Asynchronous Ring Opening of Cyclic Carbonate and Glycidyl Ether Induced Phase Evolution Towards Heat‐free and Rapid‐bonding Superior Epoxy Adhesive

Structural adhesives that do not require heating are in high demand in the automotive and electronics industries. However, it remains a challenge to develop robust adhesives that rapidly achieve super adhesion near ambient temperature. Herein, a room‐temperature curable, fast‐bonding, and super strong epoxy‐based structural adhesive was designed from the perspective of cross‐scale structure, which lies in threefold pivotal aspects: (i) high branching topology of glycerol carbonate‐capped polyurethane (PUGC) increases the kinetics of the ring‐opening reaction, contributing to fast crosslinking and the formation of abundant urethane and hydroxyl moieties; (ii) asynchronous crosslinking of epoxy and PUGC synergistically induces phase separation of PUGC within the epoxy resin and the resulting PUGC domains surrounded by interpenetrated shell serves to efficiently toughen the matrix; (iii) abundant dynamic hydrogen bonds including urethane and hydroxyl moieties, along with the elastomeric PUGC domains, dissipate energy of shearing force. As a result, the adhesive strength rapidly grows to 16 MPa within 4 hours, leveling off to 21 MPa after 7 hours, substantially outperforming commercial room‐temperature curable epoxy adhesives. The results of this study could advance the field of high‐performance adhesives and provide valuable insights into designing materials for efficient curing at room temperature.