Tunable hygromorphism: structural implications of low molecular weight gels and electrospun nanofibers in bilayer composites

Abstract

This investigation highlights the potential for electrospun nanofiber mats and self-assembled nanofiber networks to be interfaced synergistically to induce hygromorphic behaviour. Control poly(vinyl alcohol) (PVA) electrospun active layers and 1,3:2,4-di-p-methylbenyliedene sorbitol (MDBS) self-assembled passive layers encapsulated in an ethylene oxide–epichlorohydrin (EO–EPI) copolymer matrix were fabricated to examine the influence of composition on the properties guiding hygromorphism, such as water transport, layer thickness, and layer modulus. Experimentally determined material constants were utilized in conjunction with mathematical modeling to determine ideal layer properties. It was revealed that the active layer with the highest PVA content exhibited the fastest water transport, and the passive layer with the highest MDBS content displayed the slowest water transport. However, the hygromorphic bilayer fabricated utilizing the lowest PVA content and the highest MDBS fraction was predicted to induce the highest change in curvature due to the lower modulus and thickness of the PVA nanofiber active layer. Decreasing the MDBS content reduced the passive layer modulus while increasing water transport, which theoretically reduced the overall bilayer curvature. The hygromorphic bilayer composites fabricated using these ideal control layers exhibited folding bias and response variations dependent upon active layer composition and imposed folding directions. By utilizing the favorable force balances between the active layer with the lower PVA content and the passive layer with the highest MDBS amount in conjunction with folding bias in a non-preferential direction, it was possible to achieve hygromorphic unfolding and refolding with hydration. Through modelling and individual layer examination, a unique platform built on two independent fiber networks has been designed to achieve biomimetic hygromorphism in synthetic bilayer composites.