Abstract
Solid-state batteries are increasingly centre-stage for delivering more energy-dense, safer batteries to follow current lithium-ion rechargeable technologies. At the same time, wearable electronics powered by flexible batteries have experienced rapid technological growth. This perspective discusses the role that polymer design plays in their use as solid polymer electrolytes (SPEs) and as binders, coatings and interlayers to address issues in solid-state batteries with inorganic solid electrolytes (ISEs). We also consider the value of tunable polymer flexibility, added capacity, skin compatibility and end-of-use degradability of polymeric materials in wearable technologies such as smartwatches and health monitoring devices. While many years have been spent on SPE development for batteries, delivering competitive performances to liquid and ISEs requires a deeper understanding of the fundamentals of ion transport in solid polymers. Advanced polymer design, including controlled (de)polymerisation strategies, precision dynamic chemistry and digital learning tools, might help identify these missing fundamental gaps towards faster, more selective ion transport. Regardless of the intended use as an electrolyte, composite electrode binder or bulk component in flexible electrodes, many parallels can be drawn between the various intrinsic polymer properties. These include mechanical performances, namely elasticity and flexibility; electrochemical stability, particularly against higher-voltage electrode materials; durable adhesive/cohesive properties; ionic and/or electronic conductivity; and ultimately, processability and fabrication into the battery. With this, we assess the latest developments, providing our views on the prospects of polymers in batteries and wearables, the challenges they might address, and emerging polymer chemistries that are still relatively under-utilised in this area.