Intrinsic Self-healing Supramolecular Materialsbased On Polyphase Hydrogen Bonding

Self-healing polymers with microphase-separated structure are plagued with inferior self-healing efficiency at room temperature due to lack of dynamic interactions in hard domains.Herein,we describe a novel strategy of multiphase active hydrogen bonds(H-Bonds),toward real-izing fast and efficient self-healing at room temperature,even under harsh conditions.The core conception is to incorporate thiourea moieties into microphase-separated polyurea network to form multistrength H-bonds,which destroy the crystallization of hard domains,and at the same time,inserted the dynamic reversible H-bonds in both hard and soft segments,accounting for the surprisingly self-healing performances.The synthesized polymeric material,PDMS-MPI-TM completely recovers all the mechanical properties within 4 h at room temperature after rupture.Significantly,self-healing process can also take place at low temperature(restoration with 85% efficiency in48 h at-20 ?)or in the water(restoration with 95% efficiency in 4 h).Depending on the cleavage/re-formation of multiphase H-bonds,the material exhibits the unprecedented ultrastrechability and notch-insensitiveness.It can be stretched up to 31500% without fracture,and reach notch-insensitive stretching up to 15000%.These exceptional characteristics inspired us to fabricate highly stretchable self-healable underwater conductor and protective self-healing film for suppressing shuttling of polysulfides and preventing crack propagation in S cathode,which provide the path-way for applications in underwater electronic devices or advanced Li-S batteries.