Sustainable Multiblock Copolymer Elastomers Derived from Lignin with Tunable Performance toward Strong Adhesives and UV-Shielding Materials

With the increasing concern about global environmental issues, reducing the carbon footprint to achieve carbon neutrality has been particularly important. Sustainable multiblock copolymer elastomers (MBCPEs) have received tremendous interest due to their unprecedented performance and huge potential applications. However, complex multistep polymerization and postpolymerization processes are needed to design MBCPEs. In this work, a series of MBCPEs, in which vanillin acrylate (VA) derived from lignin was selected as the renewable rigid segments for the glassy block, while methyl acrylate (MA) was chosen as the soft segments for the rubbery block, were prepared by two successive reversible addition–fragmentation chain transfer (RAFT) polymerization processes with polytrithiocarbonate (PTTC). These thermally stable MBCPEs exhibit distinct microphase-separated morphology, where the hard poly(vanillin acrylate) (PVA) blocks self-assemble into discrete glassy domains serving as the physical cross-linking points in the soft poly(methyl acrylate) (PMA) matrix. The macroscopic mechanical performance, such as tensile strength, stretchability, toughness, and elastic recovery, can be adjusted well by changing the molecular weights and PVA contents. Moreover, these sustainable MBCPEs can be applied as strong adhesives and excellent UV-shielding materials, broadening their potential applications. This novel strategy is convenient and robust by combining RAFT polymerization and renewable resources toward high-performance MBCPEs, which can open a new avenue for the development of sustainable biobased elastomers.