Hydrogen bond producers in powerful protic ionic liquids for enhancing dissolution of natural cellulose

SusMat Pub Date : 2024-08-20 DOI:10.1002/sus2.238
Shi-Peng Chen, Dan-Yang Zhao, Jin-Long Zhu, Jing Wang, Gan-Ji Zhong, Hua-Dong Huang, Zhong-Ming Li
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Abstract

The manipulation of hydrogen bonding within protic ionic liquids is conducive to conquering the robust hydrogen bonding interactions in cellulose for its effective dissolution, but it is a great challenge to establish the delicate balance of hydrogen bonding network between solvent and cellulose. Herein, we proposed the concept of “hydrogen bond producers” for urea molecules in 1,1,3,3-tetramethylguanidinium methoxyacetate acid ([TMGH][MAA]) to enhance the dissolution of cellulose. The optimization of physicochemical properties for [TMGH][MAA] solvent as a function of urea concentration revealed a remarkable increase in cellulose solubility from 13% to 17% (w/w) by adding only 0.25 wt% urea, highlighting the efficiency of [TMGH][MAA] as a powerful solvent for the dissolution of cellulose. The experimental and simulation results verified that the significant improvement on dissolution of cellulose was attributed to the hydrogen bonding interaction of urea molecules with ion pairs and part of free ions, reducing the interference with the active ions bonded to cellulose. Furthermore, the considerable enhancement on comprehensive properties of regenerated cellulose films demonstrated the effectiveness of [TMGH][MAA]/urea solvent. The concept of “hydrogen bond producers” presented here opens a new avenue for significantly enhancing the dissolution of natural cellulose, promoting the sustainable development in large-scale processing of cellulose.

Abstract Image

用于提高天然纤维素溶解度的强力原生离子液体中的氢键生成器
操纵原生离子液体中的氢键有利于克服纤维素中强大的氢键相互作用,从而有效溶解纤维素,但要在溶剂和纤维素之间建立氢键网络的微妙平衡却是一项巨大挑战。在此,我们提出了 1,1,3,3- 四甲基胍甲氧基乙酸([TMGH][MAA])中尿素分子的 "氢键制造者 "概念,以提高纤维素的溶解度。通过优化[TMGH][MAA]溶剂的理化性质与尿素浓度的关系,发现只需添加 0.25 wt% 的尿素,纤维素的溶解度就能从 13% 显著提高到 17%(重量/重量),这凸显了[TMGH][MAA]作为纤维素溶解强力溶剂的高效性。实验和模拟结果证实,纤维素溶解度的显著提高是由于尿素分子与离子对和部分游离离子之间的氢键作用,减少了对纤维素上键合的活性离子的干扰。此外,[TMGH][MAA]/脲溶剂还显著提高了再生纤维素薄膜的综合性能,这也证明了[TMGH][MAA]/脲溶剂的有效性。本文提出的 "氢键生产者 "概念为显著提高天然纤维素的溶解度开辟了一条新途径,促进了纤维素大规模加工的可持续发展。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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