Stress-Tolerant Printed Architectures Toward Stable Cycling of Ultrahigh-Loading Ni-Rich Layered Oxide Cathodes for Wearable Energy Storage Devices

Fast-charging and high-energy density wearable energy storage devices working under high mass loading are in urgent demand for the state-of-the-art devices. However, the slow reaction kinetics and sluggish ion diffusion still impede their authentic commercialization. Herein, a thick and robust Ni-rich LiNi_0.8Co_0.1Mn_0.1O₂(NCM811) layered oxide cathode grid-structured electrode is developed using a three-dimensional (3D) direct ink writing (DIW) technique. On the strength of the 3D interconnected channels and conductive scaffolds, both the wettability and the Li⁺ion/electron transfer in the electrode are enhanced, which improves the utilization of active materials during the charging and discharging process. As expected, the 3D-printed (3DP) LiNi_0.8Co_0.1Mn_0.1O₂(NCM811) grid-structured electrode delivers a high areal capacity of 7.48 mAh cm^-2(∼200 mAh g^-1) even at an ultrahigh mass loading of 36.6 mg cm^-2and a low capacity fading of 0.22% per cycle after 100 cycles at 200 mA g^-1. A customized cell module composed of the 3DP NCM811 grid-structured thick cathode and the 3DP artificial graphite grid-structured thick anode, coupled with the ultralow-power offline artificial intelligence electronic module, can power smart glasses and realize augmented-reality time display. The 3D extrusion technique provides a new venue for future smart, flexible, and wearable electrons.