3D-Printed Thermoplastic Polyurethane Electrodes for Customizable, Flexible Lithium-Ion Batteries with an Ultra-Long Lifetime.

3D printing technology has demonstrated great potential in fabricating flexible and customizable high-performance batteries, which are highly desired in the forthcoming intelligent and ubiquitous energy era. However, a significant performance gap, especially in cycling stability, still exists between the 3D-printed and conventional electrodes, seriously limiting the practical applications of 3D-printed batteries. Here, for the first time, a series of thermoplastic polyurethane (TPU)-based 3D-printed electrodes is developed via fused deposition modeling for flexible and customizable high-performance lithium-ion batteries. The TPU-based electrode filaments in kilogram order are prepared via a facile extrusion method. As a result, the electrodes are well-printed with high dimensional accuracy, flexibility, and mechanical stability. Notably, 3D-printed TPU-LFP electrodes exhibit a capacity retention of 100% after 300 cycles at 1C, which is among the best cycling performance of all the reported 3D-printed electrodes. Such excellent performance is associated with the superb stress cushioning properties of the TPU-based electrodes that can accommodate the volume change during the cycling and thus significantly prevent the collapse of 3D-printed electrode structures. The findings not only provide a new avenue to achieve customizable and flexible batteries but also guide a promising way to erase the performance gap between 3D-printed and conventional lithium-ion batteries.