Structure Property Relationship of Micellar Waterborne Poly(Urethane-Urea): Tunable Mechanical Properties and Controlled Release Profiles with Amphiphilic Triblock Copolymers

Abstract

Waterborne polyurethane (WPU) has attracted significant interest as a promising alternative to solvent-based polyurethane (SPU) due to its positive impact on safety and sustainability. However, significant limitations of WPU, such as its weaker mechanical strength, limit its ability to replace SPU. Triblock amphiphilic diols are promising materials to enhance the performance of WPU due to their well-defined hydrophobic–hydrophilic structures. Yet, our understanding of the relationship between the hydrophobic–hydrophilic arrangements of triblock amphiphilic diols and the physical properties of WPU remains limited. In this study, we show that by controlling the micellar structure of WPU in aqueous solution via the introduction of triblock amphiphilic diols, the postcuring efficiency and the resulting mechanical strength of WPU can be significantly enhanced. Small-angle neutron scattering confirmed the microstructure and spatial distribution of hydrophilic and hydrophobic segments in the engineered WPU micelles. In addition, we show that the control of the WPU micellar structure through triblock amphiphilic diols renders WPU attractive in the applications of controlled release, such as drug delivery. Here, curcumin was used as a model hydrophobic drug, and the drug release behavior from WPU-micellar-based drug delivery systems was characterized. It was found that curcumin-loaded WPU drug delivery systems were highly biocompatible and exhibited antibacterial properties in vitro. Furthermore, the sustained release profile of the drug was found to be dependent on the structure of the triblock amphiphilic diols, suggesting the possibility of controlling the drug release profile via the selection of triblock amphiphilic diols. This work shows that by shedding light on the structure–property relationship of triblock amphiphilic diol-containing WPU micelles, we may enhance the applicability of WPU systems and move closer to realizing their promising potential in real-life applications.

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“…[96][97][98] Additionally, the soft and hard segments in surfactants influences the micellar system, contingent upon the ratio of surfactants in the formulation, and has been demonstrated to affect the structural properties of the carrier, enhancing micellar packing, tuning mechanical properties, and improving interactions between oil and water interfaces. [99][100][101][102] In this study, CTD-12 chose materials such as Tween 80 (surfactants) and limonene (terpenes) as the main structural components of the nano carrier, which also served as penetration enhancers, facilitating carrier disruption of sebum, permeation through the stratum corneum, or across skin tissue layers. It is speculated that through the carrier design of CTD-12, the self-assembly characteristics enable it to maintain the shape and function of the nano carrier when penetrating the skin barrier, achieving better skin penetration through the tensile properties brought by the soft material and the lipid disturbance caused by the characteristics of the carrier material.…”