An Investigation of Carbon-based Nanomaterials for Efficient Energy Production and Delivery

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dc.contributor.advisorWong, Michael S.en_US
dc.contributor.committeeMemberPasquali, Matteoen_US
dc.contributor.committeeMemberBarron, Andrew Ren_US
dc.contributor.committeeMemberAdams, Wadeen_US
dc.contributor.committeeMemberHauge, Robert Hen_US
dc.creatorGangoli, Varun Shenoyen_US
dc.date.accessioned2016-02-04T15:39:44Zen_US
dc.date.available2016-02-04T15:39:44Zen_US
dc.date.created2016-05en_US
dc.date.issued2016-01-28en_US
dc.date.submittedMay 2016en_US
dc.date.updated2016-02-04T15:39:44Zen_US
dc.description.abstractCarbon-based nanomaterials have been demonstrated to have different potential applications in the energy industry. However, there are challenges in the realization of these applications. Chirality of single wall carbon nanotubes (SWCNTs) defines their electronic properties, and obtaining an ensemble of SWCNTs of the same chirality has been a problem studied for over two decades with no clear solution yet. Other carbon-based nanomaterials, such as carbon black aggregates, are hydrophobic in nature and potential applications in the oil and gas industry require their dispersal in an aqueous solvent. Another application in the oil and gas industry is enhanced oil recovery (EOR), and here there is a need for an inexpensive, stable, and efficient surfactant compared to currently used industrial solutions. The challenge of producing SWCNTs of the same chirality is studied using two approaches- separation after synthesis of SWCNTs of mixed chiralities, and chemical control over chirality of as-synthesized SWCNTs. Agarose gel-based affinity chromatography was used as a means towards highly semiconductor- enriched SWCNTs using a family of nonionic surfactants. UV-vis-NIR spectroscopy, Raman spectroscopy and photoluminescence spectroscopy was used to quantify the separation efficiency of the metal- and semiconductor-enriched SWCNTs. This process is an improvement over other chromatography-based techniques at the time in that the nonionic surfactants used are less expensive, enable a higher purity of semiconductor SWCNTs (>95%) and decompose fully by simply heating in air thus leaving behind pristine SWCNTs. The second approach was based on using catalyst dopants to preferentially synthesize SWCNTs of a particular chirality at the expense of SWCNTs of other chiralities. Heterogeneous catalysis combined with the screw dislocation theory of SWCNT growth provided the background for this work, and both selenium and phosphorus were identified as chemical dopants for iron catalysts. Both selenium and phosphorus were demonstrated to have a direct effect on the average number density and length of SWCNTs, and selenium also was shown to have a direct control over the growth rate of SWCNTs. This, combined with some preliminary spectroscopy results, suggest chiral control over the carbon nanotubes. Collaborative work on phase transfer of hydrophobic carbon-based nanomaterials into aqueous solvents for applications including saturated oil residual (SOR) detection and quantification in underground reservoirs helped recognize the potential of hydrophobically modified polymers as surfactants for EOR. Polystyrene sulfonate was chosen as the polymer of study owing to ease of availability, low cost of the precursor material and aromatic sulfonates already being studied for EOR. Controlled desulfonation of PSS was achieved by rapid heating of an aqueous solution of PSS in a microwave reactor under acidic conditions, with the reactant temperature and pH having a strong effect on the degree of desulfonation of the product ranging from 4.9% (as-obtained PSS) to 40%. Dynamic light scattering of the desulfonated PSS (termed PDS) in brine showed good stability of the polymer aggregates at temperatures as high as 150 ÂșC, and tensiometry with aromatic oils such as toluene and aliphatic oils such as Isopar L showed good surface activity with interfacial tension going as low as 10-2 mN/m. Breakthrough experiments with sand packed columns at the lab scale, and core flooding at an independent facility confirmed good propagation of PDS through materials such as Berea sandstone, with minimal plugging and adsorption losses.en_US
dc.format.mimetypeapplication/pdfen_US
dc.identifier.citationGangoli, Varun Shenoy. "An Investigation of Carbon-based Nanomaterials for Efficient Energy Production and Delivery." (2016) Diss., Rice University. <a href="https://hdl.handle.net/1911/88348">https://hdl.handle.net/1911/88348</a>.en_US
dc.identifier.urihttps://hdl.handle.net/1911/88348en_US
dc.language.isoengen_US
dc.rightsCopyright is held by the author, unless otherwise indicated. Permission to reuse, publish, or reproduce the work beyond the bounds of fair use or other exemptions to copyright law must be obtained from the copyright holder.en_US
dc.subjectNanotubeen_US
dc.subjectCarbon Nanotubeen_US
dc.subjectSingle wall Carbon Nanotubeen_US
dc.subjectSWCNTen_US
dc.subjectChiralityen_US
dc.subjectNanotube Growthen_US
dc.subjectNanotube Separationen_US
dc.subjectChromatographyen_US
dc.subjectPolymeren_US
dc.subjectEORen_US
dc.subjectEnhanced Oil Recoveryen_US
dc.subjectSurfactanten_US
dc.titleAn Investigation of Carbon-based Nanomaterials for Efficient Energy Production and Deliveryen_US
dc.typeThesisen_US
dc.type.materialTexten_US
thesis.degree.departmentChemical and Biomolecular Engineeringen_US
thesis.degree.disciplineEngineeringen_US
thesis.degree.grantorRice Universityen_US
thesis.degree.levelDoctoralen_US
thesis.degree.nameDoctor of Philosophyen_US
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