Holmberg, Angela L.2020-10-192020-10-192016https://udspace.udel.edu/handle/19716/27843In response to global environmental concerns, an immediate need for practical, eco-friendly, and non-hazardous plastics has irrupted, yet such materials are challenging to invent. Various sustainability issues associated with commodity plastics are addressed in this dissertation via bottom-up design strategies. The main targets are block polymers (BPs), architecturally unique macromolecules that are widely employed in thermoplastic elastomers (TPEs), pressure-sensitive adhesives (PSA), and coatings. For potential TPE and PSA applications, a library of monomers is developed using model components of inexpensive, abundant, non-food (lignin and waste vegetable oil) biomasses. The corresponding polymers have properties comparable to polystyrene (PS), a common petroleum-based plastic, so these new macromolecules could become sustainable alternatives to PS. An innovative strategy for polymerizing chemically distinct biobased monomers together also is investigated as a means for tuning and enhancing material properties at reduced costs. The approach involves the <i>a priori</i> prediction of kinetic parameters and polymer properties based on feedstock composition and monomer structure. For coatings applications, sustainability challenges associated with polymeric surfaces that repel both water and oil are addressed. Novel triblock terpolymers are synthesized, and their surface properties are characterized to show the design strategy’s potential effectiveness toward an aim of minimizing unsustainable fluorine content while maintaining repellency. Altogether, the reported approaches and similar <i>de novo</i> design strategies have the potential to revolutionize material sustainability.Block copolymerLigninPolymer propertiesRAFT polymerizationRenewableSustainabilityThesis1200744147https://doi.org/10.58088/f850-ye112020-08-05en