Research progress of different plant fiber reinforced PLA/PBAT/PBS composites
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摘要: 植物纤维是由碳水化合物、苯酚类物质以及萜烯类物质组成的丝状或絮状物，种类繁多，资源丰富，且具有比强度高、可降解和可再生等优良特性，是天然绿色生物质纤维原料。将植物纤维作为树脂基复合材料的增强材料，不仅可以实现植物纤维资源的高效高值化利用，提升复合材料的综合应用性能，而且还可以降低复合材料制备成本，近年来关于不同种类植物纤维增强可降解复合材料方面的研究备受关注。本文综述了不同种类植物纤维增强聚乳酸(PLA)、聚对苯二甲酸-己二酸丁二醇酯(PBAT)、聚丁二酸丁二醇酯(PBS)三种可降解高分子材料的研究进展，对各种复合材料的综合性能进行分析比较，并对其应用性能和前景进行了总结与展望。
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关键词:
- 植物纤维 /
- 生物降解树脂 /
- 复合材料 /
- 机械性能 /
- 聚乳酸、聚对苯二甲酸-己二酸丁二醇酯、聚丁二酸丁二醇酯
Abstract: Plant fibers, composed of carbohydrates, phenolic substances, and terpenes, take the form of fibrous or fluffy strands, exhibiting a wide range of varieties and abundant resources. These fibers possess the advantages of high specific strength, biodegradability, and renewability, making them a sustainable source of natural green biomass. Utilizing plant fibers as reinforcement materials in resin-based composites not only facilitates the efficient and valuable use of plant fiber resources, thus enhancing the comprehensive application performance of composites, but also contributes to cost reduction in composite manufacturing. In recent years, research into various types of plant fiber-reinforced biodegradable composites has attracted considerable attention. This paper reviews the latest advancements in plant fiber reinforcement in three biodegradable polymer matrices: polylactic acid (PLA), poly(butylene adipate-co-terephthalate) (PBAT), and poly(butylene succinate) (PBS). It provides an analysis and comparison of the overall performance of these different composites, offering insights into their application potential and forecasting future trends. -
图 1 (a) 木质素的组成部分[28]；(b)木质素的结构[28]；(c) 木质素纳米颗粒的合成及聚乳酸(PLA)开环聚合接枝[29]；(d)复合材料中PLA与纤维素纳米原纤维(LCNF)相互作用机制[30]；(e) 木质素含量对LCNF与PLA相容性的影响[30]
Figure 1. (a) building blocks of lignin[28];(b) structure of lignin[28];(c) Synthesis of Lignin Nanoparticles and Subsequent Grafting of Poly(lactic acid) (PLA) via Lactide Ring-OpeningPolymerization[29];(d) the interaction mechanism between PLA and Cellulose nanofibrils (LCNF) in composites[30];(e) the effect of lignin content on the compatibility of LCNF and PLA[30]
图 3 (a) 聚对苯二甲酸-己二酸丁二醇酯(PBAT)及PBAT/硅烷接枝麻纤维(Si-HF)复合材料拉伸强度[49]；(b) 马来酸酐接枝PBAT(m-PBAT)/麻粉(HP)复合材料拉伸强度和断裂伸长率[50]；(c) PBAT和PBAT/硅烷接枝木质素(VL)复合材料的拉伸强度、断裂伸长率和杨氏模量[56]
Figure 3. (a) Tensile strength of Poly (butyleneadipate-co-terephthalate)(PBAT) and PBAT/Silane grafted hemp fibers(Si-HF) composites[49]; (b) Tensile strength and elongation at break of m-PBAT/HP composites[50]; (c) Tensile strength, elongation at break and Young's modulus of PBAT and PBAT/Silane grafted lignin(VL) composites[56]
图 5 (a) 280 nm和(b) 660 nm处含有木质素、木质素纳米颗粒(LNPs)和PLA接枝的木质素纳米颗粒(PLA-LNPs)分别为1、5和10 wt %的纯PLA薄膜和PLA共混物的透光率[29]；(c)不同木质素含量PBAT薄膜快速老化后断裂伸长率与初始值之比随老化时间变化图[54]；(d)不同秸秆粉与碳酸钙混合(CCS)含量下PBAT薄膜紫外光谱图[60]；(e)聚丁二酸丁二醇酯(PBS)/木质素与PBS/马来酸酐接枝木质素(MAH-g-lignin)薄膜紫外光谱[74]；(f)不同增塑剂下PBS/MAH-g-lignin薄膜紫外光谱图[74]
Figure 5. (a) Light transmittance of pure PLA films and PLA blends containing lignin, lignin nanoparticles (LNPs) and PLA grafted (PLA-LNPs) at 280 nm and (b) 660 nm, respectively[29]; (c) The ratio of elongation at break to the initial value of PBAT films with different lignin content after rapid aging with aging time[54]; (d) Ultraviolet spectra of PBAT films with different Different straw flour is mixed with calcium carbonate(CCS) contents[60]; (e) Ultraviolet spectra of Poly(butylene succinate)PBS/lignin and PBS/ Maleic anhydride grafted with lignin(MAH-g-lignin) films[74]; (f) Ultraviolet spectra of PBS/MAH-g-lignin films under different plasticizers[74]
图 6 (a) NaOH、聚多巴胺(PDA)和硅烷偶联剂协同改性处理竹纤维示意图[36]；(b) 苎麻纤维表面PDA涂层示意图[67]；(c) 硅烷接枝PDA反应机制及PBS和改性竹纤维之间界面黏附机制[69].
Figure 6. (a) Schematic diagram of bamboo fiber co-modified with NaOH, Polydopamine(PDA) and silane coupling agent[36]; (b) Schematic diagram of PDA coating on the surface of ramie fibers[67]; (c) The reaction mechanism of silane grafting and the interfacial adhesion mechanism between PBS and modified bamboo fibers[69]
图 7 (a) 马来酸酐(MA)接枝到PBAT上反应机制[50]；(b) MAH-g-lignin的合成[74]；(c) PBS/MAH-g-lignin/柠檬酸三乙酯TEC增容机制[74]
Figure 7. (a) Reaction mechanism of Maleic anhydride(MA) grafting onto PBAT[50];(b) Synthesis of MAH-g-lignin[74]; (c) The postulated compatibilizing mechanism of PBS/MAH-g-lignin/Triethyl citrate(TEC)[74]
表 1 聚乳酸(PLA)、聚对苯二甲酸-己二酸丁二醇酯(PBAT)、聚丁二酸丁二醇酯(PBS)基本性能
Table 1. Basic performance of polylactic acid (PLA), poly(butylene adipate-co-terephthalate) (PBAT), and poly(butylene succinate) (PBS)
Type Density/
(kg·m−3)Tensile strength/
MPaElongation
at break/%Glass transition
temperature/℃Melting
temperature/℃When the crystallinity
is 100%, it melts/(J·g−1)Ref. PLA 1.2-1.3 9.57-50 20-240 40-70 130-180 93.6 [2] PBAT 1.18-1.3 7.9-25 500-800 −30 110-150 114 [3] PBS 1.25 28.5-37 170-250 −32 110-140 200 [4] 
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表 2 常见复合材料制备工艺及优缺点
Table 2. Advantages and disadvantages of common composite preparation processes
Preparation process Advantage Disadvantage Ref. Injection molding The manufacturing pace is rapid, boasting high efficiency, low costs, and consistent quality standards. It is prone to the formation of weld marks and radial lines. [9] Blow molding Blow molds are simple, inexpensive to make, and are used to produce small, small-scale products Susceptible to factors such as flow direction, stretching ratio,
mold temperature, etc.[10] Compression
moldingHigh molding pressure, low internal stress in the product, minimal shrinkage, and excellent strength Not suitable for complex products using compression molding; mechanical properties are significantly affected by process
parameters such as pressure and temperature.[11] Solution casting
methodGood uniformity, easy control of film thickness The process is relatively complex, prone to introducing impurities, and finding suitable solvents for certain polymers is challenging. [12] 3D printing Wide range of printing materials, diverse structures, reduced energy consumption The molding speed is relatively slow, not suitable for manufacturing large parts. [13]
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表 3 不同含量与种类麻纤维改性后增强PLA复合材料力学性能
Table 3. Enhanced mechanical properties of PLA composites after modification of hemp fibers with different contents and types
Fiber type Fiber
content/wt%Tensile
strength/MPaYoung's
modulus/GPaFlexural
strength/MPaFlexural
modulus/GPaElongation
at break/%Ref. Kenaf 5 54.6 2.86 75.2 6.56 2.45 [19] Flax 20 44 4.15 - - 3.8 [21] Jute 30 59.94 1.81 83.56 5.95 4.28 [22] Ramie 30 84 1.6 119 7.4 - [23] Hemp 45 63 6.5 124.2 9.3 - [24] Kenaf 50 190.92 16.3 235.42 19.01 - [20]
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表 4 不同比例改性竹纤维增强PLA材料力学性能
Table 4. Mechanical properties of modified bamboo fiber reinforced PLA materials with different proportions
Author Fiber
content/%Tensile
strength/MPaTensile
modulus/GPaFlexural
strength/MPaFlexural
modulus/GPaElongation
at break/%Ref. Wang 15 60 6.3 - - - [37] Fei 20 35.97 - - 3.88 3.17 [36] Fang 30 75.67 0.806 46.93 3.88 13.63 [38] Zhang 40 43.98 2.63 75.93 5.29 - [39] Zhang 40 38.36 2.01 92.52 7.34 - [40]
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表 5 添加无机填料对纤维增强复合材料的性能优势
Table 5. Performance advantages of adding inorganic fillers to fiber-reinforced composites
matrix Fiber
reinforcementsInorganic fillers Performance Benefits Ref. PLA Flax Borax, boric acid composition, zinc borate Slow down the rate of mechanical property loss after water absorption. [26] Lignin Silicon dioxide Increase the initial decomposition temperature of PLA/lignin composite materials and reduce the maximum temperature during sample combustion. [33] Rice straw Attapulgite The thermal stability of composite materials is enhanced by the rough stick soil thermal barrier effect. [42] Wheat straw Montmorillonite Significantly increase tensile strength and flexural strength. [43] Wheat straw Graphene nanosheets,
graphene oxideIncrease tensile strength and flexural strength while significantly reducing sample water absorption rate and thickness expansion rate. [46] PBAT Jute Ammonium polyphosphate, expandable graphite The APP/EG composite system exhibits excellent flame retardant properties. [52] Wheat straw Calcium carbonate It can effectively block most of the UVA and UVB spectra, while enhancing aging resistance and water vapor barrier properties. [60] PBS Bamboo
powderBamboo charcoal, silicon
nitride, zinc oxidePromote the formation of strong hydrogen bonds between PBS and bamboo powder, significantly enhancing mechanical properties and thermal stability. [71]
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Table 6. Advantages and disadvantages of different plant fibers for reinforcing composites
Fiber type Disadvantages Advantage Ref. Hemp fibers High moisture absorption, leading to significant expansion of the composite material.
FlammableHigh strength and modulus, which can significantly enhance the mechanical properties of composite materials.
Preparing sensors by adding different stimulating fluorescent factors.
Accelerate the degradation rate.[17][19][49][50]
[51]
[26]Lignin Prone to aggregation and uneven dispersion within the matrix. Excellent water vapor and oxygen barrier properties.
Outstanding ultraviolet shielding performance.
Effective inhibition against Gram-positive bacteria, Staphylococcus aureus, mold, and Aspergillus niger.
Excellent antioxidant activity.
Enhanced thermal stability of composite materials.
Outstanding mechanical performance.[30][53]
[29][54][74]
[31][73]
[72]
[32][33]
[56][57]Bamboo fiber The high lignin content makes it difficult to remove completely, and the extraction process of bamboo fibers is rather complex. Lightweight, high strength, and excellent impact resistance.
Accelerate the degradation rate
Strong adsorption capacity, removing harmful substances.[69]
[71]Straw fiber Compared to other types of fibers, it has lower strength and is prone to combustion. Accelerate degradation rate and significantly reduce production costs.
Excellent anti-aging properties, water vapor and UV barrier properties, suitable for use in ground films.[47]
[60]
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