Convection enhanced electrochemical energy storage

Abstract

Electrochemical energy storage will play a pivotal role in our society's energy future, providing vital services to the transportation, grid, and residential markets. Depending on the power and duration requirements of a specific application, numerous electrochemical technologies exist. For the majority of the markets, lithium-ion (Li-ion) batteries are the state-of-the-art technology owing to their good cycle life and high energy density and efficiency. Their widespread penetration, however, is limited by high production cost and inherent safety concerns. Understanding the solid-electrolyte interphase (SEI) which governs the performance and lifetime of these batteries is critical to developing the next generation Li-ion batteries. As an alternative to Li-ion, redox flow batteries store energy in solutions of electroactive species, which are housed in external tanks and pumped to a power-converting electroreactor. This configuration decouples power and energy, improving the safety and flexibility of the system, however, flow battery energy density is inherently lower than Li-ion and expensive ion-selective membranes are required for efficient operation. As a contrast to Li-ion and redox flow batteries, convection batteries harnesses the key benefits of Li-ion batteries and redox flow batteries while overcoming their individual limitations. By incorporating thick electrodes into the cell, the energy density is increased and the cost of the system is reduced. To overcome the diffusive losses in the thick electrodes, electrolyte is pumped through the electrodes, enabling uniform ion transport throughout the porous structure. However, thick electrodes can lead to large ohmic losses in the cell resulting in lower energy efficiency. In this thesis, I discuss my work on understanding the SEI in Li-ion batteries, highlighting the thermodynamics of its origin, characterization of its structure, and strategies for future development. I then detail my work understanding redox active molecules from molecule characterization and mechanistic generation to redox flow cell level engineering. Finally, I highlight my work in the development of the convection battery technology explaining the synthesis of active materials, thick electrode design, and fabrication of the prototype convection cell architecture. Taken together, these projects highlight the theme of achieving low-cost electrochemical energy storage through various technical pathways.