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化学进展 2021, Vol. 33 Issue (8): 1293-1310 DOI: 10.7536/PC200759 前一篇   后一篇

• 综述 •

纤维素纳米晶体的制备及其在复合材料中的应用

李金召1, 李政1,2,*(), 庄旭品1, 巩继贤1, 李秋瑾1, 张健飞1,3   

  1. 1 天津工业大学纺织科学与工程学院 先进纺织复合材料教育部重点实验室 天津 300387
    2 宁夏中宁枸杞产业创新研究院有限公司 中宁 755199
    3 山东省生态纺织协同创新中心 青岛 266071
  • 收稿日期:2020-07-28 修回日期:2020-09-30 出版日期:2021-08-20 发布日期:2020-12-28
  • 通讯作者: 李政
  • 基金资助:
    国家重点研发计划(2017YFB0309800); 国家重点研发计划(2016YFC0400503-02); 天津市重点研发计划科技支撑重点项目(20YFZCSN00130); 新疆自治区重大专项(2016A03006-3); 天津自然科学基金项目(18JCYBJC89600); 中国纺织工业联合会科技指导性项目(2017011); 宁夏中宁枸杞产业创新研究院一般项目(ZNGQCX-B-2019006)

Preparation of Cellulose Nanocrystallines and Their Applications in CompositeMaterials

Jinzhao Li1, Zheng Li1,2(), Xupin Zhuang1, Jixian Gong1, Qiujin Li1, Jianfei Zhang1,3   

  1. 1 Key Laboratory of Advanced Textile Composites of Ministry of Education, School of Textiles Science and Engineering, Tiangong University,Tianjin 300387, China
    2 Innovation Research Institute of Wolfberry Industry Co. LTD,Zhongning 755199, China
    3 Collaborative Innovation Center for Eco-Textiles of Shandong Province,Qingdao 266071, China
  • Received:2020-07-28 Revised:2020-09-30 Online:2021-08-20 Published:2020-12-28
  • Contact: Zheng Li
  • Supported by:
    National Key Research and Development Project Foundation of China(2017YFB0309800); National Key Research and Development Project Foundation of China(2016YFC0400503-02); Tianjin Key Research and Development Project(20YFZCSN00130); Xinjiang Autonomous Region Major Significant Project Foundation(2016A03006-3); Tianjin Natural Science Foundation(18JCYBJC89600); Science and Technology Guidance Project of China National Textile and Apparel Council(2017011); Innovation Research Institute of Wolfberry Industry Co. LTD(ZNGQCX-B-2019006)

纤维素纳米晶体是纤维素原料经加工而得到的纳米级棒状或球状晶体。由于其具有高强度、大比表面积、生物相容性、可再生性和可降解性等优良性能,可应用于复合材料、生物医药和环境等多个领域。本文详细综述了近年来制备纤维素纳米晶体的常用方法,包括酸水解法、氧化法、酶水解法、机械法、溶剂法以及组合法。同时,讨论了各种制备方法的优缺点。在应用研究方面,本文总结了其在增强复合材料、膜过滤复合材料、导电复合材料和无机纳米复合材料等热门领域的研究情况。最后,对纤维素纳米晶体的未来发展方向进行了展望。

Cellulose nanocrystal(CNC) is a nano-scaled rod-like or spherical crystal isolated from cellulosic materials. CNC has shown many advantages of, for example, high strength, high specific surface area, biocompatibility, renewability and degradability. Therefore, it can be applied to the composite materials, biomedicine and environment fields. The preparation methods of CNC are detailedly summarized in this review such as acid hydrolysis, oxidation method, enzymatic hydrolysis, mechanical method, solvent methods and combined processes. Meanwhile, the advantages and shortcomings of the preparation methods are discussed. In the field of applied research, this review summarizes the research status of CNC in some popular fields such as reinforced composite materials, membrane filtration composite materials, conductive composite materials and inorganic nanocomposites. Finally, the future prospective of CNC is presented.

Contents

1 Introduction

2 Physicochemical characteristics of CNC

2.1 Size distribution and morphology

2.2 Thermal performance

2.3 Rheological properties

3 Methods to prepare CNC

3.1 Acid hydrolysis

3.2 Oxidation methods

3.3 Enzymatic hydrolysis

3.4 Mechanical methods

3.5 Solvent methods

3.6 Combined processes

4 Application of CNC in the field of composite materials

4.1 Reinforced composite materials

4.2 Membrane filtration composite materials

4.3 Conductive composite materials

4.4 Inorganic nanocomposites

5 Conclusion and outlook

()
图1 (a)理想的纤维素微原纤的示意图,显示了结晶和非晶区,(b)酸水解纤维素无序区后的纤维素纳米晶体[3]
Fig. 1 (a) Schematics of idealized cellulose microfibril showing one of the suggested configurations of the crystalline and amorphous regions, and(b) cellulose nanocrystals after acid hydrolysis dissolved the disordered regions[3]
表1 不同长度和宽度的CNC
Table 1 Examples of length(L) and diameter(d) of CNC from various sources obtained via different methods
图2 不同原料制备的纳米纤维素晶体透射电镜图:(a)被囊动物,(b)细菌,(c)苎麻,(d)剑麻[5]
Fig. 2 TEM images of cellulose nanocrystals derived from(a) tunicate,(b) bacteria,(c) ramie,(d) sisal[5]
图3 纤维素纳米晶制备过程中的表面化学[3]
Fig. 3 Surface chemistry in the preparation of cellulose nanocrystallines[3]
表2 不同原料来源通过不同制备方法获得的CNC的长度、直径和收率
Table 2 Length, diameter and yield of different preparation methods for producing CNC
Main method Raw source Length(nm) Diameter(nm) Yield(%) ref
mineral acid hydrolysis bleached hardwood pulp 600~800 15~40 60.0% 24
mineral acid hydrolysis spent mushroom substrate 10~30 42.8% 25
mineral acid hydrolysis bacterial cellulose 100~300 5~20 >80.0% 10
mineral acid hydrolysis surgical cotton 297.7 ± 98.9 18.4±7.2 56.0% 26
organic acid hydrolysis corncob residue 421 ± 112 6.5 ± 2.0 66.3% 11
organic acid hydrolysis bleached birch kraft pulp 200~1200 8~15 85.0% 27
organic acid hydrolysis unbleached hardwood kraft pulp ca. 230 25 <6.0% 28
organic acid hydrolysis bleached eucalyptus kraft pulp 150~400 5~20 >70.0% 29
oxidation method jute fibers 100~200 3~10 >80.0% 30
oxidation method oil palm empty fruit bunch 122 6 93.0% 31
oxidation method hemp flax triticale ca.150 3~6 28.0%~36.0% 12
oxidation method cotton linters 136 ± 90 10 ± 5 95.8% 32
enzymatic hydrolysis MCC 120 ± 36.25 40.74 ± 7.59 22.0% 33
mechanical method MCC 50~250 10~20 ≤10.0% 34
mechanical method wood flour <500 1~9 22.4% 13
mechanical method microcrystalline cellulose 280 11 72.2% 35
mechanical method cotton cellulose powder 60~320 4~14 80.0% 36
ionic liquid MCC 146.8 ± 62 3.6 ± 1.8 48.0% 37
ionic liquid cotton fiber 150~350 ca. 20 38
ionic liquid MCC 70~80 15~20 14
deep eutectic solvent cotton fiber 100~350 3~25 74.2% 16
deep eutectic solvent bleached eucalyptus kraft pulp 50~300 5~20 73.0% 39
deep eutectic solvent cotton fiber 500~800 50~100 40
combined process bamboo pulp 200~300 25~50 88.4% 41
图4 CCNC提取过程示意图[49]
Fig. 4 Illustration of the extraction process of CCNC[49]
图5 有机酸水解法综合制备 CNC 和 CNF 以及有机酸回收的实验流程图[51]
Fig. 5 Schematic flow diagram of experiments for integrated CNC and CNF production with recovery of organic acid[51]
图6 TEMPO介导对纤维素进行区域选择性氧化[57]
Fig. 6 Regioselective oxidation of cellulose by TEMPO-mediated oxidation[57]
图7 APS溶胀然后氧化制备CNC示意图[32]
Fig. 7 Schematic representation of the preparation of CNC by APS swelling followed by oxidation[32]
图8 通过复合酶水解进行形态控制的CNC的示意图[66]
Fig. 8 Schematic diagram of morphology-controlled CNC via compound enzymatic hydrolysis[66]
图9 超声处理MCC过程示意图[34]
Fig. 9 Schematic diagram of the MCC ultrasonication process[34]
图10 球磨过程的工作原理[68]
Fig. 10 Working principle of ball milling process[68]
图11 单链纤维素重复单元与[BMIM]HSO4反应示意图[14]
Fig. 11 Schematic diagram showing reaction of single cellulose chain repeating unit with [BMIM]HSO4[14]
图12 TBAA/DMAc和乙酸酐一锅法制备疏水性CNC(上)和传统制备方法(下)[75]
Fig. 12 One-pot preparation of hydrophobic CNCs in TBAA/DMAc with acetic hydride(upper), and the more typical route(lower)[75]
图13 原位化学聚合制备PPy/CNC示意图[105]
Fig. 13 Schematic illustration of in situ chemical polymerization in the synthesis of PPy/CNC nanostructures[105]
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