Scalable Pore Engineering Strategy for Promoting Ion Transport and Rate Capability in Thick Li-Ion Battery Electrodes

Since the first commercialization of lithium-ion batteries (LIBs) in the early 1990s, previous research has been extensive on electrode material development. Due to its high volumetric energy and power densities and its low cost, the LIBs have aided in the widespread adoption of advanced mobile electronic devices, slowly spurred the market penetration of electric vehicles (EVs) globally and been incorporated in household energy storage systems to promote efficient use of renewable energy1,2. Unfortunately, after rapid improvements in LIB technology, the present progress in increasing energy density and reducing the costs of LIBs has been slow. To overcome the performance limitations on the material side, increasing the nickel (Ni) content of layered lithium nickel cobalt aluminum oxide (NCA) and lithium nickel cobalt manganese oxide (NCM) cathode materials and blending silicon with graphite anode materials have shown promise3,4,5. On the manufacturing side, there is a push to use thicker and denser electrodes and increase areal capacity loadings from 3-4 mAh/cm2 to 5-7 mAh/cm2 to reduce the mass and volume fraction of inactive materials and thus reduce costs and improve the energy density and specific energy of LIB cells beyond about 700 Wh/L and 250 Wh/kg, respectively6.-8 . Unfortunately, the characteristic Li+ ion diffusion time is proportional to the square of the average diffusion path through the electrode, which depends on both the electrode thickness and the tortuosity. As a result, the charging time and power performance characteristics in high-loading, dense electrodes may become undesirably poor. Herein, we report on several manufacturing pathways to create straight channel pores within electrodes to accelerate electrolyte wetting and facilitate rapid ion transport to overcome these rate limitations. References: Armand, M. & Tarascon, J.-M. Building Better Batteries. Nature 451, 652–657 (2008). Larcher, D. & Tarascon, J.-M. Towards greener and more sustainable batteries for Electrical Energy Storage. Nature Chemistry 7, 19–29 (2014). Manthiram, A., Knight, J. C., Myung, S.-T., Oh, S.-M. & Sun, Y.-K. Nickel-rich and lithium-rich layered oxide cathodes: Progress and perspectives. Advanced Energy Materials 6, 1501010 (2015). Liu, W. et al. Nickel-rich layered lithium transition-metal oxide for high-energy lithium-ion batteries. Angewandte Chemie International Edition 54, 4440–4457 (2015). Eshetu, G. G. et al. Production of high-energy Li-ion batteries comprising silicon-containing anodes and insertion-type cathodes. Nature Communications 12, (2021). Kuang, Y., Chen, C., Kirsch, D. & Hu, L. Thick electrode batteries: Principles, opportunities, and challenges. Advanced Energy Materials 9, 1901457 (2019). Patry, G., Romagny, A., Martinet, S. & Froelich, D. Cost modeling of lithium‐ion battery cells for Automotive Applications. Energy Science & Engineering 3, 71–82 (2014). Turcheniuk, K., Bondarev, D., Amatucci, G. G. & Yushin, G. Battery materials for low- cost electric transportation. Materials Today 42, 57–72 (2021).