There is a growing demand for the utilization of sustainable materials, such as cellulose-based alternatives, over fossil-based materials. However, the inherent drawbacks of cellulosic materials, such as extremely low wet strength and resistance to moisture, need significant improvements. Moreover, several of the commercially available wet-strength chemicals and hydrophobic agents for cellulosic material treatment are toxic or fossil-based (e.g., epichlorohydrin and fluorocarbons). Herein, we present an eco-friendly, high-yield, industrially relevant, and scalable method inspired by birch bark for fabricating hydrophobic and strong cellulosic materials. This was accomplished by combining simple surface modification of cellulosic fibers in water using colloidal particles of betulin, an abundant triterpene extracted from birch bark, with sustainable chemical engineering (e.g., lignin modification and hot-pressing). This led to a transformative process that not only altered the morphology of the cellulosic materials into a more dense and compact structure but also made them hydrophobic (contact angles of up to >130°) with the betulin particles undergoing polymorphic transformations from prismatic crystals (betulin III) to orthorhombic whiskers (betulin I). Significant synergistic effects are observed, resulting in a remarkable increase in wet strength (>1400%) of the produced hydrophobic cellulosic materials.
© 2024 The Authors. Published by American Chemical Society.