The Impact of Hydrogen Bond Basicity of Ionic Liquids on Cotton Cellulose Dissolution: Experimental and Simulation Study

This study explores the influence of anion hydrogen-bond basicity, quantified by the Kamlet–Taft β parameter, on cellulose dissolution in imidazolium-based ionic liquids (ILs). A series of ILs sharing the common cation 1-benzyl-3-methylimidazolium were synthesized with varying anions, including chloride, acetate, formate, methoxyacetate, and methylphosphonate. The hydrogen-bond accepting ability (β) of each IL was experimentally determined and correlated with cellulose dissolution performance. Dissolution capability was evaluated by solubilizing 5 wt% cotton cellulose at 90 °C and monitoring under polarized light microscopy. Among the studied systems, 1-benzyl-3-methylimidazolium acetate (β = 1.01) demonstrated the highest dissolution efficiency, highlighting the critical role of strong hydrogen-bond basicity in disrupting the cellulose hydrogen-bonding network. To support the experimental observations, COSMO-RS simulations were conducted to probe the molecular-level interactions between anions and cellulose. Parameters such as anion size, theoretical density, viscosity, and surface charge density distribution were analyzed to elucidate their contributions to dissolution behavior. The regenerated cellulose was further characterized using scanning electron microscopy (SEM) and Fourier transform infrared (FTIR) spectroscopy.