Synthesis of high-strength microcrystalline cellulose hydrogel by viscosity adjustment

Developing hydrogels with enhanced mechanical strength is desirable for bio-related applications. For such applications, cellulose is a notable biopolymer for hydrogel synthesis due to its inherent strength and stiffness. Here, we report the viscosity-adjusted synthesis of a high-strength hydrogel through the physical entanglement of microcrystalline cellulose (MCC) in a solvent mixture of tetrabutylammonium fluoride/dimethyl sulfoxide (TBAF/DMSO). MCC was strategically dissolved with TBAF in DMSO at a controlled ratio to induce the formation of a liquid crystalline phase (LCP), which was closely related to the viscosity of the cellulose solution. The highest viscosity was obtained at 2.5% MCC and 3.5% TBAF, leading to the strongest high-strength MCC hydrogel (strongest HS-MCC hydrogel). The resulting hydrogel exhibited a high compressive strength of 0.38 MPa and a densely packed structure. Consequently, a positive linear correlation was determined between the viscosity of the cellulose solution and the mechanical strength of the HS-MCC hydrogel.