High-Performance Stimulus-Healable Sustainable Multiblock Copolymer Elastomers with Magnetothermal and Photothermal Properties

Sustainable elastomers with high strength and unique functions are highly desired yet challenging. In this work, multiblock copolymer elastomers (MBCPEs) were synthesized by two sequential reversible addition–fragmentation chain transfer polymerization procedures with polytrithiocarbonate (PTTC) as the chain transfer agent and lignin-derived monomer vanillin acrylate as the rigid segment for the glassy blocks. Furthermore, magnetite (Fe3O4) microparticles were introduced into the as-prepared MBCPE to fabricate magnetic MBCPE@Fe3O4 composite elastomers. These composite elastomers exhibit significantly enhanced mechanical properties due to the excellent interfacial interaction between the microparticles and the matrix via the Schiff-base reaction. Besides, MBCPE@Fe3O4 composite elastomers show outstanding adhesion performance, magnetothermal behavior, and photothermal properties. Under near-infrared irradiation, the composite elastomers display rapid stimulus-healing and actuating phenomena via fast photothermal conversion. The combination of sustainable MBCPEs and functional microparticles can provide great potential for the development of intelligent materials with unique stimulus-responsive applications.