Ionically Conductive Self‐Healing Binder for Low Cost Si Microparticles Anodes in Li‐Ion Batteries

Abstract A self‐healing polymer (SHP) with abundant hydrogen bonds, appropriate viscoelasticity, and stretchability is a promising binder to improve cycle performance of Si microparticle anodes in lithium (Li) ion batteries. Besides high capacity and long cycle life, efficient rate performance is strongly desirable for practical Si anode implementation. Here, polyethylene glycol (PEG) groups are incorporated into the SHP, facilitating Li ionic conduction within the binder. The concept of the SHP‐PEG binder involves improving the interface between Si microparticles and electrolytes after cycling based on the combination of self‐healing ability and fast Li ionic conduction. Through the systematic study of mixing PEG Mw and ratio, the polymeric binder combining SHP and PEG with M w 750 in an optimal ratio of 60:40 (mol%) achieves a high discharging capacity of ≈2600 mA h g −1 , reasonable rate performance especially when >1C and maintains 80% of their initial capacity even after ≈150 cycles at 0.5C. The described concept for the polymeric binder, embedding both self‐healing ability and high Li ionic conductivity, should be equally useful for next generation batteries utilizing high capacity materials which suffer from huge volume change during cycling.