Fully Bio‐Based Ionic Liquids for Green Chemical Modification of Cellulose in the Activated‐State

Biopolymers, especially cellulose, are vital to transitioning to a circular economy and reducing our reliance on fossil fuels. However, for many applications a high degree of cellulose hydroxyl modification is necessary. The challenge is that the chemical features of the hydroxyls of cellulose and water are similar. Therefore, chemical modification of cellulose is often explored under non-aqueous conditions with systems that result in high hydroxyl accessibility and reduce cellulose aggregation. Unfortunately, these systems depend on hazardous and complex solvents from fossil resources, which diverge from the initial sustainability objectives. To address this, we developed three new betaine-based ionic liquids that are fully bio-based, scalable, and green. We found that a specific ionic liquid had the perfect chemical features for the chemical activation of cellulose without disturbing its crystalline ordering. The high activation in heterogeneous conditions was exemplified by reacting cellulose with succinic anhydride, resulting in more than 30 % conversion of all hydroxyls on cellulose. Overall, this work opens new perspectives for the derivatization of cellulosic materials while simultaneously "keeping it green".