Significant Performance Enhancement of Polymer Resins by Bioinspired Dynamic Bonding

Marine mussels use catechol-rich interfacial mussel foot proteins (mfps) as primers that attach to mineral surfaces via hydrogen, metal coordination, electrostatic, ionic, or hydrophobic bonds, creating a secondary surface that promotes bonding to the bulk mfps. Inspired by this biological adhesive primer, it is shown that a ≈1 nm thick catecholic single-molecule priming layer increases the adhesion strength of crosslinked polymethacrylate resin on mineral surfaces by up to an order of magnitude when compared with conventional primers such as noncatecholic silane- and phosphate-based grafts. Molecular dynamics simulations confirm that catechol groups anchor to a variety of mineral surfaces and shed light on the binding mode of each molecule. Here, a ≈50% toughness enhancement is achieved in a stiff load-bearing polymer network, demonstrating the utility of mussel-inspired bonding for processing a wide range of polymeric interfaces, including structural, load-bearing materials.

All current load-bearing composites use covalent bonds to bridge between mineral and resin surfaces, thereby increasing hardness but compromising extensibility. Translating the dynamic bonds found in biology to manmade materials has only been attempted in the context of soft synthetic materials, such as elastomers. It is shown that dynamic bonds can increase toughness in a manmade load-bearing system.

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