Abstract
The integration of polymer materials with self-healing features into advanced lithium batteries is a promising and attractive approach to mitigate degradation and, thus, improve the performance and reliability of batteries. Polymeric materials with an ability to autonomously repair themselves after damage may compensate for the mechanical rupture of an electrolyte, prevent the cracking and pulverization of electrodes or stabilize a solid electrolyte interface (SEI), thus prolonging the cycling lifetime of a battery while simultaneously tackling financial and safety issues. This paper comprehensively reviews various categories of self-healing polymer materials for application as electrolytes and adaptive coatings for electrodes in lithium-ion (LIBs) and lithium metal batteries (LMBs). We discuss the opportunities and current challenges in the development of self-healable polymeric materials for lithium batteries in terms of their synthesis, characterization and underlying self-healing mechanism, as well as performance, validation and optimization.