Nonprestretching double-network enabled by physical interaction-induced aggregation

Abstract

The design of double-network (DN) improves the properties of matrix effectively, which has attracted wide attention. The recently reported construction of DN structure usually involves the prestretching process (swelling process). However, such complicated multistep swelling processes become more difficult in high molecular weight matrix, which are not suitable for constructing DN structure in the universal elastomers (for example, natural rubber and polyisoprene rubber). To expand the application fields of DN, this work designs the dense crosslinking domain and the sparse crosslinking domain to construct nonprestretching DN structure through physical interaction-induced aggregation. We find that physical interaction induced-aggregation form the dense crosslinking domain and the sparse crosslinking domain, which builds the two contrasting DN structures. Double-quantum nuclear magnetic resonance, dynamic mechanical analyzer, and mechanical property characterization demonstrate that the dense crosslinking domain as the brittle first network is preferentially ruptured upon deformation, leading to a large energy dissipation. This design concept represents a general approach to develop the nonprestretching DN structure, which expands the application fields of DN structure in the elastomer matrix.