 60 at. %) membranes were synthesized and investigated. The surface oxides may result in the lower experimental hydrogen permeability lower than that predicted by the simulations. The permeability decrease indicates that the Cu-Zr alloys crystallized in less than two hours during the test (performed at 300 °C) at temperatures below the glass transition temperature. This original experimental results show that thermal stability of amorphous metallic membranes is critical for hydrogen separation applications.

The hydrogen permeability of Ni60Nb35M5 (M=Sn, Ti and Zr) amorphous metallic membranes was investigated. Nanoindentation shows that the Young’s modulus and hardness increased after hydrogen permeability test. The structure is maintained amorphous after 24 hours of hydrogen permeability testing at 400°C. The maximum hydrogen permeability of three alloys is 10-10 mol m-1 s-1 Pa-0.5. Though these alloys exhibited a slight hydrogen permeability decreased during the test, the amorphous metallic membranes were thermally stable and did not crystalize.
ContributorsLai, Tianmiao (Author) / Lind, Mary Laura (Thesis advisor) / Lin, Jerry (Committee member) / Li, Jian (Committee member) / Arizona State University (Publisher)
Created2015
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Description
Silicone compounds have a very low surface energy due to highly flexible Si-O-Si backbone and large number of –CH3 groups, but these compounds are extremely hydrophobic and thus have limited applications in aqueous formulations. Modification of such silicone compounds by grafting hydrophilic chains provides a wide range of silicone products

Silicone compounds have a very low surface energy due to highly flexible Si-O-Si backbone and large number of –CH3 groups, but these compounds are extremely hydrophobic and thus have limited applications in aqueous formulations. Modification of such silicone compounds by grafting hydrophilic chains provides a wide range of silicone products called "Silicone Surfactants". Silicone surfactants are surface active agents which get adsorbed at the air-water interface thereby, reducing the interfacial tension. Some of the larger applications of silicone surfactant are in the manufacture of plastic foams, in personal care products and as spreading and wetting agents (Hill, R.M, 2002).

In this thesis, a series of silicone surfactant graft copolymers were synthesized via hydrosilylation reaction. Poly(ethylene glycol) (PEG) of different chain length was grafted to a hydrophobic Poly(methylhydrosiloxane) (PMHS) backbone to improve the final hydrophilicity. Also, a positively charged quaternary ammonium salt (allyltriethylammonium bromide) was grafted to the PMHS backbone. The objective of this thesis was to synthesize polymers in predefined ratios of the above mentioned side groups and utilize these polymers to-

1) Study the effect of PEG chain length and its composition on the hydrophilicity of the polymer.

2) Study the effect of PEG: ammonium salt ratio on the surface tension of aqueous systems.

Analysis of FT-IR and 1H NMR spectra of the polymers confirmed the predicted structure. The absence of characteristic Si-H absorbance peak at 2160 cm-1 in FT-IR spectra indicates consumption of silane groups along the polymer backbone. The actual moles of the side chain grafted on the backbone are calculated by 1H NMR peak integration. The results of contact angle studies indicated an increase in hydrophilicity with an increase in the composition of PEG in molecule. A 2*2 factorial DOE analysis reported that the fraction of Si-H bonds converted to PEG grafts was the critical factor towards increasing the hydrophilicity (p value of 0.015). Surface tension studies report that the air-water interfacial tension of the synthesized polymers is between 28mN/m – 45mN/m. The amount of Si-H was concluded to be the deciding factor in lowering the surface tension.
ContributorsSingh, Pummy (Author) / Green, Matthew (Thesis advisor) / He, Ximin (Committee member) / Lind, Mary Laura (Committee member) / Arizona State University (Publisher)
Created2016
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Description
Water recovery from impaired sources, such as reclaimed wastewater, brackish groundwater, and ocean water, is imperative as freshwater resources are under great pressure. Complete reuse of urine wastewater is also necessary to sustain life on space exploration missions of greater than one year’s duration. Currently, the Water Recovery System (WRS)

Water recovery from impaired sources, such as reclaimed wastewater, brackish groundwater, and ocean water, is imperative as freshwater resources are under great pressure. Complete reuse of urine wastewater is also necessary to sustain life on space exploration missions of greater than one year’s duration. Currently, the Water Recovery System (WRS) used on the National Aeronautics and Space Administration (NASA) shuttles recovers only 70% of generated wastewater.1 Current osmotic processes show high capability to increase water recovery from wastewater. However, commercial reverse osmosis (RO) membranes rapidly degrade when exposed to pretreated urine-containing wastewater. Also, non-ionic small molecules substances (i.e., urea) are very poorly rejected by commercial RO membranes.

In this study, an innovative composite membrane that integrates water-selective molecular sieve particles into a liquid-barrier chemically resistant polymer film is synthetized. This plan manipulates distinctive aspects of the two materials used to create the membranes: (1) the innate permeation and selectivity of the molecular sieves, and (2) the decay-resistant, versatile, and mechanical strength of the liquid-barrier polymer support matrix.

To synthesize the membrane, Linde Type A (LTA) zeolite particles are anchored to the porous substrate, producing a single layer of zeolite particles capable of transporting water through the membrane. Thereafter, coating the chemically resistant latex polymer filled the space between zeolites. Finally, excess polymer was etched from the surface to expose the zeolites to the feed solution. The completed membranes were tested in reverse osmosis mode with deionized water, sodium chloride, and rhodamine solutions to determine the suitability for water recovery.

The main distinguishing characteristics of the new membrane design compared with current composite membrane include: (1) the use of an impermeable polymer broadens the range of chemical resistant polymers that can be used as the polymer matrix; (2) the use of zeolite particles with specific pore size insures the high rejection of the neutral molecules since water is transported through the zeolite rather than the polymer; (3) the use of latex dispersions, environmentally friendly water based-solutions, as the polymer matrix shares the qualities of low volatile organic compound, low cost, and non- toxicity.
ContributorsKhosravi, Afsaneh Khosravi (Author) / Lind, Mary Laura (Thesis advisor) / Dai, Lenore (Committee member) / Green, Matthew (Committee member) / Lin, Jerry (Committee member) / Seo, Don (Committee member) / Arizona State University (Publisher)
Created2016
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Description
Ionic liquids (ILs), or low-temperature liquid salts, are a class of materials with unique and useful properties. Made up entirely of ions, ILs are remarkably tunable and diverse as cations and anions can be mixed and matched to yield desired properties. Because of this, IL/water systems range widely—from homogeneous mixtures

Ionic liquids (ILs), or low-temperature liquid salts, are a class of materials with unique and useful properties. Made up entirely of ions, ILs are remarkably tunable and diverse as cations and anions can be mixed and matched to yield desired properties. Because of this, IL/water systems range widely—from homogeneous mixtures to multiphasic systems featuring ionic liquid/liquid interfaces. Even more diversity is added when particles are introduced to these systems, as hard particles or soft-matter microgels interact with both ILs and water in complex ways. This work examines both miscible ionic liquid/water mixture and two-phase, immiscible ionic liquid/water systems. Extensive molecular dynamics (MD) simulations are utilized in conjunction with physical measurements to inform theoretical understanding of the nature of these systems, and this theoretical understanding is related to practical applications—in particular, the development of a low-temperature liquid electrolyte for use in molecular electronic transducer (MET) seismometers, and particle self-assembly and transport at ionic liquid/liquid interfaces such as those in Pickering emulsions.

The homogenous mixture of 1-butyl-3-methylimidazolium iodide and water is examined extensively through MD as well as physical characterization of properties. Molecular ordering within the liquid mixture is related to macroscopic properties. These mixtures are then used as the basis of an electrolyte with unusual characteristics, specifically a wide liquid temperature range with an extremely low lower bound combined with relatively low viscosity allowing excellent performance in the MET sensor. Electrolyte performance is further improved by the addition of fullerene nanoparticles, which dramatically increase device sensitivity. The reasons behind this effect are explored by testing the effect of graphene surface size and through MD simulations of fullerene and a silica nanoparticle (for contrast) in [BMIM][I]/water mixtures.

Immiscible ionic liquid/water systems are explored through MD studies of particles at IL/water interfaces. By increasing the concentration of hydrophobic nanoparticles at the IL/water interface, one study discovers the formation of a commingled IL/water/particle pseudo-phase, and relates this discovery to previously-observed unique behaviors of these interfaces, particularly spontaneous particle transport across the interface. The other study demonstrates that IL hydrophobicity can influence the deformation of thermo-responsive soft particles at the liquid/liquid interface.
ContributorsNickerson, Stella Day (Author) / Dai, Lenore L (Thesis advisor) / Yu, Hongyu (Committee member) / Lind, Mary Laura (Committee member) / Mu, Bin (Committee member) / Emady, Heather (Committee member) / Arizona State University (Publisher)
Created2016
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Description
As selenium is toxic at low levels, treatment methods to remove selenium from industrial waste waters are needed. In this work, three groups of sorbent materials were investigated in detail for their effectiveness for selenium and arsenic removal from water: 1) nanostructured carbon-based materials, 2) layered double hydroxide (LDH)-based materials,

As selenium is toxic at low levels, treatment methods to remove selenium from industrial waste waters are needed. In this work, three groups of sorbent materials were investigated in detail for their effectiveness for selenium and arsenic removal from water: 1) nanostructured carbon-based materials, 2) layered double hydroxide (LDH)-based materials, and 3) biopolymer-based sorbents. The materials were investigated in spiked de-ionized water and waters collected from different locations at Salt River Project’s (SRP) Santan Generating Station in Gilbert, AZ. The results show that nanostructured carbon-based materials removed ~80% and up to 100% selenium and arsenic, respectively in spiked DI water. Heat treated layered double hydroxides removed close to 100% removal in selenium and arsenic spiked DI water. Isotherms conducted in spiked DI water fit the Langmuir model and showed a maximum selenate adsorption capacity of 67 mg/g for the calcined LDH powder. Results from SRP waters showed that certain LDH sorbents were effective for removing the selenium, but that higher pH and existence of competing ions affected the removal efficiencies. The functionalized biopolymer sorbent from Crystal Clear Technologies: CCT-149/OCI-B showed good removal efficiencies for both selenate and selenite in DI water. Isotherms conducted in spiked DI water for CCT-149 fit the Langmuir model and showed a maximum selenate adsorption capacity of 90.9 mg/g. Column tests using spiked DI water and waters obtained from SRP wells were investigated using both LDH and CCT-149/OCI-B. Removal of sulfate using chemical pre-treatment of the water with barium chloride resulted in about three times higher selenate loading onto the granular LDH and doubled the water volume that can be treated using CCT-149/OCI-B. The results from the column tests are being used to guide the pilot testing investigating the implementation of LDH sorbents at pilot scale at the Santan plant. The good results in the cooling tower #5 blowdown water and combined discharge waste water of SRP provide valuable information about the efficacy and efficiency of adsorptive media for the removal of selenium. Composites comprising LDH nanosheets with different substrates were successfully synthesized that were able to retain the performance in removing selenate of nanosheet LDH.
ContributorsLi, Man (Author) / Chan, Candace (Thesis advisor) / Lind, Mary Laura (Committee member) / Perreault, Francois (Committee member) / Arizona State University (Publisher)
Created2017
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Description
The aims of this project are to demonstrate the design and implementation of separations modalities for 1) in situ product recovery and 2) upstream pretreatment of toxic feedstocks. Many value-added bioproducts such as alcohols (ethanol and butanol) developed for the transportation sector are known to be integral to a sustainable

The aims of this project are to demonstrate the design and implementation of separations modalities for 1) in situ product recovery and 2) upstream pretreatment of toxic feedstocks. Many value-added bioproducts such as alcohols (ethanol and butanol) developed for the transportation sector are known to be integral to a sustainable future. Likewise, bioproduced aromatic building blocks for sustainable manufacturing such as phenol will be equally important. The production of these compounds is often limited by product toxicity at 2- 20 g/L, whereas it may desirable to produce 20-200 g/L for economically feasible scale up. While low-cost feedstocks are desirable for economical production, they contain highly cytotoxic value-added byproducts such as furfural. It is therefore desirable to design facile detoxification methods for lignocellulose-derived feedstocks to isolate and recover furfural preceding ethanol fermentation by Escherichia coli. Correspondingly it is desirable to design efficient facile in situ recovery modalities for bioalcohols and phenolic bioproducts. Accordingly, in-situ removal modalities were designed for simultaneous acetone, butanol, and ethanol recovery. Additionally, a furfural removal modality from lignocellulosic hydrolysates was designed for upstream pretreatment. Solid-liquid adsorption was found to serve well each of the recovery modalities characterized here. More hydrophobic compounds such as butanol and furfural are readily recovered from aqueous solutions via adsorption. The primary operational drawback to adsorption is adsorbent recovery and subsequent desorption of the product. Novel magnetically separable mesoporous carbon powders (MMCPs) were characterized and found to be rapidly separable from solutions at 91% recovery by mass. Thermal desorption of value added products was found efficient for recovery of butanol and furfural. Fufural was desorbed from the MMCPs up to 57% by mass with repeated adsorption/thermal desorption cycles. Butanol was recovered from MMCPs up to an average 93% by mass via thermal desorption. As another valuable renewable fermentation product, phenol was also collected via in-situ adsorption onto Dowex Optipore L-493 resin. Phenol recovery from the resins was efficiently accomplished with tert-butyl methyl ether up to 77% after 3 washes.
ContributorsStaggs, Kyle William (Author) / Nielsen, David R (Thesis advisor) / Lin, Jerry S (Committee member) / Torres, César I (Committee member) / Lind, Mary Laura (Committee member) / Wang, Xuan (Committee member) / Arizona State University (Publisher)
Created2017