The combination of excellent mechanical performances, high reprocess efficiency, and wide-range tunability for functional dynamic siloxane materials is a challenging subject. Herein, the fabrication of mechanically strong, autonomous self-healing, and fully recyclable silicone elastomers with unique photoluminescent properties by coordination of poly(dimethylsiloxane) (PDMS) containing coordination bonding motifs with Zn 2+ ions is reported. Salicylaldimine groups, which are introduced into the polysiloxane backbone via mild Schiff-base reaction, coordinate with zinc ions to form elastomeric networks The obtained supramolecular elastomers have excellent mechanical properties, with the optimized tensile strength up to 10.0 MPa, which is unprecedented among the reported thermoplastic polysiloxane-based elastomers. Both mechanical properties and stress relaxation kinetics are tunable via adjusting the length of PDMS segments or the molar ratio of metal versus salicylaldimine. Furthermore, these elastomers can be conveniently healed and recycled to regain their original mechanical properties and integrity under mild conditions. In addition, this new kind of polysiloxane also exhibits coordination-enhanced fluorescence, showing great promise for preparing photoluminescent elastomers or coatings.

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