Research progress on cationic modification of plant fibers based on DES solvent systems

doi:10.11949/0438-1157.20250535

Abstract

Abstract:

Deep eutectic solvents (DES), as a new, green, and efficient solvent system, have demonstrated significant advantages in the cationic modification of plant fibers. This paper systematically reviews recent research progress on DES in the cationic modification of plant fibers, with a focus on the chemical processes, modification mechanisms, and application performance of binary and ternary TDES solvents. First, the effects of different pretreatment methods (physical, chemical, and enzymatic) on improving fiber accessibility and reactivity are analyzed. Subsequently, the mechanisms of binary DES solvent systems—such as carboxylic acid-based, urea-based, and glycerol-based systems—in fiber cationization are elaborated in detail. Additionally, research findings on ternary DES (TDES) solvents, which further enhance modification efficiency through multicomponent synergistic effects, are summarized. Studies have shown that DES solvent efficiently introduces quaternary ammonium groups into cellulose molecules by breaking the hydrogen bond network of cellulose, improving the dispersion of fibers and increasing the yield of nanofibers. The modified cationized fibers have broad applications in pulping and papermaking, nanomaterials, wastewater treatment, and biomedicine. Furthermore, this paper discusses current technical challenges in DES systems, including component interaction mechanisms, solvent recovery, and industrial-scale applications, while proposing future research directions. The findings provide a theoretical foundation and technical reference for the high-value utilization of plant fibers.

Key words: DES, TDES, cationic modification, biomass, nanomaterials, chemical reaction

摘要：

低共熔溶剂（DES）作为一种绿色、高效的新型溶剂体系，在植物纤维阳离子化改性领域中展现出显著优势。本文系统综述了DES体系在植物纤维阳离子化改性中的研究进展，重点探讨了二元和三元TDES溶剂的化学工艺、改性机理及其应用性能。首先，分析了不同预处理方法（物理、化学及生物酶法）对提升纤维可及性和反应活性的作用；其次，详细阐述了羧基酸类、尿素类及甘油类二元DES溶剂体系在纤维阳离子化中的作用机制，并总结了三元TDES溶剂通过多元组分协同效应进一步优化改性效果的研究成果。研究表明，DES溶剂通过破坏纤维素的氢键网络，高效将季铵基团引入纤维素分子，提高了纤维分散性和纳米纤维产率。改性后的阳离子化纤维在制浆造纸、纳米材料、污水处理及生物医药等领域具有广泛应用。本文进一步探讨了当前DES体系在组分相互作用机制、溶剂回收及工业化应用中的技术瓶颈，并对未来研究方向提出了展望，可为植物纤维的高值化利用提供理论依据和技术参考。

关键词: DES, TDES, 阳离子改性, 生物质, 纳米材料, 化学反应

CLC Number:

TS 72

Luxuan GUO, Lingzhi HUANG, Wenchao JIA, Lu WU, Hongwei ZHU, Meihong NIU, Haiqiang SHI. Research progress on cationic modification of plant fibers based on DES solvent systems[J]. CIESC Journal, 2025, 76(10): 4988-5002.

郭璐轩, 黄灵芝, 贾文超, 吴鲁, 朱宏伟, 牛梅红, 石海强. 基于DES溶剂体系的植物纤维阳离子改性研究进展[J]. 化工学报, 2025, 76(10): 4988-5002.

Figures/Tables 10

Fig.1 Schematic diagram of cationization preparation and application of plant fibers[3,5-7]

Fig.2 Plant fiber pretreatment method: (a) Pretreatment effect of plant fiber[5]; (b) PFI refining pretreatment [32]; (c) Pretreatment of acids and bases[33]; (d) Biological enzyme pretreatment[34]; (e) New pretreatment technology assists DES technology[14]; (f) Advantages and disadvantages of pretreatment technology

Fig.3 (a) Reaction mechanism of cationic cellulose with LA/ChCl DES; (b) Production of CNF by CA/ChCl DES combined microwave processing technology[51]; (c) Experimental process and SEM image of cellulose pretreatment with RCOOH/ChCl DES[52]

Fig.4 (a) Glu/TA DES cationized cellulose process and mechanism[56]; (b) Mechanism of action of ChCl/Urea DES cationized cellulose [60]; (c) Mechanism of action of TMAH·5H2O/Urea DES cationized cellulose[49]

Fig.5 (a) Mechanism of TDES-modified cellulose introduced by P/N/S[61];(b) Mechanism of Bh/Gl DES cationization of cellulose[27]; (c) AhG/Gl DES interatomic distance reaction theory[62,64]; (d) C-CNC flocculation diagram at different times[64]

Fig.6 (a) Reaction mechanism of p-TSA/ChCl DES to sorbitol[67]; (b) NaIO4 two-step cationized cellulose[68]; (c) Mechanism of cationization of cellulose by Bh/p-TSA/TEMA DES[23]; (d) Reaction mechanism diagram of bamboo fiber treated with FeCl3/Gly/GH DES[69]; (e),(f) lignin removal rate, xylan yield and enzymatic digestibility of bamboo fiber samples[69]

Table 1 Summary of the reaction mechanism of binary DES cationic fibers

分类	羧基酸-季铵盐 DES	尿素-季铵盐 DES	甘油-季铵盐 DES
反应性	中等反应性，羧基与季铵盐的静电作用较强	较高反应性，尿素易与纤维羟基形成氢键	较低反应性，甘油需催化剂促进反应
反应机理	羧基与季铵盐的离子键结合，可能伴随酯化反应	尿素与纤维羟基缩合形成氨基甲酸酯或氢键网络	甘油羟基与纤维羟基醚化或形成交联结构
特点	耐水性较好,柔软性中等,稳定性高	吸湿性强,易生物降解成本低	亲水性佳,环保性好,反应条件温和
经济性	原料成本中等，需控制pH和温度	原料廉价，工艺简单，适合大规模生产	甘油来源广泛，但可能需要额外催化剂增加成本

Fig.7 (a) TDES experimental flow chart[70]; (b) Reaction mechanism of TDES modified bamboo fiber[70]; (c)—(f) SEM images of fiber sample[70]

Table 2 Summary of DES treatment of plant fibers

序号	原料	DES			辅助工艺	成品	产率/%	应用	文献
序号	原料	HBD	HBA	比例	辅助工艺	成品	产率/%	应用	文献
1	漂白针叶木牛皮纸浆	CA	ChCl	1∶1	高压均质	CNF	84.19	纳米纸( CNP )	[51]
2	小麦秸秆	AA	ChCl	1,2,3∶1	NaIO₄	LCNC	—	水凝胶	[57]
3	橙皮	TA	Glu	2∶1	机械、超声	CNF	95.8	抗菌	[56]
4	玉米秸秆	GA、EG	TMBAC	1∶1∶2	热解炉	固体残渣	66.9~71.9	生物油	[9]
5	木薯渣	CA、LA	ChCl	1∶10∶1	球磨	木质纤维素	82.52	回收利用	[37]
6	纤维素整体柱	Urea	ChCl	2∶1	热致相分离法	阳离子化纤维	—	阴离子吸附	[59]
7	竹纤维	CAA、Urea	ChCl	1∶2∶1	研磨	CMCNF	70~85	CMCNF	[70]
8	漂白硫酸盐桦木浆	Gly	Bh	2∶1	微射流仪	CNF	72.5	纤维素薄膜	[27]
9	相思阔叶木浆	Gly	AGH、ChCl	4∶1∶1	NaIO₄	CCNF	—	CCNF	[68]
10	毛竹	Gly	AGH、FeCl₃	2∶1∶1	微波加热耦合	残余纤维素	81.17	组分分离	[69]

Fig.8 Summary and application of cationic fibers under DES solvent system[6-7,67,81]

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