Implementing self-healing capabilities in a deformable platform is one of the critical challenges for achieving future wearable electronics with high durability and reliability. Conventional systems are mostly based on polymeric materials, so their self-healing usually proceeds at elevated temperatures to promote chain flexibility and reduce healing time. Here, we propose an ion-cluster-driven self-healable ionoconductor composed of rationally designed copolymers and ionic liquids. After complete cleavage, the ionoconductor can be repaired with high efficiency (∼90.3%) within 1 min even at 25 °C, which is mainly attributed to the dynamic formation of ion clusters between the charged moieties in copolymers and ionic liquids. By taking advantages of the superior self-healing performance, stretchability (∼1130%), non-volatility (over 6 months), and ability to be easily shaped as desired through cutting and re-assembly protocol, reconfigurable, deformable light-emitting electroluminescent displays are successfully demonstrated as promising electronic platforms for future applications.
14 November 2019 in ACS Applied Materials & Interfaces
A facile random copolymer strategy based on poly(styrene-ran-methyl methacrylate) (PS-r-PMMA) is proposed for the preparation of highly conductive and mechanically elastic solid-state gel electrolytes. In contrast to previous random copolymers serving as polymer hosts, PS-r-PMMA can be readily synthesized by one-pot reversible additional–fragmentation chain transfer (RAFT) polymerization. PS-r-PMMA and the ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMI][TFSI]) are blended to fabricate physically cross-linked ion gel electrolytes. We systematically investigate the dependence of gel properties on experimental variables, such as the styrene fraction and molecular weight of PS-r-PMMAs, and the ion gel composition. The physical properties of the gels are optimized to simultaneously exhibit good ionic conductivity (∼0.98 mS cm−1) and mechanical resilience (∼7.2 × 104 Pa) at room temperature. The versatility of the PS-r-PMMA-based gels as a solid-state electrolyte platform is successfully demonstrated by applying it in two types of electrochemical devices, electrochemiluminescent (ECL) and electrochromic (EC) displays. These results imply that PS-r-PMMAs can be easily synthesized without post reactions and are a simple and effective polymer host for high-performance ion gel electrolytes for diverse electrochemical applications.