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Solid-state Polymer Electrolytes for Advanced Lithium-ion Battery Manufacturing

Lai, Yueh-Ting
http://rave.ohiolink.edu/etdc/view?acc_num=akron1720447411436966

Abstract Details

, Doctor of Philosophy, University of Akron, Polymer Science.
Lithium-ion batteries (LIBs) are crucial energy sources across diverse sectors, from medical devices in nanotechnology to grid energy storage. However, their liquid electrolytes pose significant safety risks, particularly during overheating, leading to battery explosions. This hazard is especially pronounced in electric vehicles, where breaches can trigger catastrophic cell explosions. Solid-state batteries (SSBs) have emerged as a promising alternative, offering enhanced safety by replacing liquid electrolytes with solid-state electrolytes (SSEs). Despite this, scaling up LIB production and improving energy and power density remain significant challenges. Chapter I presents a novel approach using 3D printing technology to fabricate solid polymer electrolyte membranes for SSBs. This method replaces conventional polymer separators and liquid electrolytes with a thin, ionically conductive composite based on poly(ethylene glycol) diacrylate (PEGDA) reinforced with polyamide for mechanical strength. Using a digital light processing (DLP) 3D printer, we created thin SSE films. Lithium plating/stripping tests showed that the printed PEGDA/polyamide electrolyte maintained stable cycling performance over 1,400 hours at a current density of 0.05 mA/cm². Additionally, LIBs with the 30 μm polyamide-reinforced electrolyte exhibited excellent cyclability at a 0.2 C rate under ambient conditions (30°C). Chapter II addresses issues with traditional cathode electrode processes, such as the insulating polyvinylidene fluoride (PVDF) binder and toxic organic N-methyl-2-pyrrolidone (NMP) solvent. We introduced a solvent-free electrode processing technique using a thermal cross-linkable polymer electrolyte as a binder substitute. This method allows the creation of higher mass loading electrodes without volatile organic compounds (VOCs). Cathode electrodes were prepared on the current collector using hydraulic thermal pressing, with adjustments to the pressing force. Structural parameters, particularly thickness and porosity, were correlated with electrochemical performance, significantly impacting the lithium diffusion coefficient and determining the battery's rate performance. This non-solvent fabricated cathode achieved an areal capacity exceeding 4 mAh/cm². Chapter III explores sulfide-based SSEs combined with solid-state polymer electrolytes. Sulfide-based SSEs, known for their high ionic conductivity exceeding 10 mS/cm at room temperature, require high pressure for preparation and use, presenting practical limitations. In contrast, polymer-based electrolytes, while easier to process, suffer from poor ionic conductivity and mechanical robustness. Hybrid materials, balancing high performance and ease of processing, offer a promising solution. We prepared laminar configurations of soft materials and sulfide electrolytes to investigate charge transport in battery devices, achieving an ionic conductivity of 0.46 mS/cm. In a Li|LFP cell with a mass loading of 7.8 mg/cm², the specific capacity was approximately 136.98 mAh/g, with about 97.0% capacity retention after 50 cycles without additional operational pressure. These findings underscore the potential of innovative manufacturing techniques and hybrid materials in enhancing the performance, safety, and scalability of future LIBs and SSBs.
Yu Zhu (Advisor)
Steven S.C. Chuang (Committee Chair)
Chunming Liu (Committee Member)
Weinan Xu (Committee Member)
Tianbo Liu (Committee Member)
145 p.
Chemistry; Energy; Materials Science
Energy Storage, Lithium-ion Battery, Solid-state Electrolyte, Solvent-free Cathode, Electrochemistry

Recommended Citations

Citations

  • Lai, Y.-T. (2024). Solid-state Polymer Electrolytes for Advanced Lithium-ion Battery Manufacturing [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron1720447411436966

    APA Style (7th edition)

  • Lai, Yueh-Ting. Solid-state Polymer Electrolytes for Advanced Lithium-ion Battery Manufacturing . 2024. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron1720447411436966.

    MLA Style (8th edition)

  • Lai, Yueh-Ting. "Solid-state Polymer Electrolytes for Advanced Lithium-ion Battery Manufacturing ." Doctoral dissertation, University of Akron, 2024. http://rave.ohiolink.edu/etdc/view?acc_num=akron1720447411436966

    Chicago Manual of Style (17th edition)

akron1720447411436966
© 2024, all rights reserved.
This open access ETD is published by University of Akron and OhioLINK.