Cellulose fiber‐reinforced polylactic acid

Polymer composites from polylactic acid (PLA) and two types of cellulose fibers obtained either by acid hydrolysis of microcrystalline cellulose (HMCC) or by mechanical disintegration of regenerated wood fibers (MF) were prepared and characterized. To enhance the compatibility of the cellulose fibers with PLA matrix, a surface treatment based on 3‐aminopropyltriethoxysilane (APS) was performed. The Fourier Transform Infrared (FTIR) spectroscopy was used to determine the chemical groups involved in the surface modification reaction. The silanization treatment resulted in different modifications on both types of cellulose fibers because of their different structural and morphological characteristics. The composites were prepared by incorporating 2.5% of the treated or untreated HMCC and MF into a PLA matrix using a melt‐compounding technique. An improved adhesion between the two phases of the composite materials was observed by scanning electron microscopy thanks to treatment. The dynamic mechanical thermal analyses showed that both untreated and silane treated fibers led to an improvement of the storage modulus of PLA in the glassy state. A higher enhancement of the storage modulus in the case of PLA/HMCC composites than the composites containing MF was obtained as a result of the high aspect ratio of these fibers which allows better matrix‐to‐filler stress transfer. Furthermore, the storage modulus of PLA composites was enhanced by silanization even at higher temperatures especially after thermal treatment. The cellulose fibers addition in PLA matrix modified significantly the relaxation phenomenon as observed in tan δ curves, emphasizing strongly modified molecular mobility of PLA macromolecules and crystallization changes. POLYM. COMPOS., 2011. © 2011 Society of Plastics Engineers.     

Moisture uptake and hygroexpansion of wood fiber composite materials with polylactide and polypropylene matrix materials

Effects of butantetracarboxylic acid (BTCA) modification, choice of matrix, and fiber volume fraction on hygroexpansion of wood fiber composites have been investigated. Untreated reference wood fibers and BTCA‐modified fibers were used as reinforcement in composites with matrices composed of polylactic acid (PLA), polypropylene (PP), or a mixture thereof. The crosslinking BTCA modification reduced the out‐of‐plane hygroexpansion of PLA and PLA/PP composites, under water‐immersed and humid conditions, whereas the swelling increased when PP was used as matrix material. This is explained by difficulties for the BTCA‐modified fibers to adhere to the PP matrix. Fiber volume fraction was the most important parameter as regards out‐of‐plane hygroexpansion, with a high‐fiber fraction leading to large hygroexpansion. Fiber‐matrix wettability during processing and consolidation also showed to have a large impact on the dimensional stability and moisture uptake. POLYM. COMPOS., 2009. © 2008 Society of Plastics Engineers     

拉伸速率对PLA/PUR–T材料拉伸行为与形态的影响

以聚乳酸(PLA)和热塑性聚氨酯(PUR–T)为基体,通过双螺杆挤出机进行熔融混合制备了一系列PLA/PUR–T(质量比分别为90/10,50/50,10/90)共混物,将共混物通过立式注塑机制备标准拉伸试样;再利用万能试验机制备了PLA/PUR–T材料的拉伸样条并对其进行了不同拉伸速率下的拉伸测试,选取不同拉伸状态下的试样分别进行扫描电子显微镜观察。结果表明,当PLA为基体相,PUR–T为分散相时,PLA/PUR–T材料的最大塑性应力较高,在较低的拉伸速率下,其材料的屈服平台区和断裂应力较大,断面形貌呈现液滴态–粗纤态–细纤态的演变,随着拉伸速率的升高,其材料的屈服平台区消失,断面形貌呈现粗纤态–细纤态的演变;当PUR–T为基体相,PLA为分散相时,PLA/PUR–T材料的最大塑性应力较低,其材料的表现出强烈的拉伸强化和极大的拉伸应变行为,断面形貌呈现连续的粗长纤态–细长纤态的演变。     

Treatment of ramie fiber with different techniques: the influence of diammonium phosphate on interfacial adhesion properties of ramie fiber-reinforced polylactic acid composite

Ramie fiber-reinforced polylactic acid (PLA) composites were successfully prepared by hot compression molding. Different treatment techniques were used to modify the surface of ramie fiber. The influence of diammonium phosphate (DAP) on the interfacial adhesion between ramie fiber and PLA composites was investigated by the contact angle measurements, FTIR and SEM analyses. The contact angle measurement results showed that alkali treatment combined with DAP was very efficient in decreasing the hydrophilicity of fibers. After treatment, the hydrophilicity of untreated ramie fiber from 5.9 ± 1.3 decreased to 2.0 ± 0.8 mJ/m². The wettability of alkali/silane/DAP-treated ramie fiber/PLA composite was higher (95.4° ± 1.3°) than that of pure ramie fiber/PLA composite (87.3° ± 1.9°). The FTIR results were consistent with the wetting measurements as the increment of hydrophilicity. Thermal analysis indicated that DAP-modified ramie fiber/PLA composites exhibited a lower thermal decomposition temperature, unique decomposition behavior and more residual char formation at decomposition temperature. The tensile, flexural and impact properties of DAP-modified ramie fiber composites were comparable to those of untreated ramie fiber composite. Moreover, proper alignment and uniform distribution of ramie fibers within the PLA matrix were found to be excellent. The morphological structures observed by SEM showed that well-modified ramie fibers enhanced the failure of the PLA composites in tensile, flexural and impact tests.     

Study on flax fiber toughened poly (lactic acid) composites

Poly (lactic acid) (PLA) is a renewable and biodegradable polymer with high modulus, high strength but low toughness. Blending PLA with plant fiber has been believed an available strategy to improve the toughness of PLA. PLA/Flax composites were fabricated by extrusion and injection molding processes. The flax fiber surfaces were modified before blending to improve the compatibility, and the chemical structures of both untreated and treated fiber were characterized by Fourier transform infrared spectroscopy. Results of mechanical test showed that the impact strength and elongation at break of PLA/Flax composites were remarkably higher than PLA. The impact fractures of PLA/Flax composites were also observed by scanning electron microscope. The results showed uniform dispersion of fibers in PLA matrix and good compatibility between treated fibers and PLA matrix. Moreover, it can be observed that crazing propagation was hindered by fibers and transcrystalline developed along fibers by polarized optical microscope. Differential scanning calorimetry analysis was carried out to study the crystallinity of PLA and it was found that incorporation of fiber improved the crystallinity of PLA. The toughening mechanism of PLA/Flax composites was discussed according to the results. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42573.     

Preparation,characterization, and mechanical properties of poly(ε‐caprolactone)/polylactic acid blend composites

Mechanical properties of poly(ε‐caprolactone) (PCL) and polylactic acid (PLA) blend reinforced with Dura and Tenera palm press fibers were studied. Dicumyl peroxide (DCP) was used as compatibilizer in the blend composites. Fourier transforms infrared spectrophotometer (FTIR) and field emission scanning electron microscope (FESEM) was used to study the effect of treatment on the fibers and fiber/matrix adhesion respectively. The uncompatibilized blend composites exhibited higher Young's modulus than the compatibilized blend composites. Impact strength of compatibilized blend composites of Tenera fibers (FM) increased by 161% at 10 wt% fiber load more than the uncompatibilized blend composites at same fiber load. The Dura fibers (FN) enhanced impact strength by 133% at 10 wt% fiber load. Tensile strength increased by 40% for compatibilized FM blend composites. In conclusion, it was observed that DCP incorporation resulted in good interfacial adhesion as revealed by the FESEM micrographs and evidenced in the improved mechanical properties. POLYM. COMPOS., 2013. © 2013 Society of Plastics Engineers     

On the effectiveness of the addition of milkweed floss fibers on processing and mechanical properties of PLA biocomposites

This study aimed at investigating the reinforcement effect of milkweed (MW) floss, a smooth and homogeneous natural fiber with a wide hollow lumen, on bio-based polymer composites. First, MW floss was thoroughly characterized in terms of morphology, surface roughness, and tensile and thermal resistance. Then, MW floss was compared to flax fibers, one of the most widely used natural fibers in the composite industry. Subsequently, bio-based composites made of polylactic acid (PLA) and 1 wt% MW floss were produced by injection molding and compared to composites reinforced with 1 wt% of flax fibers. Finally, thermal behavior, mechanical properties, and impact resistance of composites were determined. Results showed that MW floss, with respect to flax fibers, exhibits lower tensile modulus, ultimate tensile strength, surface roughness as well as a shorter critical length. Nonetheless, and despite the lower intrinsic properties of MW floss, UTS and impact resistance of MW/PLA composites were found to be 60% and 15% higher than those of Flax/PLA composites, respectively. In addition, micrographs of MW/PLA interface revealed a lack of adhesion in MW/PLA, which should be overcome by surface treatment in upcoming work.     

Preparation and properties of successive alkali treated completely biodegradable short jute fiber reinforced PLA composites

The natural fiber reinforced biodegradable polymer composites were prepared with short jute fiber as reinforcement in PLA (Poly lactic acid) matrix. The short jute fiber is successively treated with NaOH at various concentrations (5%, 10%, and 15%) and H₂O₂. The composites were prepared with untreated and treated short jute fibers at different weight proportions (up to 25%) in PLA and investigated for mechanical properties. The results showed that the composite with successive alkali treated jute fiber at 10% NaOH and H₂O₂ with 20% fiber loading has shown 18% higher flexural strength than neat PLA and untreated jute/PLA composite. The flexural modulus of the composite at 25% fiber loading was 125% and 110% higher than that of composites with untreated fibers and neat PLA, respectively. The impact strength of composite with untreated fibers at higher fiber weight fraction was 23% high as compared to neat PLA and 26% high compared to composite with treated fibers. The water absorption was more for untreated jute/PLA composite at 25% fiber loading than all other composites. The composite with untreated fibers has high thermal degradation compared with treated fibers but lower than that of pure PLA matrix. The enzymatic environment has increased the rate of degradation of composites as compared to soil burial. Surface morphology of biodegraded surfaces of the composites were studied using SEM method. POLYM. COMPOS., 37:2160–2170, 2016. © 2015 Society of Plastics Engineers     

Influence of pulp bleaching and compatibilizer selection on performance of pulp fiber reinforced PLA biocomposites

This article focuses on the effect of pulp bleaching and emerging commercial compatibilizers on physical performance of pulp fiber reinforced poly(lactic acid) (PLA) biocomposites. Industrially bleached and unbleached hardwood kraft pulp fibers are treated with several additive types, and compounded with PLA to fiber content of 30 wt %. After injection molding, the produced biocomposites are evaluated by their mechanical performance and fiber–matrix adhesion. For selected materials, fiber surface and fiber properties are reflected to composite performance by analyzing the compositions, dimensions, and lignin coverage of original fibers, as well as fiber dispersion and dimensions after melt processing. As a conclusion, unbleached kraft pulp fibers provide significant improvement in physical properties of PLA/pulp fiber composites. Of the screened compatibilizers, epoxidated linseed oil has a clear positive effect on performance when bleached kraft pulp fibers are used. The improvements correspond to enhanced fiber–matrix adhesion and differences in remaining fiber length distributions. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47955.     

Composites of poly(lactic acid) with flax fibers modified by interstitial polymerization

Natural fiber composites were designed and optimized to achieve good mechanical properties and resistance to growth of living organisms. Composite materials were prepared from poly(lactic acid) (PLA) with flax fibers, where the flax fibers had been subjected to interstitial polymerization to replace the water in the cellulose fibers. Before polymerization, the flax fibers were extracted with sodium hydroxide and acetone to remove lignin, pectin, and waxes from the cellulose. Differential scanning calorimetry was used to study the crystallization and melting of the composites as compared with pure PLA. The surface wetting of the fibers and morphology of the composites were studied by scanning electron microscopy and optical microscopy. Mechanical properties were studied using dynamic mechanical analysis. The influence of the interstitial polymerization on the dynamic storage modulus was found to be significant. The composites of polymerization treated flax, with acetone washed fibers, had higher storage moduli than the unwashed fiber composites, which suggested adhesion between flax fibers, and the matrix was improved by the treatments. The composites were subjected to moist environmental conditions to test for development of mold and fungi, and the acetone washed polymerization treated flax composites were resistant to these growths. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci, 2006     

Influence of surface treatment of carbon fibers on interfacial adhesion strength and mechanical properties of PLA‐based composites

In the present study C/PLA composites with different fiber surface conditions (untreated and with nitric acid oxidation for 4 h and 8 h) were prepared to determine the influence of surface treatment on the interfacial adhesion strength and mechanical properties of the composites. A chemical reaction at the fiber–matrix interfaces was confirmed by XPS studies. Nitric acid treatment was found to improve the amount of oxygen‐containing functional groups (particularly the carboxylic group, —COOH) on carbon fiber surfaces and to increase the surface roughness because of the formation of longitudinal crevices. The treated composites exhibited stronger interface adhesion and better mechanical properties in comparison to their untreated counterparts. There was a greater percentage of improvement in interfacial adhesion strength than in the mechanical properties. The strengthened interfaces and improved mechanical performance have been mainly attributed to the greater extent of the chemical reaction between the PLA matrix and the carbon fibers. The increased surface roughness also has had a slight contribution. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 80: 367–376, 2001     

Composites of poly(lactic acid) with flax fibers modified by interstitial polymerization

Natural fiber composites were designed and optimized to achieve good mechanical properties and resistance to growth of living organisms. Composite materials were prepared from poly(lactic acid) (PLA) with flax fibers, which had been subjected to interstitial polymerization to replace the water in the cellulose fibers. Prior to the polymerization, the flax fibers were extracted with sodium hydroxide and acetone to remove lignin, pectin, and waxes from the cellulose. Differential scanning calorimetry was used to study the crystallization and melting of the composites compared to pure PLA. The surface wetting of the fibers and morphology of the composites were studied by scanning electron microscopy and optical microscopy. Mechanical properties were studied using dynamic mechanical analysis. The influence of the interstitial polymerization on the dynamic storage modulus was found to be significant. The composites of polymerization treated flax with acetone washed fibers had higher storage moduli than the unwashed fiber composites, which suggested that the adhesion between the flax fibers and the matrix was improved by the treatments. The composites were subjected to moist environmental conditions in order to test for development of mold and fungi, and the acetone washed polymerization treated flax composites were resistant to these growths. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 3620–3629, 2006     

Studies of different kinds of fiber pretreating on the properties of PLA/sweet sorghum fiber composites

In this article, truly degradable composites were prepared using sweet sorghum fibers which are residue of ethanol fermentation industry as reinforcement and renewable resource‐based biodegradable polyester, poly(L ‐lactide) (PLLA) as matrix, they were fabricated by melt‐blending. The effect of different kinds of pretreatments (dilute sulfuric acid pretreatment, mild alkaline/oxidative pretreatment, steam explosion pretreatment) on mechanical properties of composites were investigated. Besides the composition of untreated and treated fibers as determined by Van soest method, Fourier transformed infrared (FTIR) spectroscopic and scanning electron microscopic (SEM) were also used to study the change of sweet sorghum fibers before and after pretreatments. Mechanical properties testing indicated that tensile strength and impact strength of PLLA/treated fibers were improved except the dilute sulfuric acid pretreated fibers reinforced PLA composite. The mild alkaline/oxidative pretreated fiber reinforced PLA composite showed highest tensile strength of 46.12 MPa and impact strength of 8.02 kJ/m² which was 15.5 and 33% higher than that of the control. The SEM of impact fracture surface and DMTA test were carried out to investigate the interfacial morphology and interfacial adhesion between the fiber and matrix. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

Preparation and Properties of α-Cellulose Short Fiber-Reinforced Poly(lactic Acid) Composites

The objective of this study is to fabricate the PLA/α-cellulose composites and to investigate the effect of α-cellulose short fibers on the toughness improvement of PLA. To homogeneously disperse the polar α-cellulose in the non-polar PLA matrix, the as-received α-cellulose was subjected to surface modification using stearic acid to impart the hydrophobic characteristics to the short fibers. The α-cellulose fibers dispersed more homogeneously in PLA through this modification, and consequently, the fiber pull-out and longer micro-crack length could improve the toughness and damping property of the resulting PLA composites. The inclusion of α-cellulose short fibers considerably decreased the spherulite dimension of the PLA/α-cellulose composites to accommodate larger deformation through grain boundary sliding. The PLA/α-cellulose composite improved its toughness by three times that of the neat PLA with low α-cellulose content (～4 wt.%), and maintained its transparency.     

PLA/lignocellulosic fiber composites: Particle characteristics,interfacial adhesion,and failure mechanism

Poly(lactic acid) (PLA) composites were prepared using six lignocellulosic fibers with widely varying particle characteristics. The composites were characterized by tensile testing, scanning electron (SEM), and polarization optical microscopy (POM). Micromechanical deformation processes during loading were followed by acoustic emission measurements. Interfacial adhesion was estimated by three independent methods. Contrary to most claims published in the literature, interfacial adhesion between PLA and natural fibers was found to be rather strong, a result confirmed by the quantitative estimation of adhesion strength, acoustic emission measurements, and SEM study. Strong interfacial adhesion results in weak dependence of the extent of reinforcement on the particle characteristics of the reinforcing fibers. Both acoustic emission measurements and microscopy indicated that the dominating micromechanical deformation process is the fracture of the fibers and close correlation was found between the initiation stress of fiber fracture, reinforcement, and the ultimate strength of the composites. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 39902.     

Effects of alkali and alkali/silane treatments of corn fibers on mechanical and thermal properties of its composites with polylactic acid

Different chemically modified (including treatments with alkali alone and a combination of alkali and silane coupling agent) corn fibers (CFs) have been used as reinforcements in polylactic acid (PLA) matrix to improve the mechanical and thermal properties of the CF/PLA composites. A comparative study has been made to find out how the two treatments affect the mechanical and thermal properties such as tensile, flexural, and impact strengths and glass transition temperature (T_g), crystallinity, and heat deflection temperature (HDT) of the CF/PLA composites. Scanning electron microscopy analyses have been conducted to evaluate the fiber–matrix adhesion. It has been observed that the treatment with a combination of alkali and silane is more efficient in strengthening fiber–matrix bonding, and thus more significantly improving the tensile and flexural strengths, crystallinity, T_g, and HDT of the CF/PLA composites than the treatment with alkali alone. However, alkali treatment produces the optimal impact strength. Mechanisms have been proposed to interpret the observed changes in mechanical and thermal properties as a result of fiber treatments. It is inferred that the surface treatment of CFs with a combination of alkali and silane may also be applied in other CF–polymer composite systems. POLYM. COMPOS., 37:3499–3507, 2016. © 2015 Society of Plastics Engineers     

Improvement in mechanical properties of grafted polylactic acid composite fibers via hot melt extrusion

The aim of this study was to develop fiber reinforced polylactic acid (PLA) composites via twin screw extrusion with the addition of a compatibilizer. Initial studies were performed to establish the optimum initiator percentage in terms of grafting efficiency between PLA and maleic anhydride (MA). Results show that PLA MA 7 obtained the highest level of grafting efficiency. Subsequent viscometric titration analysis on the compatibilized and uncompatibilized PLA composites showed an increase in the interfacial adhesion for the compatibilized PLA composites. Tensile and flexural properties also confirmed this increase in interfacial adhesion for the compatibilized composites, where the mechanical properties improved considerably, compared with virgin PLA and uncompatibilized composites. Results showed that the mechanical properties increase as PLA‐g‐MA loading increased. Finally, the rate of compostability of compatibilized composites decreased with the addition of PLA‐g‐MA. This was attributed to a lack of water absorption due to the bonding of hydroxyl groups on the fibers surface with MA. POLYM. COMPOS., 35:1792–1797, 2014. © 2014 Society of Plastics Engineers     

Properties of kenaf fiber/polylactic acid biocomposites plasticized with polyethylene glycol

Biocomposites of kenaf fiber (KF) and polylactic acid (PLA) were prepared by an internal mixer and compression molding. PLA was plasticized with polyethylene glycol (PEG) (10 wt%) and evaluated as the polymer matrix (p‐PLA). Fiber loadings were varied between 0 and 40 wt%. The tensile, dynamic mechanical, and morphological properties and water absorption behavior of these composites were studied. Reinforcing effect of KF was observed when fiber loading exceeded 10 wt% despite of the inferior fiber‐matrix adhesion observed via scanning electron microscopy (SEM). Un‐plasticized PLA/KF composite exhibited higher tensile properties than its plasticized counterpart. Fiber breakage and heavily coated short pulled‐out of fibers were observed from the SEM micrographs of the composite. The presence of PEG might have disturbed the fiber‐matrix interaction between KF and PLA in the plasticized composites. Addition of PEG slightly improved the un‐notched impact strength of the composites. Dynamic mechanical analysis showed that the storage and loss moduli of p‐PLA/KF composites increased with the increase in fiber loading due to increasing restrictions to mobility of the polymer molecules. The tan delta of the composites in contrast showed an opposite trend. p‐PLA and p‐PLA/KF composites exhibited non‐Fickian behavior of water absorption. SEM examination revealed microcracks on p‐PLA and p‐PLA/KF surfaces. POLYM. COMPOS., 31:1213–1222, 2010. © 2009 Society of Plastics Engineers     

Effect of glass fibers on rheology,thermal and mechanical properties of recycled PET

PET‐glass fiber composites were prepared by melt mixing of recycled PET with chopped glass fibers (15, 20, and 30 wt%) and their degree of dispersion was assessed by scanning electron microscopy. Rotational rheometry was employed to analyze the interfacial shear strength between the fibers and polymer matrix in the molten state. The composite containing 30 wt% of glass fibers revealed a moderate G′ secondary plateau; hence strong fiber‐matrix interactions were confirmed. Results of mechanical testing were in a good accordance with structural and rheological measurements. The higher rate of mixing under production‐scale conditions resulted in lower fiber‐matrix adhesion and in a similar level of fiber dispersion as compared to the same mixture compounded on pilot‐plant scale. Thermal characterization of the composites was performed by differential scanning calorimetry and total crystalline fraction was analyzed. POLYM. COMPOS., 2008. © 2008 Society of Plastics Engineers     

剑麻纤维增强聚乳酸复合材料酶降解研究

通过热压成型的方式制备了剑麻纤维增强聚乳酸（PLA/SF）复合材料,并通过K蛋白酶降解方式研究了该复合材料的生物降解性能,利用差热扫描量热仪测试分析了复合材料在酶降解过程中的非等温结晶性能。研究发现,剑麻纤维的加入加快了聚乳酸及其复合材料的降解速率,且随着剑麻纤维含量的增加,其降解速率提高;剑麻纤维的加入对聚乳酸的结晶性能有一定的影响,进而也影响了复合材料的酶水解速度。