Self-Healable, Highly Stretchable, Ionic Conducting Polymers as Efficient Protecting Layers for Stable Lithium-Metal Electrodes

Although numerous studies on polymeric protective films to stabilize lithium (Li)-metal electrodes have been reported, the construction of self-healing polymers that enables the longterm operation of Li-metal batteries (LMBs) at relatively low temperatures has rarely been demonstrated. Herein, a highly stretchable, autonomous self-healable, and ionic-conducting polymer network (SHIPN) is synthesized as an efficient protective film for LMBs. The network backbone, synthesized from copolymerization of poly(ethylene glycol)-mono-methacrylate (PEGMMA) and 2-[[(butylamino)carbonyl]oxy]ethyl acrylate (BCOE), is chemically cross-linked via diisocyanate. With SHIPN-modified electrodes, enhanced electrochemical performance can be achieved in Li/Cu, Li/Li, and Li/LiFePO4 (Li/LFP) cells. The SHIPN@Li/LFP cell delivers a capacity retention of 85.6% after 500 cycles at 5 degrees C, resulting from the low-temperature self-healability of SHIPN. In full cells with a high-mass-loading LFP cathode (similar to 17 mg cm-2), the capacity retention is at least 300% higher than that with a bare Li electrode. Further physical characterizations of electrodes confirm the effect of SHIPN in enhancing the interfacial stability and suppressing Li dendrite growth. Our results will provide insights into rationally designing soft and hybrid materials toward stable LMBs at different temperatures.

Automated summary

In this study, a highly stretchable, autonomous self-healable, and ionic-conducting polymer network (SHIPN) was synthesized as a protective film for lithium metal batteries (LMBs). The SHIPN-modified electrodes exhibited improved electrochemical performance in various LMB systems. The physical characterizations confirmed the effect of SHIPN in enhancing interfacial stability and suppressing lithium dendrite growth.