Superfast, large-scale harvesting of cellulose molecules via ethanol pre-swelling engineering of natural fibers

Cellulose molecules, as the basic unit of biomass cellulose, have demonstrated advancements in versatile engineering and modification of cellulose toward sustainable and promising materials in our low-carbon society. However, harvesting high-quality cellulose molecules from natural cellulosic fibers (CF) remains challenging due to strong hydrogen bonds and unique crystalline structure, which limit solvents (such as ionic liquid, IL) transport and diffusion within CF, making the process energy/time-intensively. Herein, we superfast and sustainably engineer biomass fibers into high-performance cellulose molecules via ethanol pre-swelling of CF followed by IL treatment in the microwave (MW) system. Ethanol-pre-swelled cellulosic fibers (SCF) feature modified morphological and structural distinctions, with improved fiber width, pore size, and specific surface area. The ethanol in the SCF structure is appropriately removed through MW heating and cooling, leaving transport and diffusion pathways of IL within the SCF. Such strategy enables the superfast (140 s) and large-scale (kilogram level) harvesting of cellulose molecules with high molecular weight, resulting in high-performance, versatile cellulose ionogel with a 300 % increase in strength and 1027 % in toughness, monitoring human movement, external pressure, and temperature. Our strategy paves the way for time/energy-effectively, sustainably harvesting high-quality polymer molecules from natural sources beyond cellulose toward versatile and advanced materials.