CRYSTALLOGRAPHIC CONTROL AND INTERFACE DESIGN STRATEGIES FOR SODIUM-BASED SECONDARY BATTERY ANODES
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Rechargeable sodium batteries have garnered increasing interest as a promising pathway for low-cost, long-duration energy storage. With a high theoretical specific capacity of 1166 mAh/g and low reduction potential of −2.71 V, batteries incorporating metallic sodium as the anode hold great potential. However, the high reactivity and poor electrochemical reversibility of sodium anodes present significant challenges for practical implementation. We investigate the failure mechanisms of room-temperature, liquid electrolyte sodium metal anodes through in operando optical visualization and polarization measurements. Electronic disconnection of mossy metallic sodium deposits, known as "orphaning," is identified as a dominant source of anode irreversibility. To overcome this issue, nonplanar electrode architectures and thin metallic coatings are explored to accommodate fragile sodium deposits and promote good root growth, addressing poor reversibility and cell failure. Additionally, design principles for heterointerfacial alloying kinetics at metallic anodes are investigated. The crucial role of a moderate strength of chemical interaction between the deposit and substrate is revealed, enabling the highest reversibility and stability of plating/stripping redox processes. Crystallographic control is another key aspect for optimizing electrode performance. Textured electrodes formed via severe plastic deformation and optimized deposition conditions are explored to manipulate the built-in crystallographic heterogeneity of metal electrodes, resulting in significant improvements in plating/stripping performance. Collectively, this body of work contributes to the advancement of rechargeable sodium battery technologies by providing insights into alloying kinetics, electrode design strategies, and crystallographic control. The findings highlight the potential to enhance the performance of metal electrodes in sodium-based systems and beyond, fostering the development of high-performance, durable, and sustainable energy storage solutions.
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Kourkoutis, Lena