Consecutive 3D-printed layered cathodes with anisotropic ion transport networks for ultrahigh-areal-capacity lithium-ion batteries

High-performance thick electrodes are regarded as a feasible strategy for enhancing the energy density of lithium-ion batteries. However, fast ion transport and long-life cyclability in thick cathode remain significant challenges. Here, we developed a multidirectional-ion-transport Ni-rich thick cathode LiNi0.8Co0.1Mn0.1O2 (NCM811), which exhibits excellent consecutive layer-by-layer contact and fast ion-flow diffusion, achieving high areal capacity and superior rate capability toward 3D-printed batteries. By balancing the viscosity of electrode inks and mechanical strength of thick electrodes, a multilayer NCM811 cathode with strong interfacial bonding, reaching an electrode thickness of 3 mm and ultra-high mass loading of 185 mg cm−2, delivers a record areal capacity of 38.4 mAh cm−2 up to date. The 3D-printed porous frameworks featuring the multidirectional transport of Li ion and superior affinity of electrolyte, exceptionally boost active material utilization and fast electrochemical kinetics of thick electrodes, resulting in a high specific capacity of 208 mAh g−1. Furthermore, the printed electrode has a capacity retention rate of 88% after 150 cycles at 2 C. A full cell assembled with a printed NCM811 cathode and graphite anode shows high energy density of 417 Wh kg−1 at electrode level and long-term cyclability. This work provides an effective strategy for fabricating long-lifespan and high-energy-density lithium-ion batteries.