Structure-Property Relationships in Sustainable Thermoplastic Elastomers

dc.contributor.advisorRobertson, Megan L.
dc.contributor.committeeMemberConrad, Jacinta C.
dc.contributor.committeeMemberYao, Yan
dc.contributor.committeeMemberHarth, Eva M.
dc.contributor.committeeMemberRimer, Jeffrey D.
dc.creatorDing, Wenyue
dc.date.accessioned2019-11-07T03:16:27Z
dc.date.createdAugust 2019
dc.date.issued2019-08
dc.date.submittedAugust 2019
dc.date.updated2019-11-07T03:16:28Z
dc.description.abstractThermoplastic elastomers (TPEs), predominantly composed of ABA triblock copolymers containing glassy polystyrene endblocks and rubbery polydiene midblocks, are widely used in electronics, adhesives and automotive components. Sustainable TPEs derived from renewable resources can be attractive alternatives to petroleum-based TPEs when sustainability requirements are met without compromising material performance. Vegetable oils and their fatty acids are promising replacements for petroleum sources as polymer feedstocks due to their abundance, lack of toxicity and ease of functionalization. However, fatty acid-derived TPEs exhibit inferior mechanical properties to petroleum-based products due to lack of entanglements, stemming from the presence of long alkyl chains on the fatty acids. To facilitate the adoption of polymers derived from vegetable oils and fatty acids, we aim to develop approaches to enhance the mechanical properties of this class of materials. In this study, two approaches were evaluated as means to enhance the mechanical properties of sustainable TPEs with fatty acid-derived midblocks: incorporation of hydrogen bonds or ionic interactions. In the first approach, the hydrogen bond-containing comonomer acrylamide was incorporated into midblock. The triblock copolymers exhibited not only greatly improved mechanical properties, but also accessible processing temperatures. In the second approach, ionic interactions were introduced into midblock by neutralizing the comonomer methacrylic acid. The tensile strength and modulus were significantly enhanced by the incorporation of ionic interactions and the strain at break was improved at low degrees of neutralization. In addition, the fatty acid-derived triblock copolymers exhibited a closed packed spherical (CPS) morphology under oscillatory shear, attributed to the presence of the higher dispersity midblock. The presence of CPS morphology in the bulk block copolymers has rarely been reported, which motivated the investigation of the kinetics and mechanisms through in-situ small-angle X-ray scattering and Fourier transform-rheology. The orientation of CPS layers was found to be affected by the strain amplitudes. For the first time, we observed shear deordering at high strain amplitude for the sphere-forming block copolymers in the bulk. Finally, to expand the library of renewable building blocks for TPEs, a rosin-derived polymer possessing a high glass transition temperature was evaluated as the endblocks in sustainable TPEs. The triblock copolymers exhibited elastomeric behavior at room temperature and accessible order-disorder transitions, appropriate for thermoplastic elastomer applications.
dc.description.departmentChemical and Biomolecular Engineering, Department of
dc.format.digitalOriginborn digital
dc.format.mimetypeapplication/pdf
dc.identifier.citationPortions of this document appear in: Ding, Wenyue, and Megan L. Robertson. "Sustainable thermoplastic elastomers with a transient network." European Polymer Journal 113 (2019): 411-423. And in: Ding, Wenyue, Shu Wang, Kejian Yao, Mitra S. Ganewatta, Chuanbing Tang, and Megan L. Robertson. "Physical behavior of triblock copolymer thermoplastic elastomers containing sustainable rosin-derived polymethacrylate end blocks." ACS Sustainable Chemistry & Engineering 5, no. 12 (2017): 11470-11480.
dc.identifier.urihttps://hdl.handle.net/10657/5296
dc.language.isoeng
dc.rightsThe author of this work is the copyright owner. UH Libraries and the Texas Digital Library have their permission to store and provide access to this work. UH Libraries has secured permission to reproduce any and all previously published materials contained in the work. Further transmission, reproduction, or presentation of this work is prohibited except with permission of the author(s).
dc.subjectThermoplastic elastomers
dc.subjectSustainability
dc.subjectMechanical properties
dc.subjectBlock copolymers
dc.titleStructure-Property Relationships in Sustainable Thermoplastic Elastomers
dc.type.dcmiText
dc.type.genreThesis
local.embargo.lift2021-08-01
local.embargo.terms2021-08-01
thesis.degree.collegeCullen College of Engineering
thesis.degree.departmentChemical and Biomolecular Engineering
thesis.degree.disciplineChemical Engineering
thesis.degree.grantorUniversity of Houston
thesis.degree.levelDoctoral
thesis.degree.nameDoctor of Philosophy

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