TEMPO氧化修饰的天然多糖纳米纤维增强复合材料及其功能化研究进展

陈黄敬一; 俞娟; 蒋杰; 刘亮; 范一民

doi:10.13801/j.cnki.fhclxb.20211223.002

TEMPO氧化修饰的天然多糖纳米纤维增强复合材料及其功能化研究进展

doi: 10.13801/j.cnki.fhclxb.20211223.002

南京林业大学　化学工程学院，南京 210037

基金项目: 国家自然科学基金 (31901275)；江苏省自然科学基金(BK20190761)

详细信息

通讯作者:
范一民，博士，教授，博士生导师，研究方向为生物质纳米材料　E-mail: fanyimin@njfu.edu.cn

中图分类号: O636.1；TQ352
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出版历程
- 收稿日期: 2021-10-26
- 修回日期: 2021-12-09
- 录用日期: 2021-12-19
- 网络出版日期: 2021-12-27
- 刊出日期: 2022-04-01

Research progress of TEMPO oxidation modified natural polysaccharide nanofiber reinforced composites and their functionality

College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, China

摘要

摘要: 纤维素和几丁质具有相似的结构，是自然界中储量丰富的两类天然多糖。经2, 2, 6, 6-四甲基哌啶氮氧化物(TEMPO)氧化修饰制备的纤维素和几丁质纳米纤维，不仅具有多糖类物质的良好亲水性、生物可降解性、生物相容性及丰富的官能团(羟基、羧基、乙酰氨基和氨基等)所带来的特定化学性质，而且还具有纳米纤维的纳米尺寸效应、大比表面积、高表面活性、高结晶度和手性液晶相结构等特点，已成为生物质纳米材料领域的研究重点之一。本文对TEMPO氧化修饰制备天然多糖纳米纤维的方法及剥离机制进行了总结，同时重点综述了TEMPO氧化修饰的天然多糖纳米纤维在薄膜、凝胶、导电、医用、电磁屏蔽及环境等复合材料的增强和功能升级等方面的研究进展，强调了纤维素和几丁质纳米纤维的官能团及纳米尺寸在复合材料中的增效机制。最后，对天然多糖纳米纤维的发展方向及其在各领域应用的机遇与挑战进行了展望。
- 多糖纳米纤维 /
- 纤维素 /
- 几丁质 /
- TEMPO氧化 /
- 复合材料
Abstract: Cellulose and chitin are polysaccharides that abundantly exist in nature and have similar structures. Cellulose and chitin nanofibers prepared by using 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO) oxidization, not only have good hydrophilicity, biodegradability, biocompatibility and the active chemical properties brought by various functional groups (hydroxyl, carboxyl, acetyl, amino, etc.), but also have the characteristics of large specific surface area, chiral liquid crystal phase, high crystallinity, high transparency and specific nano effect caused by nano size. These natural polysaccharide nanofibers have become one of the research focuses in the field of biomass nanomaterials. In this review, the TEMPO oxidation methods used for the preparation of natural polysaccharide nanofibers, as well as the nanofiber extraction mechanism, were comprehensive summarized. At the same time, the up to now research progress on the as-prepared polysaccharide nanofibers-based composites, such as film, gel, conductive, medical, electromagnetic shielding and environmental materials, with focusing on its mechanical enhancement and function upgradation performance were reviewed. Specific focus is giving to the contributions of the functional groups and nano size of cellulose and chitin nanofibers on the performance improvements of the composites. Finally, the development direction of natural polysaccharide nanofibers and the opportunities and challenges of their applications in various fields are prospected.
- polysaccharide nanofiber /
- cellulose /
- chitin /
- TEMPO-oxidation /
- composite

HTML全文

图 1 纤维素 (a)和几丁质 (b)的化学结构

Figure 1. Chemical structures of cellulose (a) and chitin (b)

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图 2 几种典型的天然多糖纳米纤维的TEM图像：机械法制备的纤维素纳米纤维(CNF)和几丁质纳米纤维(ChNF) ((a)、(b))、酸水解法制备的CNC和ChNC ((c)、(d)) 和低共熔溶剂(DES)处理法制备的CNF和ChNF ((e)、(f))^[27]

Figure 2. TEM images of the represent natural polysaccharide nanofibers: Cellulose nanofiber (CNF) and chitin nanofiber (ChNF) prepared by using mechanical treatment ((a), (b)), CNC and ChNC prepared by using acid hydrolysis ((c), (d)), as well as CNF and ChNF prepared by using eutectic solvent (DES) treatment ((e), (f))^[27]

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图 3 2, 2, 6, 6-四甲基哌啶氮氧化物(TEMPO)氧化修饰的天然多糖纳米纤维增强复合材料及其功能化

Figure 3. Research progress of TEMPO oxidation modified natural polysaccharide nanofiber reinforced composites and their functionality

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图 4 纤维素 (a) 和几丁质 (b) TEMPO氧化中的羧基化过程

Figure 4. Carboxylation of cellulose (a) and chitin (b) in TEMPO-mediated oxidation

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图 5 碱性TEMPO-NaBr-NaClO化学氧化体系氧化纤维素 (a) 和几丁质 (b) 反应机制示意图

Figure 5. Schematic diagram of reaction mechanism of cellulose (a) and chitin (b) oxidation by alkaline TEMPO-NaBr-NaClO chemical oxidation system

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图 6 碱性TEMPO-NaBr-NaClO化学氧化体系制备的天然多糖纳米纤维 CNF (a)、ChNC (b)和ChNF (c) 的TEM图像^[4,16,44]

Figure 6. TEM images of CNF (a), ChNC (b) and ChNF (c) prepared by TEMPO-NaBr-NaClO oxidation at alkali condition^[4,16,44]

DP—Degree of polymerization

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图 8 中性TEMPO-NaClO-NaClO₂化学氧化体系氧化纤维素 (a) 和几丁质 (b)反应机制示意图

Figure 8. Schematic diagram of reaction mechanism for oxidation of cellulose (a) and chitin (b) by neutral TEMPO-NaClO-NaClO₂chemical oxidation system

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图 7 中性TEMPO-NaClO-NaClO2化学氧化体系制备的天然多糖纳米纤维 CNF (a) 和ChNF (b) 的TEM图像^[51-52]

Figure 7. TEM images of CNF (a) and ChNF (b) prepared by TEMPO-NaClO-NaClO₂ oxidation system at netural condition^[51-52]

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图 9 TEMPO/漆酶/O₂酶氧化体系制备的天然多糖纳米纤维CNF ((a)、(b)) 和ChNF (c) 的AFM图像^[53-54]

Figure 9. AFM image of CNF ((a), (b)) and ChNF (c) prepared by TEMPO/laccase/O₂ oxidation^[53-54]

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图 10 TEMPO-laccase-O₂酶氧化体系氧化纤维素原理示意图^[53]

Figure 10. Schematic diagram of mechanism of cellulose oxidation by TEMPO-laccase-O₂^[53]

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图 11 TEMPO电化学氧化体系氧化纤维素原理示意图^[70]

Figure 11. Schematic diagram of mechanism of cellulose oxidation by TEMPO electro-mediated oxidation^[70]

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图 12 TEMPO电化学氧化体系制备天然多糖纳米纤维CNF的TEM图像^[61]

Figure 12. TEM image of CNF prepared by TEMPO electro-mediated oxidation^[61]

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图 13 通过纤维素和几丁质纳米纤维的逐层沉积制成的多功能涂层膜^[79]

Figure 13. Multifunctional coating films by layer-by-layer deposition of cellulose and chitin nanofibrils^[79]

PET—Polyethylene terephthalate

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图 14 界面电荷络合进行连续超细纤维拉伸^[87]

Figure 14. Continuous microfiber drawing by interfacial charge complexation ^[87]

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图 15 几丁质纳米晶须复合制备高强度纸张^[96]

Figure 15. High-strength paper enhanced by chitin nanowhiskers^[96]

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图 16 还原氧化石墨烯(RGO)/CNF复合薄膜制作示意图^[125]

Figure 16. Schematic of the fabrication of the reduced graphene oxide (RGO)/CNF composite films^[125]

GO—Graphene oxide; HI—Hydroiodic acid

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图 17 纤维素纤维/CNF(CCNM)制备纤维素基复合巨凝胶^[146]

Figure 17. Cellulose-based composite macrogels from cellulose fiber/CNF(CCNM)^[146]

CFM—Cellulose fiber macrogels

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图 18 交联TiO₂-ChNF-聚丙烯酰胺(PAM)水凝胶制备示意图^[155]

Figure 18. Schematic representation of the fabrication of crosslinked TiO₂-ChNF-polyacrylamide (PAM) hydrogels^[155]

MBAA—Methylene bisacrylamide; AM—Acrylamide

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表 1 天然多糖纳米纤维类型^[13–17]

Table 1. Classification of natural polysaccharide nanofiber^[13–17]

Source	Product		Size (width×length)/nm
Woods, herbs, tunicates and algae	Cellulose nanofiber/nanofibril	(CNF)	2×500-20×2000
Woods, herbs, tunicates and algae	Cellulose nanocrystal/cellulose nanowisker	(CNC/CNW)	3×130-10×200

Shrimps and crabs, fungi, yeast cell walls and insect cuticle	Chitin nanofiber/nanofibril	(ChNF)	20×200-50×400
	Chitin nanocrystal/chitin nanowisker	(ChNC/ChNW)	16×160-18×240

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