Molecular dynamics study on effects of the synergistic effect of anions and cations on the dissolution of cellulose in ionic liquids.

[Display omitted] • A delicate balance among anion-cation-cellulose interactions is essential. • Cation facilitates cellulose dissolution in AA ILs, differing from imidazole-based ionic liquids. • Typically provide the interaction mechanism of cellulose with the next-gen ILs featuring amino acid-derived cations. This work systematically explores the interaction between cellulose and various ionic liquids (ILs) formed by the pairing of glycine cations with diverse anions. Results show that the interaction of anions with cellulose decreases in the order of [CH 3 COO]− > [Im]− > [SCN]− > Cl− > [PF 6 ]−, differing from imidazole-based ionic liquids. The synergistic effect of anions and cations is crucial for cellulose dissolution. Moreover, the electronegativity of anions can enhance their interaction with cellulose. Short alkyl chains (n = 1, 3, 5) reduce hydrogen bonding due to steric hindrance, while longer chains (n = 9) promote diffusion and hydrogen bond formation. The introduction of electron-withdrawing groups to anions weakens their interaction with cellulose, while marginally strengthening the association between cations and cellulose. Overall, a delicate balance among anion-cation-cellulose interactions is essential for effective cellulose dissolution. The obtained results are anticipated to be of significant importance in the rational design of innovative amino acid-based ionic liquids, aiming to achieve efficient cellulose dissolution. [ABSTRACT FROM AUTHOR]