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在有机酸介质中高度纤维素溶解的分子起源:一项综合实验和计算研究

Kanta Hayashi¹, Tomoya Tashiro¹, Tomohiro Hashizume²

¹Graduate School of Sciences and Technology for Innovation, Yamaguchi University, 2-16-1 Tokiwadai, Ube, Yamaguchi 755-8611, Japan. k-fujii@yamaguchi-u.ac.jp.

Physical chemistry chemical physics : PCCP

|December 22, 2025

概括

酸 (FA) 和酸 (PA) 通过化学修改其结构来溶解高分子量纤维素 (CL). 这些酸破坏了纤维素的键,并通过溶解稳定了链,从而实现了前所未有的可溶性.

科学领域:

聚合物化学聚合物化学
材料科学材料科学材料科学
物理化学物理化学

背景情况:

高分子量纤维素 (CL) 由于其广泛的分子间结网络,在常见溶剂中具有较差的溶解性.
了解纤维素溶解机制对于开发先进材料和可持续工艺至关重要.
像简单有机酸这样的非传统溶剂为纤维素加工提供了潜力.

研究的目的:

阐明纤维素在酸 (FA) 和酸 (PA) 中溶解的分子机制.
研究这些有机酸作为反应性和稳定性溶剂的双重作用.
为这些介质中的纤维素溶解性提供物理化学视角.

主要方法:

组合实验技术:红外 (IR) 光谱和高能X射线总散射 (HEXTS).
计算方法:密度函数理论 (DFT) 计算和全原子分子动力学 (MD) 模拟.
分析化学变化和溶解物-溶剂相互作用.

主要成果:

红外光谱学和DFT计算证实了纤维素基基的协同修饰由FA和PA,形成甲基和衍生物.
这些修改破坏了原生纤维素结网络,并改变了与溶剂的相互作用.
在HEXTS和MD模拟中,通过与未反应的溶剂分子的结,对修改的纤维素链进行了热力学稳定.

结论:

酸和酸作为双重功能溶剂,通过化学修饰诱导溶解,然后通过溶解稳定.
这项研究提供了分子层面的见解,了解纤维素在这些有机酸中的可溶性.
这些发现为在反应性溶剂系统中纤维素溶解提供了新的物理化学理解.

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