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Development of Polysulfide-co-Polyoxide Electrolyte for High Specific Capacity Lithium Metal Batteries and Supercapacitors

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, Doctor of Philosophy, University of Akron, Polymer Engineering.
As the demand for next-generation batteries rises, the present dissertation is designed to illustrate the governing principles and novel technologies via development of multifunctional polymer electrolyte membrane for energy storage devices such as lithium-ion batteries and supercapacitors. Customarily, polymeric materials have been used to afford mechanical support as membrane separators and ion transport through liquid electrolyte media of energy storage devices, which are currently dominated by ceramic or inorganic metal oxide electrodes. The ultimate goal is aimed at understanding how polymer electrolyte matrix (PEM) can enhance both energy and power density beyond those afforded by the electrode active materials. Chapter 3 delves into the innovative application of polymer materials in battery formulation, leveraging ion-dipole complexation within a multifunctional polymer electrolyte membrane (PEM). This complexation entails the interaction between lithium ions, ether oxygen, and amine groups within the thermally cured poly(ethylene glycol) diglycidyl ether (PEGDGE) and polyether amine co-network. While this process may temporarily hinder ion transport, resembling temporary lithium ion storage, the prelithiation process ensures excess lithium ions for transport, enhancing PEM energy storage capacity and ionic conductivity. Additionally, diffusion, facilitated by ion concentration gradients in bilayer PEM composites, aids in supplying lithium ions to the PEM. The emergence of redox reactions, as demonstrated by cyclic voltammetry (CV) measurements, further supports the energy storage strategy of multifunctional PEM networks. In Chapter 4, the energy storage concept is exemplified through a high Ni-cathode, leveraging chemical reactions at the electrode-PEM interface. Introducing a PEM composed of a polysulfide and polyoxide blend with succinonitrile and LiTFSI salt enhances ion transport and storage capacity, exhibiting a conductivity of 1.18 x10-3 S/cm at room temperature, surpassing standard lithium-ion batteries. Chapter 5 validates this approach by substituting a high Ni-cathode with lithium titanium oxide (LTO) active materials, emphasizing the role of single and dual polymer networks in enhancing lithium battery storage capacity. Results from cyclic voltammetry and other tests showcase the promise of these polymer designs in improving battery performance. Chapter 6 shifts focus to supercapacitors, investigating fundamental research such as PEM thickness effects, electrode AC/CB ratios, and driving potential windows on electrochemical performance. Discoveries include an optimal PEM thickness of 100 𝜇m or smaller, as depicted in the Ragone plot, establishing relationships between power and energy density performances under various supercapacitor configurations. Last chapter aims to decipher the potential roles of polymer electrolytes in efficient batteries, aligning with the future needs of environmentally friendly energy storage solutions.
Thein Kyu (Advisor)
Xiong Gong (Committee Chair)
Toshikazu Miyoshi (Committee Member)
Kevin Cavicchi (Committee Member)
Jae-Won Choi (Committee Member)
262 p.

Recommended Citations

Citations

  • Hyunsang, L. (2024). Development of Polysulfide-co-Polyoxide Electrolyte for High Specific Capacity Lithium Metal Batteries and Supercapacitors [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron1714601294760754

    APA Style (7th edition)

  • Hyunsang, Lee. Development of Polysulfide-co-Polyoxide Electrolyte for High Specific Capacity Lithium Metal Batteries and Supercapacitors. 2024. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron1714601294760754.

    MLA Style (8th edition)

  • Hyunsang, Lee. "Development of Polysulfide-co-Polyoxide Electrolyte for High Specific Capacity Lithium Metal Batteries and Supercapacitors." Doctoral dissertation, University of Akron, 2024. http://rave.ohiolink.edu/etdc/view?acc_num=akron1714601294760754

    Chicago Manual of Style (17th edition)