Non-Equilibrium, Ultra-Fast Heating Techniques for Material Synthesis, PFAS Mineralization and Upcycling.

dc.contributor.advisorTour , Jamesen_US
dc.contributor.advisorHan , Yimoen_US
dc.creatorScotland, Phelecia Zen_US
dc.date.accessioned2025-05-30T21:10:04Zen_US
dc.date.created2025-05en_US
dc.date.issued2025-04-25en_US
dc.date.submittedMay 2025en_US
dc.date.updated2025-05-30T21:10:04Zen_US
dc.description.abstractThe increasing demand for sustainable technologies and materials has led to a critical need for efficient, scalable, and environmentally friendly solutions for material synthesis, environmental remediation, and resource recovery. Among the innovative technologies addressing these challenges, Flash Joule Heating (FJH) has emerged as a versatile and transformative technique. This thesis explores the application of FJH in four significant areas: heteroatom-substituted graphene synthesis, the destruction of per- and polyfluoroalkyl substances (PFAS), the recovery of critical metals from lithium-ion batteries (LIBs) aided by waste PFAS and the synthesis of silicon carbide nanowires using waste glass. Graphene, a two-dimensional carbon-based material, is renowned for its extraordinary properties, including high electrical and thermal conductivity, mechanical strength, and chemical versatility. These properties make graphene a highly sought-after material for applications in energy storage, electronics, and catalysis. The functionality of graphene can be further enhanced by heteroatom substitution, which involves incorporating non-carbon atoms, such as nitrogen, boron, sulfur, and fluorine, into its lattice structure. These heteroatoms modify the electronic and chemical properties of graphene, expanding its range of potential applications. Traditional methods for heteroatom substitution, such as chemical vapor deposition and solvothermal processes, are often time-consuming, resource-intensive, and difficult to scale. In contrast, FJH offers a rapid, energy-efficient, and scalable alternative for producing high-quality, heteroatom-substituted graphene. By subjecting pre-formed graphene or carbon precursors to rapid high-temperature heating in the presence of heteroatom-containing precursors, FJH enables precise control over doping levels and ensures structural integrity, making it a promising method for scalable graphene functionalization. This is covered in chapter one of this thesis. In addition to its role in material synthesis, FJH provides a novel solution to a pressing environmental challenge: the destruction of PFAS, often referred to as "forever chemicals." PFAS are a class of synthetic organofluorine compounds widely used in industrial and consumer applications, including firefighting foams, non-stick coatings, and water-resistant materials. The strong carbon-fluorine bonds in PFAS make them highly resistant to degradation, leading to their accumulation in the environment and posing significant risks to human health and ecosystems. Current remediation techniques, such as adsorption onto granular activated carbon (GAC), capture PFAS but do not degrade them, leaving behind secondary waste. FJH addresses this limitation by degrading PFAS adsorbed onto GAC through high-temperature treatment, breaking the carbon-fluorine bonds and converting PFAS into benign byproducts. This process not only eliminates PFAS but also enables the upcycling of PFAS-contaminated GAC into valuable materials, such as graphene, demonstrating a sustainable approach to waste management. This is covered in chapter two of this thesis. We then demonstrate that FJH offers a sustainable and efficient approach for resource recovery from spent lithium-ion batteries (LIBs), which play a crucial role in modern energy storage systems. LIBs contain valuable metals, such as lithium and cobalt, whose extraction and processing are energy-intensive and environmentally damaging. The growing demand for these metals, driven by the proliferation of electric vehicles and renewable energy technologies, has raised concerns about resource scarcity and the environmental impact of conventional recycling methods. FJH offers a rapid and solvent-free approach to metal recovery, facilitating the fluorination of lithium into lithium fluoride (LiF) and the reduction of cobalt into metallic form. These transformations occur within a few seconds, minimizing energy consumption and environmental impact while enabling the efficient separation of metals for reuse. FJH addresses the challenges associated with LIB recycling as well as waste PFAS degradation. This is covered in chapter three. Finally, we demonstrate a flash process for upcycling waste glass into SiC nanowires within seconds. By introducing fluorine, iron oxide present in the waste glass is activated, catalyzing the formation of one-dimensional (1D) SiC nanowires. The resulting SiC nanowires exhibit superior performance in composite reinforcement compared to conventional SiC powders. Additionally, a life cycle assessment (LCA) and techno-economic analysis (TEA) reveal that our process significantly reduces environmental impact and production costs compared to conventional synthesis methods. This work highlights fluorine as a versatile and cost-effective agent for modulating nanomaterial growth kinetics and tailoring morphology, providing a sustainable and scalable approach for advanced material synthesis and is discussed in chapter 4 of this thesis. This thesis underscores the versatility and scalability of FJH as a platform for material innovation, environmental remediation, and resource recovery. Through its application in heteroatom-doped graphene synthesis, PFAS destruction, metal recovery from LIBs, and synthesis of one-dimension materials, FJH demonstrates its potential to bridge the gap between fundamental research and practical solutions, advancing both sustainability and technological progressen_US
dc.embargo.lift2025-11-01en_US
dc.embargo.terms2025-11-01en_US
dc.format.mimetypeapplication/pdfen_US
dc.identifier.urihttps://hdl.handle.net/1911/118532en_US
dc.language.isoenen_US
dc.subject1-D and 2-D Material Synthesis, Waste Upcyclingen_US
dc.titleNon-Equilibrium, Ultra-Fast Heating Techniques for Material Synthesis, PFAS Mineralization and Upcycling.en_US
dc.typeThesisen_US
dc.type.materialTexten_US
thesis.degree.departmentMaterials Science and NanoEngineeringen_US
thesis.degree.disciplineMaterials Science & NanoEngen_US
thesis.degree.grantorRice Universityen_US
thesis.degree.levelDoctoralen_US
thesis.degree.nameDoctor of Philosophyen_US
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