Optimizing Aqueous Processing of Nickel-Rich Cathode Material in Ultra-Thick Lithium-Ion Batteries

Lithium-ion batteries (LIBs) have been an instrumental technology since their commercialization in the 1990s. Although much progress has been made in terms of cost and efficiency of production, several challenges remain. Notably, as LIB technology continues to be applied to the transportation sector for electrified mobility in the form of electric vehicles, the question of production ethics and environmental sustainability becomes paramount. The aim of this dissertation is to address some of these concerns in the form of cathode processing techniques. This dissertation focuses on optimization of aqueous processing applied to cathode active materials. First, a study demonstrating the feasibility of aqueous processing for ultra-thick nickel-rich cathode active material via phosphoric acid addition shows both mechanical and electrochemical improvements in aqueous processed full cells. This study is then expanded upon by pursuing structured cathode designs for improved high-rate discharge capacity in ultra-thick cathodes. An improved cathode structure is identified and shown to not only be mechanically robust but also improve the utilization and energy density of the overall battery. Next, drying mechanics of aqueous cathodes are investigated in a comparative study focused on the first stage of slurry drying. A 10X increase in drying rate is identified and benefits are discussed. Finally, polymer electrolytes and the potential of aqueous processing applied to solid-state LIBs is explored and techniques for determining optimal compositions are identified.