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Nanoscale insights into cellulose-imidazolium ionic liquid interactions via atomic force microscopy.
Ruimei Cao1, Hongshuai Gao2, Wanxue Lv3
1School of Chemical Engineering, Zhengzhou University, Zhengzhou, 450001, China; Longzihu New Energy Laboratory, Zhengzhou Institute of Emerging Industrial Technology, Henan University, Zhengzhou, 450046, China.
Carbohydrate Polymers
|March 14, 2026
Summary
Understanding cellulose interaction forces is key. Atomic force microscopy revealed hydrogen bonds and van der Waals forces dominate cellulose cohesion and dissolution in ionic liquids, enabling regenerated fiber production.
Area of Science:
- Materials Science
- Nanotechnology
- Polymer Chemistry
Background:
- Cellulose interaction forces are crucial for material properties but challenging to quantify experimentally at the nanoscale.
- Understanding these forces is vital for developing advanced cellulose-based products and efficient dissolution processes.
Purpose of the Study:
- To quantitatively measure cellulose intermolecular forces using atomic force microscopy (AFM) in various environments (air, water, ionic liquids).
- To elucidate the role of hydrogen bonding, van der Waals forces, and ionic liquid properties in cellulose cohesion and dissolution.
- To propose a dual-site interaction mechanism and visualize fiber evolution for regenerated cellulose production.
Main Methods:
- Atomic Force Microscope (AFM) force spectroscopy to measure intermolecular forces.
- Nuclear Magnetic Resonance (NMR) spectroscopy and molecular dynamics (MD) simulations to investigate interaction mechanisms.
- In-situ AFM to visualize cellulose fiber swelling and single-chain stripping in ionic liquids.
Main Results:
- Intermolecular forces decreased significantly upon hydroxy group modification (60.3% for methyl, 34.0% for hydroxyethyl), highlighting hydrogen bond and van der Waals dominance.
- Ionic liquid cooperativity drastically reduced interaction forces by 84.5% (39.13 nN to 6.08 nN), emphasizing the role of hydrogen bond ability, hydrophobicity, and van der Waals forces in dissolution.
- A dual-site interaction mechanism was proposed, supported by NMR and MD simulations.
- In-situ AFM visualized fiber swelling and single-chain stripping, leading to successful preparation of regenerated cellulose fibers with good mechanical properties.
Conclusions:
- Hydrogen bonds and van der Waals forces are primary drivers of cellulose cohesion.
- Ionic liquid properties, including cation-anion cooperativity, significantly impact cellulose dissolution by reducing intermolecular forces.
- The study provides a nanoscale understanding of cellulose interactions, guiding the design of ionic liquids for efficient cellulose dissolution and the development of high-performance regenerated cellulose materials.
