Patterned Nanostructures on Cathodes: A Pathway to Stronger, High-Energy, High-Power Li-Ion Batteries

Conventional cathodes are produced by layering materials on flat, two-dimensional substrates, imposing a trade-off between capacity retention, energy and power output, and mechanical stability. Herein, we employ programmable spray-deposition manufacturing to introduce flexibility through enabling form factors and tailored morphological nanostructures to overcome this limitation. This tailorability is achieved by creating distinct patterns─disk and ring formations─on the electrode using spray-deposition. The pattern formation is controlled by the self-assembly of lithium iron phosphate (LFP) and reduced graphene oxide (rGO), mixed at tailored mass ratios, and deposited using an in-house spray system onto an aluminum current collector. We show that when active materials are assembled into repeatable, spatially controlled patterned architecture, the resulting structure amplifies certain functionalities such as capacity retention, energy, and power density or interfacial adhesion and structural cohesion. Specifically, disk-patterned cathodes exhibit lower charge transfer resistance, faster kinetics, higher energy and power density, and cyclic stability, whereas ring-patterned cathodes provide superior interfacial adhesion and cohesion compared to disk-patterned cathodes. Interestingly, combining both patterns yields a cathode that simultaneously exhibits superior capacity, cyclic stability, and interfacial adhesion compared with either the disk- or ring-patterned configurations alone. We use molecular dynamics to show that the disk pattern's superior ion mobility and diffusion kinetics come with a higher chance of trapping lithium ions, whereas the less dense ring pattern, though lower in capacity, can preserve it over longer cycles. Strategically integrating these patterns enables a synergistic multifaceted cathode design to overcome classical engineering trade-offs between electrochemical functionality and mechanical stability.