Tailoring Hydronium ion Driven Dissociation-Chemical Cross-Linking for Superfast One-Pot Cellulose Dissolution and Derivatization to Build Robust Cellulose Films

• Published in: ACS nano 2024-03, Vol.18 (12), p.8754-8767
• Main Authors: Chen, Yi, Huang, Chengling, Miao, Zhouyu, Gao, Youjie, Dong, Yanjuan, Tam, Kam Chiu, Yu, Hou-Yong
• Format: Article
• Language: English
• ISSN: 1936-0851; 1936-086X
• DOI: 10.1021/acsnano.3c11335

Concepts of sustainability must be developed to overcome the increasing environmental hazards caused by fossil resources. Cellulose derivatives with excellent properties are promising biobased alternatives for petroleum-derived materials. However, a one-pot route to achieve cellulose dissolution and derivatization is very challenging, requiring harsh conditions, high energy consumption, and complex solubilizing. Herein, we design a one-pot tailoring hydronium ion driven dissociation-chemical cross-linking strategy to achieve superfast cellulose dissolution and derivatization for orderly robust cellulose films. In this strategy, there is a powerful driving force from organic acid with a pK a below 3.75 to dissociate H+ and trigger the dissolution and derivatization of cellulose under the addition of H2SO4. Nevertheless, the driving force can only trigger a partial swelling of cellulose but without dissolution when the pK a of organic acid is above 4.26 for the dissociation of H+ is inhibited by the addition of inorganic acid. The cellulose film has high transmittance (up to ∼90%), excellent tensile strength (∼122 MPa), and is superior to commercial PE film. Moreover, the tensile strength is increased by 400% compared to cellulose film prepared by the ZnCl2 solvent. This work provides an efficient solvent, which is of great significance for emerging cellulose materials from renewable materials.