Mechanically Robust and Recyclable EPDM Rubber Composites by a Green Cross-Linking Strategy

Covalently cross-linked rubbers are indispensable in many important fields due to their unique entropic elasticity. For rubbers cross-linking, the addition of toxic curing agents, release of toxic volatile organic compounds (VOCs), and recycling of waste rubber are three important issues. A combination of green curing chemistry and efficient recycling into commercial polyolefin rubbers is of great importance. Herein, we demonstrate a facile and promising way to incorporate dynamic covalent bonds into ethylene-propylene-diene monomer (EPDM)/carbon black (CB) composites. The epoxy-functionalized EPDM (e-EPDM) was prepared using an in situ epoxidation reaction and then cured with biobased decanedioicacid (DA) through the reactions between the epoxy groups in e-EPDM and the carboxylic groups in DA. Because of the existence of exchangeable β-hydroxyl ester, the covalently cross-linked networks in e-EPDM/CB composites were able to rearrange their topological structure at high temperature, endowing the composites with recycled and reshaped abilities. More importantly, the recycled e-EPDM/CB composites still exhibit outstanding mechanical properties which can meet the needs of practical applications. This strategy may provide an efficient, green, and sustainable way to address the problems brought from rubbers cross-linking.