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Progress in Chemistry 2021, Vol. 33 Issue (8): 1293-1310 DOI: 10.7536/PC200759 Previous Articles   Next Articles

• Review •

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: Revised: Online: Published:
  • 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)
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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

Key words: cellulose, cellulose nanocrystal, preparation, composite materials
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]
Table 1 Examples of length(L) and diameter(d) of CNC from various sources obtained via different methods
Source L, nm d, nm Method ref
Bacterial cellulose 100~300 5~20 Acid hydrolysis 10
Corncob residue 421 ± 112 6.5 ± 2.0 Acid hydrolysis 11
Hemp flax triticale ca.150 3~6 Oxidation method 12
Wood flour <500 1~9 Mechanical method 13
MCC 70~80 15~20 Ionic liquid 14
Softwood 100~150 4~5 Acid hydrolysis 15
Cotton fiber 100~350 3~25 Deep eutectic solvent 16
Fig. 2 TEM images of cellulose nanocrystals derived from(a) tunicate,(b) bacteria,(c) ramie,(d) sisal[5]
Fig. 3 Surface chemistry in the preparation of cellulose nanocrystallines[3]
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
Fig. 4 Illustration of the extraction process of CCNC[49]
Fig. 5 Schematic flow diagram of experiments for integrated CNC and CNF production with recovery of organic acid[51]
Fig. 6 Regioselective oxidation of cellulose by TEMPO-mediated oxidation[57]
Fig. 7 Schematic representation of the preparation of CNC by APS swelling followed by oxidation[32]
Fig. 8 Schematic diagram of morphology-controlled CNC via compound enzymatic hydrolysis[66]
Fig. 9 Schematic diagram of the MCC ultrasonication process[34]
Fig. 10 Working principle of ball milling process[68]
Fig. 11 Schematic diagram showing reaction of single cellulose chain repeating unit with [BMIM]HSO4[14]
Fig. 12 One-pot preparation of hydrophobic CNCs in TBAA/DMAc with acetic hydride(upper), and the more typical route(lower)[75]
Fig. 13 Schematic illustration of in situ chemical polymerization in the synthesis of PPy/CNC nanostructures[105]
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