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Batteries have been in increasing demand over the last decade for portable electronic devices, electric vehicles, and grid-scale energy storage systems. While the electrode materials define the characteristic features of a battery system, the composition of the electrolyte is of critical importance and needs to be engineered for different battery systems to ensure superior electrochemical performance. In this thesis, the basic functionality and fundamental mechanism of the electrolytes in battery systems are first introduced. Then, three major electrolyte engineering strategies are demonstrated, including electrolyte composition formulation, electrolyte-electrode component modification, and function-oriented electrolyte design. Firstly, the low-temperature capacity restraint of lithium metal batteries is addressed by introducing an electrolyte additive that constructs a robust solid-electrolyte interphase layer on the surface of lithium metal electrodes. Secondly, solid-state electrolytes paired with nano-architectured sodium sulfide/carbon composite cathodes in sodium sulfur batteries are demonstrated, which effectively prevent the shuttling of polysulfides and alleviate the capacity decay over cycling. Lastly, the contact issue at the electrode/electrolyte interface in all-solid-state sodium sulfur batteries is tackled by the design and synthesis of a novel solid-state sodium thiophosphate electrolyte.
Zhang, Yiwen, "Electrolyte Synthesis and Engineering for Alkali Metal Batteries" (2023). Dartmouth College Ph.D Dissertations. 133.
Available for download on Friday, January 10, 2025