ABSTRACT
Poly(2,2,6,6-tetramethyl-1-piperidinyloxy methacrylate) (PTMA) is one of the most promising organic cathode materials thanks to its relatively high redox potential, good rate performance, and cycling stability. However, being a p-type material, PTMA-based batteries pose additional challenges compared to conventional lithium-ion systems due to the involvement of anions in the redox process. This study presents a comprehensive approach to optimize such batteries, addressing challenges in electrode design, scalability, and cost. Experimental results at a laboratory scale demonstrate high active mass loadings of PTMA electrodes (up to 9.65 mg cm-2), achieving theoretical areal capacities that exceed 1 mAh cm-2. Detailed physics-based simulations and cost and performance analysis clarify the critical role of the electrolyte and the impact of the anion amount in the PTMA redox process, highlighting the benefits and the drawbacks of using highly concentrated electrolytes. The cost and energy density of lithium metal batteries with such high mass loading PTMA cathodes were simulated, finding that their performance is inferior to batteries based on inorganic cathodes even in the most optimistic conditions. In general, this work emphasizes the importance of considering a broader perspective beyond the lab scale and highlights the challenges in upscaling to realistic battery configurations.
