Tough, Highly Oriented, Super Thermal Insulating Regenerated All-Cellulose Sponge-Aerogel Fibers Integrating a Graded Aligned Nanostructure.

Thermal insulating fibers can effectively regulate the human body temperature and decrease indoor energy consumption. However, designing super thermal insulating fibers integrating a sponge and aerogel structure based on biomass resources is still a challenge. Herein, a flow-assisted dynamic dual-cross-linking strategy is developed to realize the steady fabrication of regenerated all-cellulose graded sponge-aerogel fibers (CGFs) in a microfluidic chip. The chemically cross-linked cellulose solution is used as the core flow, which is passed through two sheath flow channels, containing either a diffusion solvent or a physical cross-linking solvent, resulting in CGFs with a porous sponge outer layer and a dense aerogel inner layer. By regulating and simulating the flow process in the microfluidic chip, CGFs with adjustable sponge thicknesses, excellent toughness (26.20 MJ m -3 ), and ultralow thermal conductivity (0.023 W m -1 K -1 ) are fabricated. This work provides a new method for fabricating graded biomass fibers and inspires attractive applications for thermal insulation in textiles.