Ionic Liquids (ILs) have been used to address issues such as recyclability, cost-effectiveness, and tailored thermophysical properties. This is most relevant to recent efforts directed at dissolving cellulose for filament spinning and bioproduct development. Herein, we introduce a simple method to investigate how interactions between cellulose films (roughness, Rh = 37 nm) and ILs specifically 1-butyl-3-methylimidazolium acetate ([bmim][OAc]), 1-butyl-3-methylimidazolium chloride ([bmim][Cl]), 1-ethyl-3-methylimidazolium acetate ([emim][OAc]), and 1-ethyl-3-methylimidazolium chloride ([emim][Cl]), along with their water mixtures (0, 5, and 10 wt%) affect thermophysical properties relevant to cellulose dissolution (surface tension, γ; contact angle, θ; diffusivities, D; and bulk density, ρ) at 363.15 K and 0.1 MPa under argon and air atmospheres. Thermophysical properties relevant to cellulose dissolution were measured at 363.15 K and 0.1 MPa under argon (surface tension, γ, contact angle, θ), and air (diffusivities, D and bulk density, ρ) atmospheres to reveal the effect of the IL counter ions on the involved interactions with water. In general, water increased γ, θ, but reduced D, which supports experimental observations indicating the detrimental effect of water on IL-cellulose interactions. The [emim]+ cation (in [emim][OAc] and [emim][Cl]), produced a lower contact angle with cellulose while the interfacial properties (γ, θ, D) for ILs with the [OAc]− anion were marginally affected by water. By contrast, the two ILs carrying [Cl]− anions exhibited a significant reduction in D (from 11.7·10-13\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\cdot {10}^{-13}$$\\end{document} to 2.9·10-13m2s-1\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\cdot {10}^{-13} {m}^{2}{s}^{-1}$$\\end{document}) in the cation shift from [emim]+ to [bmim]+ at 363.15 K and 0.1 MPa, with 0% water content. Overall, we present a methodical approach rooted in experimental and theoretical approaches to facilitate our understanding of ionic liquids (ILs), especially within the domain of bioprocessing.Graphical
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