胶原蛋白基纳米复合材料的性能及界面研究进展

刘晨阳; 马建中; 张跃宏

doi:10.13801/j.cnki.fhclxb.20210108.001

胶原蛋白基纳米复合材料的性能及界面研究进展

doi: 10.13801/j.cnki.fhclxb.20210108.001

刘晨阳^{1, 2, 3,},
马建中^{1, 2, 3, ,},
张跃宏^{1, 2, 3, ,}

1.
陕西科技大学　轻工科学与工程学院，西安 710021
2.
轻化工程国家级实验教学示范中心(陕西科技大学)，西安 710021
3.
西安市绿色化学品与功能材料重点实验室，西安 710021

基金项目: 国家自然科学基金 (21838007)

详细信息

通讯作者:
马建中，博士，教授，博士生导师，研究方向为高分子助剂的合成理论与作用机制、无机-有机杂化纳米材料及其与动植物纤维作用机制E-mail：majz@sust.edu.cn

张跃宏，博士，副教授，硕士生导师，研究方向为生物质高分子材料的绿色转化与高值化利用　 E-mail：yuehong.zhang@sust.edu.cn

中图分类号: TB332；TQ93
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出版历程
- 收稿日期: 2020-10-26
- 录用日期: 2020-12-31
- 网络出版日期: 2021-01-09
- 刊出日期: 2021-06-23

Progress on properties and interface of collagen-based nanocomposites

LIU Chenyang^{1, 2, 3
,},
MA Jianzhong^{1, 2, 3
, ,},
ZHANG Yuehong^{1, 2, 3
, ,}

1.
College of Bioresources Chemical and Materials Engineering, Shaanxi University of Science & Technology, Xi’an 710021, China
2.
National Demonstration Center for Experimental Light Chemistry Engineering Education, Shaanxi University of Science & Technology, Xi’an 710021, China
3.
Xi’an Key Laboratory of Green Chemicals and Functional Materials, Xi’an 710021, China

摘要

摘要: 胶原蛋白(COL)是一种绿色可再生的有机天然高分子材料，具有优异的生物相容性、可生物降解性和低抗原性等特点，将具有独特功能特性的无机纳米材料引入其中，可以开发出兼具二者优异性能的新型COL基纳米复合材料。然而，无机纳米材料与有机COL之间的界面结合特性会显著影响所制备复合材料的性能。因而，有必要研究纳米材料与COL之间的界面结合特性。本文系统回顾了未改性/有机化改性纳米材料对COL基纳米复合材料性能影响的研究现状，重点阐述了通过现代仪器分析表征方法和分子动力学模拟两种方法对纳米材料与COL之间的界面研究进展，对比了两种方法的优缺点，展望了COL基纳米复合材料性能及界面研究未来可能的发展趋势，指出在COL中引入新型纳米材料制备绿色化、多功能化、高性能化、应用多元化的COL基纳米复合材料及利用多种现代仪器分析方法和计算机模拟相结合的手段进行界面研究是未来的主要研究方向。
- 复合材料 /
- 胶原蛋白 /
- 纳米材料 /
- 界面 /
- 分子动力学
Abstract: Collagen (COL) is a green and renewable organic natural polymer material with excellent biocompatibility, biodegradability and low antigenicity. A series of novel collagen-based nanocomposites combining excellent properties of two components could be developed by introducing inorganic nanomaterials with unique functional characteristics into collagen matrix. However, the interface interaction characteristics between inorganic nanomaterials and organic COL have a significant effect on the properties of the corresponding nanocomposites. Therefore, it is necessary to investigate the interface interaction between nanomaterials and COL. This paper systematically reviewed the main research status of the effect of unmodified/modified nanomaterials on the properties of COL-based nanocomposite, and summarized the progress of the interface research between nanomaterials and COL through methods of modern instrumental analysis and molecular dynamics simulation. Moreover, the advantages and disadvantages of the two methods were compared. Finally, the possible future research trend of the interface interaction between nanomaterials and COL matrix was prospected. It is pointed out that the introduction of nanomaterials into the COL matrix to prepare environmentally friendly, multi-functional, high-performance, and widely used COL-based nanocomposites, and the combination of modern instrument analysis methods and computer simulation methods to conduct interface research will be the main research directions in the future.
- composites /
- collagen /
- nanomaterials /
- interfacial /
- molecular dynamics

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图 1 氧化石墨烯(GO)-胶原蛋白(COL)复合材料制备示意图^[21]

Figure 1. Schematic illustrating the preparation of graphene oxide (GO)-collagen (COL) composites^[21]

EDC—1-ethyl-(3-dimethylaminopropyl) carbodiimide hydrochloride

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图 2 Fe₃O₄/COL磁性纳米复合材料合成示意图^[31]

Figure 2. Schematic illustrating the preparation of Fe₃O₄ /COL nanocomposites ^[31]

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图 3 聚乙烯亚胺(PEI)-单壁碳纳米管(SWNT)作为交联剂制备胶原蛋白基水凝胶^[33]

Figure 3. Synthesis of crosslinking collagen hydrogels by utilizing polyethyleneimine (PEI)-single-walled carbon nanotube (SWNT) as a macro-crosslinking agent^[33]

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图 4 SiO₂(a) 和SiO₂/COL复合材料 (b) 的TEM图像^[38]

Figure 4. TEM images of SiO₂ (a) and SiO₂/COL composites (b)^[38]

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图 5 GO、草鱼皮胶原蛋白(GCSC)和GCSC-GO的拉曼谱图^[39]

Figure 5. Raman spectra of GO, grass carp skin collagen protein (GCSC) and GCSC-GO^[39]

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图 6 COL凝胶和负载反蛋白石(IO)@TiO₂的COL凝胶的高分辨率C1s XPS图谱^[40]

Figure 6. High resolution C1s XPS spectra of collagen gel and collagen gel containing inverse opal (IO)@TiO₂^[40]

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图 7 加入胶原后碳纳米管(CNT)在10 min内发生聚集 (a)， CNT聚集放大图(b)^[41]

Figure 7. Aggregation of carbon nanotube (CNT) occurred within 10 mins after addition of collagen (a), enlarged view of the CNT aggregation (b)^[41]

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图 8 表面形貌图及三维形貌图^[43]

Figure 8. Surface topographic image and 3D image through AFM^[43]((a1), (a2)) TiO₂; ((b1), (b2)) TiO₂-COL^EPF; ((c1), (c2)) TiO₂-COL^CL; ((d1), (d2)) Titanium nanotubes (TNT); ((e1), (e2)) TNT-COL^EPF; ((f1), (f2)) TNT-COL^CL)

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图 9 不同COL和SiO₂浓度的SiNR-COL复合水凝胶的储能模量(G′)；采用单因素方差分析和Dunnett法计算同一胶原浓度下水凝胶G′的方差，*P < 0.05；箭头表示同一胶原浓度下水凝胶G′最小时对应的SiO₂浓度^[44]

Figure 9. Storage modulus (G′) of SiNR-collagen composite hydrogels with various COL and SiO₂ concentrations; Variance of the G′ value between the hydrogels with same collagen concentration was determined by one-way analysis of variance with Dunnett post hoc test, *P < 0.05; Arrows indicate the SiNR concentration for minimal G′ value^[44]

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图 10 CNT-胶原样肽(CPs)的分子动力学模拟快照^[50]

Figure 10. Molecular dynamics simulation snapshot of CNT-glue the same peptide collagen peptides (CPs)^[50]

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图 11 嵌入石墨纳米带(GNR)的COL的模拟快照^[53]

Figure 11. Simulation snapshots of the COL fibers embedded with a graphene nanoribbon (GNR)^[53]

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图 12 COL表面上的Ca-P团簇随动力学时间进程的演化^[57]

Figure 12. Evolution of Ca-P clusters on COL surface with kinetic time course^[57]

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表 1 现代仪器分析方法在界面研究中的应用

Table 1. Application of modern instrument analysis in interface research

Characterization	Information
SEM, TEM	Microstructure of interfacial phase
FTIR, UV-vis, Raman spectra	Composition and chemical structure of interfacial phase
Turbidimetric method	Aggregation at the interface phase
XPS	Binding energy, element composition and chemical bond
XRD	Phase analysis of interfacial phase
DSC, TGA	Thermal properties of interfacial phase
Rheometer, DMA	Viscoelasticity (storage modulus and loss modulus) of interfacial phase
AFM	Nanoscale imaging and mechanical properties of interface morphology

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表 2 分子动力学模拟中的相关计算参数及应用

Table 2. Calculation parameters and their application in molecular dynamics simulation

Calculation parameter	Application
Radius of gyration, root mean square deviation	Conformational change of collagen
Radial distribution function, interaction energy	Type and size of interface interaction
Pull-out studies, adhesion energy, surface free energy	Bonding performance of interface

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