A universal strategy for decoupling stiffness and extensibility of polymer networks

TL;DR

This paper introduces a universal method to independently control the stiffness and extensibility of polymer networks using foldable bottlebrush polymers, overcoming the traditional trade-off between these properties.

Contribution

The study presents a novel approach employing foldable bottlebrush polymers to decouple stiffness and extensibility in single-network elastomers, enabling high stretchability without sacrificing stiffness.

Findings

Achieved nearly constant Young's modulus while increasing tensile strain by 40-fold.

Validated the strategy across different polymer species and network topologies.

Demonstrated potential for designing polymer networks with exceptional mechanical properties.

Abstract

Since the invention of polymer networks in the 19th century (e.g., crosslinked natural rubber by Goodyear), it has been a dogma that stiffer networks are less stretchable, a trade-off inherent to the molecular nature of polymer network strands. Here, we report a universal strategy for decoupling the stiffness and extensibility of single-network elastomers. Instead of using linear polymers as network strands, we use foldable bottlebrush polymers, which feature a collapsed backbone grafted with many linear side chains. Upon elongation, the collapsed backbone unfolds to release stored length, enabling remarkable extensibility. By contrast, the network elastic modulus is inversely proportional to the network strand mass and is determined by the side chains. We validate this concept by creating a series of unentangled single-network elastomers with nearly constant Young's modulus (30 kPa) while increasing tensile breaking strain by 40-fold, from 20% to 800%. We show that this strategy applies to networks of different polymer species and topologies. Our discovery opens an avenue for developing polymer networks with extraordinary mechanical properties.