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Investigation of Novel Solid Polymer Electrolytes and Lithium Salts for Rechargeable Lithium Batteries
Title
Investigation of Novel Solid Polymer Electrolytes and Lithium Salts for Rechargeable Lithium Batteries
Creator
Zhao, Wendy
Date
2021
Description
Lithium-ion batteries (LIBs) are extensively used in many consumer electronic products. LIBs have great potential for application in electric...
Show moreLithium-ion batteries (LIBs) are extensively used in many consumer electronic products. LIBs have great potential for application in electric vehicles by virtue of their high power density and charge cycles. Research and development in this area has been focused on all around the globe. The major challenges include high cost, safety issues of the solvent based electrolytes, and low conductivities at ambient temperature of the solid polymer electrolytes (SPEs).This dissertation describes four novel electrolyte systems and a series of low lattice energy lithium salts synthesized and characterized for applications in LIBs. First, a new SPE has been derived from oligomeric poly(ethylene oxide) (PEO)-grafted crosslinked polystyrene (XPS) microspheres containing 1-2 lithium sulfonate moieties. This SPE possesses amorphous character with a glass transition temperature (Tg) around 135 ºC, displayed a good electrochemical stability with excellent ionic conductivity in excess of 10^-4 S/cm at 25ºC, and no significant thermal decomposition until 420 ºC. Second, a hybrid composite polymer electrolyte (CPE) was constructed with a gel matrix formed through hydrogen bonding by incorporating nanoparticles of fumed silica into the nanoscale network of PEO-XPS. Fumed silica with large surface modification group like polysiloxane formed an ideal gel structure offering significant high mechanical strength above 10^4 Pa, and a good ionic conductivity at 25°C. Third, a nonvolatile x-linked gel membrane electrolyte was synthesized with amino methacrylate, to introduce hemi-labile ligands as ionic liquid, into the polymer network. This new material exhibited improved salt solubility and ionic conductivity, due to the fast ligand exchange that facilitates the lithium ion structural transport, and also displayed an excellent electrochemical stability(4.8 V vs, Li/Li+). Fourth, a self-healing and thermal reversible polymer electrolyte designed based on Diels-Alder conjugation between multi-maleimides (2M-3M) and multi-furans (2F-4F) was synthesized. The reversible x-linking was realized through Diels-Alder (DA) and Retro-DA reactions by applying heating (>130°C)/cooling (<90°C) cycles. Last, new lithium salts with star and branch structures containing 1-4 of imide or methide moieties were synthesized and evaluated in PEO electrolyte system. These salts demonstrated good ambient temperature ionic conductivity at low concentrations, and the electrochemical stabilities were equal to or better than the most commonly used lithium salt, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). Synthesis and characterization, including electrochemical properties, thermal and electrochemical stabilities, mechanical behaviors and surface morphologies of these new materials are described and discussed.
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