Vapor-phase synthesis of a reagent-free self-healing polymer film with rapid recovery of toughness at room temperature and under ambient conditions

A rapidly self-healable polymer is highly desirable but challenging to achieve. Herein, we developed an elastomeric film with instant self-healing ability within 10 s at room temperature. For this purpose, a series of copolymers of poly(glycidyl methacrylate- co -2-hydroxyethyl acrylate) (poly(GMA- co -HEA), or pGH) were synthesized in the vapor phase via an initiated chemical vapor deposition (iCVD) process. The elastomer includes a large amount of hydroxyl groups in the 2-hydroxyethyl acrylate (HEA) moiety capable of forming rapid, reversible hydrogen bonding at room temperature, while glycidyl methacrylate (GMA) with a rigid methacrylic backbone chain in the copolymer provides mechanical robustness to the elastic copolymer. With the optimized copolymer composition, pGH indeed showed instant recovery of the toughness within a minute; a completely divided specimen could be welded within a minute at room temperature and under ambient conditions simply by placing the pieces in close contact, which showed the outstanding recovery performance of elastic modulus (93.2%) and toughness (15.6 MJ m −3 ). The rapid toughness recovery without supplementing any external energy or reagents ( e.g. light, temperature, or catalyst) at room temperature and under ambient conditions will be useful in future wearable electronics and soft robotics applications. A rapidly self-healable polymer was synthesized via iCVD process, and this polymer showed rapid recovery of mechanical properties in the ambient condition.