Self-crosslinked cellulose for tough ionogel

As a natural polymer, cellulose has emerged as a promising candidate for constructing versatile materials and products due to its intrinsic biocompatibility, environmental degradability, and structural stability. As a state-of-the-art output, cellulose ionogel has demonstrated advanced applications in various scenarios in the Internet-of-Things era, while the weak mechanical strength is significantly challenging. To address this limitation, we developed a simple self-crosslinked stagey of cellulose molecules by triggering the chemical reactions of the hydroxyl and dialdehyde groups. Such chemical bonds between cellulose molecules create the tough self-crosslinked cellulose-ionogel (SCCell-ionogel), which demonstrates super high strength of 4.23 MPa with 540 % improvement, toughness of 1.36 MJ/m 3 with a 900 % increase. In addition, the resultant SCCell-ionogel also features high transmittance (93 %) and desirable biodegradation. The self-crosslinked strategy paves the way for constructing high-performance, advanced ionogel of natural polymer for next-generation smart materials. • Easy-to-prepared, chemical crosslinking of cellulose for building self-crosslinked cellulose for tough ionogel. • Cellulose ionogel features high strength and toughness. • Such a strategy enables excellent optical transparency and environmental compatibility for cellulose ionogel.