Highly Robust Fluorinated Cellulose‐Based Elastomers With Tunable Mechanical Properties Toward Strong Reusable Hot Melt Adhesives

ABSTRACT This work reports a series of fluorinated thermoplastic elastomers (FTPE) constructed by grafting on the cellulose surface through reversible addition‐fragmentation chain transfer (RAFT) polymerization. The organofluoride monomer 2,2,2‐trifluoroethyl acrylate (TFEA) was successfully grafted on microcrystalline cellulose‐based macromolecule chain transfer agent (MCC‐CTA) by RAFT polymerization and FTPE was prepared. The maximum thermal weight loss temperature of FTPE is 414.8°C under the synergistic action of the C–F bond. By changing the content of microcrystalline cellulose and acrylamide, the tensile strength of these fluorinated copolymers can be adjusted between 0.022 and 5.82 MPa, and their length can maintain a recovery rate of over 90% after multiple cycles. Meanwhile, owing to the soft rubber brushes in the side chains of MCC‐g‐P (AM‐ co ‐TFEA) and the strong cohesive force, the shear strength of the copolymer can reach 9.89 MPa when it is applied as a hot‐melt adhesive. This effective strategy can be further applied to improve the thermal and mechanical properties of bio‐based elastomer. Additionally, the design of brush topology and the adjustment of dynamic network structure can achieve better adhesion performance than the general acrylate adhesive, so as to seek to adapt to a broader application scenario.