Authors: Binbin Yang, Chenglong Deng, Nan Chen, Fengling Zhang, Kaikai Hu, Boshun Gui, Liyuan Zhao, Feng Wu, Renjie Chen
Published: 2024-04-07
Source: Full article
AbstractComposite polymer solid electrolytes (CPEs), possessing good rigid flexible, are expected to be used in solid‐state lithium‐metal batteries. The integration of fillers into polymer matrices emerges as a dominant strategy to improve Li+ transport and form a Li+‐conducting electrode–electrolyte interface. However, challenges arise as traditional fillers: 1) inorganic fillers, characterized by high interfacial energy, induce agglomeration; 2) organic fillers, with elevated crystallinity, impede intrinsic ionic conductivity, both severely hindering Li+ migration. Here, a concept of super‐ionic conductor soft filler, utilizing a Li+ conductivity nanocellulose (Li‐NC) as a model, is introduced which exhibits super‐ionic conductivity. Li‐NC anchors anions, and enhances Li+ transport speed, and assists in the integration of cathode–electrolyte electrodes for room temperature solid‐state batteries. The tough dual‐channel Li+ transport electrolyte (TDCT) with Li‐NC and polyvinylidene fluoride (PVDF) demonstrates a high Li+ transfer number (0.79) due to the synergistic coordination mechanism in Li+ transport. Integrated electrodes’ design enables stable performance in LiNi0.5Co0.2Mn0.3O2|Li cells, with 720 cycles at 0.5 C, and 88.8% capacity retention. Furthermore, the lifespan of Li|TDCT|Li cells over 4000 h and Li‐rich Li1.2Ni0.13Co0.13Mn0.54O2|Li cells exhibits excellent performance, proving the practical application potential of soft filler for high energy density solid‐state lithium‐metal batteries at room temperature.