Unlike biological materials that can sense mechanical force and actively remodel locally,synthetic polymers typically break down under stress.Molecular-level responses to damage with both stress-reporting and self-str...Unlike biological materials that can sense mechanical force and actively remodel locally,synthetic polymers typically break down under stress.Molecular-level responses to damage with both stress-reporting and self-strengthening functions are significant yet difficult to realize for synthetic polymers.To overcome this challenge,chemo-mechanical coupling into polymers that can simultaneously ameliorate mechanical,optical,or other functional properties of a polymer combined with mechanical treatment will offer a new principle for materials design.Here,we report a kind of elastomer in which destructive forces are channelled into productive and bond-forming reactions by using diselenide(Se–Se)as a mechanophore.Polyurethane has been functionalized with labile Se–Se bonds,whosemechanical activation generates seleno radicals that trigger radical transfer and cross-linking reactions in situ.These reactions are activated efficiently in a mechanical way by compression in bulk materials.The resulting covalent networks possess turn-on mechano-fluorescence and increased moduli,which provide the functions of stress reporting,mechano-healing,and mechano-remodeling for the deformed film.This study not only illuminates themechano-responsive nature of Se–Se bonds in the bulk state but also paves the way for the development of new stress-responsive materials.展开更多
基金support of this research by the National Natural Science Foundation of China(grant nos.21734006 and 21975178)the National Key Research and Development Program of China(grant nos.2017YFA0207800 and 2017YFA0204503)is gratefully acknowledged.
文摘Unlike biological materials that can sense mechanical force and actively remodel locally,synthetic polymers typically break down under stress.Molecular-level responses to damage with both stress-reporting and self-strengthening functions are significant yet difficult to realize for synthetic polymers.To overcome this challenge,chemo-mechanical coupling into polymers that can simultaneously ameliorate mechanical,optical,or other functional properties of a polymer combined with mechanical treatment will offer a new principle for materials design.Here,we report a kind of elastomer in which destructive forces are channelled into productive and bond-forming reactions by using diselenide(Se–Se)as a mechanophore.Polyurethane has been functionalized with labile Se–Se bonds,whosemechanical activation generates seleno radicals that trigger radical transfer and cross-linking reactions in situ.These reactions are activated efficiently in a mechanical way by compression in bulk materials.The resulting covalent networks possess turn-on mechano-fluorescence and increased moduli,which provide the functions of stress reporting,mechano-healing,and mechano-remodeling for the deformed film.This study not only illuminates themechano-responsive nature of Se–Se bonds in the bulk state but also paves the way for the development of new stress-responsive materials.