Ultrafast Self‐Healing Elastomer with Closed‐Loop Recyclability

Abstract The loss of function after prolonged periods of use is inevitable for all materials including plastics. Hence, self‐healing capabilities are a key development to prolong the service lifetime of materials. One of such self‐healing capabilities can be achieved by integrating dynamic bonds such as boronic ester linkages into polymeric materials, however the rate of self‐healing in these materials is insufficient and current methods to accelerate it are limited. In this study, we report the rational design, synthesis and characterization of a fluorinated elastomer (FBE15) that utilizes enhanced interaction between polymer chains afforded by strong dipole‐dipole interactions from −CF 3 , which showed a significant increase in binding energy to −7.71 Kcal/mol from −5.51 Kcal/mol, resulting in increased interaction between the boronic ester linkages and improving self‐healing capabilities of boronic ester materials, drastically reducing the time required for stress relaxation by 900 %. The bulk elastomer is capable of ultrafast self‐healing in a one‐click fashion that can happen in mere seconds, which can then be stretched to 150 % of its original length. By utilising the dynamic cross‐linking, FBE15 is also capable of both mechanical reprocessing into the same materials and chemical recycling into its starting materials, respectively, further allowing reconstruction of the elastomers that have comparable properties to the original ones at the end of its service lifespan.