Biodegradability and mechanical properties of agro‐flour–filled polybutylene succinate biocomposites

The objective of this study was the production of rice husk flour (RHF) and wood flour (WF) filled polybutylene succinate (PBS) biocomposites as alternatives to cellulosic material filled conventional plastic (polyolefins) composites. PBS is one of the biodegradable polymers, made from the condensation reaction of 1,4‐butanediol and succinic acid that can be naturally degraded in the natural environment. We compared the mechanical properties between conventional plastics and agro‐flour–filled PBS biocomposites. We evaluated the biodegradability and mechanical properties of agro‐flour–filled PBS biocomposites according to the content and filler particle size of agro‐flour. As the agro‐flour loading was increased, the tensile and impact strength of the biocomposites decreased. As the filler particle size decreased, the tensile strength of the biocomposites increased but the impact strength decreased. The addition of agro‐flour to PBS produced a more rapid decrease in the tensile strength, notched Izod impact strength, and percentage weight loss of the biocomposites during the natural soil burial test. These results support the application of biocomposites as environmentally friendly materials. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 97: 1513–1521, 2005     

Development and study of fully biodegradable composite materials based on poly(butylene succinate) and hemp fibers or hemp shives

The use of natural fibers to reinforce polymers is an established practice, and biocomposites have gained an increased interest in areas such as automotive, construction, and agriculture. The purpose of the present work was the preparation and study of fully biodegradable (“green”) composite materials using poly(butylene succinate) (PBSu) as polymeric matrix and hemp fibers and shives as fillers. Composites containing 15, 30, 50, 60, and 70 wt% of fillers were prepared by melt mixing in a twin screw extruder. The composites were studied using Fourier transform infrared spectroscopy, X‐ray diffraction, and differential scanning calorimeter while the dispersion and interfacial adhesion were studied with scanning electron microscopy. From mechanical properties measurements, it was found that tensile and impact strength are both affected by the type and the amount of the used filler. The degree of crystallinity of PBSu was found to decrease by increasing the filler content, although that both fillers can act as nucleating agents. Finally, the degradation rate during enzymatic hydrolysis and soil burial increased in all biocomposites by increasing the filler content. PBSu/hemp shive composites showed higher biodegradation rates than PBSu/hemp fiber composites. POLYM. COMPOS., 37:407–421, 2016. © 2014 Society of Plastics Engineers     

Rice husk‐derived porous carbon/silica particles as green filler for electronic package application

Bio‐based porous carbon/silica particles (denoted as RH‐carbon/silica) were successfully prepared from agricultural waste rice husk by using acid‐hydrothermal treatment and pyrolysis under nitrogen condition. As green filler, the cure behavior, thermal‐mechanical properties, and thermal conductivity of the epoxy‐carbon/silica biocomposites at different filler contents (5, 9, 17, 29 wt %) were characterized. Because of superior surface properties (surface area, porosity, and silica segment) and high content of carbon component in the RH‐carbon/silica, the characteristics of the biocomposites were significantly improved with the increase of the filler content. At 29 wt % of filler content, the epoxy biocomposites exhibit lower curing temperature (148 °C), lower CTE (42 ppm/°C), higher T_g (123 °C), higher storage modulus (4059 MPa), and higher effective thermal conductivity (0.29 W/mK). In brief, the RH‐carbon/silica particles that can serve not only as reinforcing agent but also as thermal transport medium used in epoxy composite, is a green and high‐performance filler for this purpose. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44699.     

Thermal pretreatment of kudzu biomass (pueraria lobata) as filler in cost‐effective pla biocomposite fabrication process

This article aims on the fabrication of cost‐effective polylactic acid (PLA) biocomposites using kudzu biomass derivatives as new filler. In this way, it has been realized that pretreatment of the filler was an essential requirement. We demonstrated thermal pyrolysis process that targeted to extraction and isolation of all extractable and unnecessary compounds such as intracellular water and bio‐oil from the biomass. Also, to further improve the compatibility of the filler with PLA, noncatalytic thermal esterification reactions of kudzu after thermal pyrolysis (called char) were carried out as second pretreatment stage in the presence of phthalic anhydride. Kudzu derivatives obtained from either first or second pretreatment reactions were melt‐blended with PLA in various rates. The blends were then compression molded into dumbbell specimens. Physicomechanical properties of the prepared biocomposites were evaluated using several analytical techniques. It was found that biocomposites containing treated biomass had higher values of physicomechanical properties than untreated ones. The final rate of filler to PLA with acceptable properties was set up to 50%. Obviously, the cost of PLA can be reduced using higher rates of low‐cost filler on a finished‐product basis. Extracted valuable compounds from biomass via thermal pyrolysis could be another benefit of the process. POLYM. ENG. SCI., 55:340–348, 2015. © 2014 Society of Plastics Engineers     

Mechanical and thermal properties of coconut shell powder filled polylactic acid biocomposites: effects of the filler content and silane coupling agent

The effects of the filler content and the coupling agent 3-aminopropyltriethoxysilane (3-APE) on the mechanical properties, thermal properties, and morphologies of polylactic acid (PLA)/coconut shell powder (CSP) biocomposites were investigated. It was found that increasing the CSP content decreased the tensile strengths and elongations at break of the PLA/CSP biocomposites. However, incorporating CSP increased their modulus of elasticity. The tensile strengths and modulus of elasticity of the PLA/CSP biocomposites were enhanced by the presence of 3-APE, which can be attributed to a stronger filler–matrix interaction. The thermal stabilities of the biocomposites increased with the filler content, and they were enhanced by 3-APE treatment. Meanwhile, the presence of CSP increased the glass transition temperatures (T _g) and crystallinities (X _c) of the PLA/CSP biocomposites at a filler content of 30 php. After 3-APE treatment, T _g and X _c of the PLA/CSP biocomposites increased due to enhanced interfacial bonding. The presence of a peak crystallization temperature (T _c) for the PLA/CSP biocomposites indicated that the CSP has a nucleating effect. The melting temperatures (T _m) and the T _c values of the biocomposites were not significantly affected by the filler content and 3-APE. PLA/CSP biocomposites that had been treated with 3-APE presented the strongest filler–matrix interaction, as confirmed by SEM.     

A study on the moisture sorption characteristics in woven sisal fabric reinforced natural rubber biocomposites

Textile biocomposites were prepared by reinforcing natural rubber with woven sisal fabric. Sisal fabric was subjected to various chemical modifications like mercerization, silanization, and thermal treatment. The moisture uptake of the textile composites was found to depend upon fiber content as well as architecture. The mechanism of diffusion in the composites was found to be fickian in nature. The effect of chemical modification of sisal fabric on moisture uptake was also analyzed. Mercerization was seen to increase the water uptake in the composites while thermally treated fabric reinforced composites exhibited lower water uptake. The influence of temperature on water sorption of the biocomposites is also analyzed. The thermodynamic parameters of the sorption process were also evaluated. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 416–423, 2006     

Fabrication, characterization and bioactivity evaluation of calcium pyrophosphate/polymeric biocomposites

The design of the biocomposites offers the opportunity to create grafting materials with excellent bioactivity, resorbability and improved mechanical properties. In this study, we are concerned with the preparation of calcium pyrophosphate (CPP) and its composites with polymeric matrix to enhance these properties. The fabricated biocomposites were characterized by X-ray diffraction (XRD), Fourier transformer infrared spectra (FT-IR), thermogravimetric (TGA) analyses and scanning electron microscope with X-ray elemental analysis (SEM-EDAX). The characterization results confirmed homogeneity, interaction and integration between the CPP filler and polymeric matrix. The mechanical properties of biocomposites had enhanced values compared to the original copolymer matrices and were comparable to those of cancellous bone. In vitro test results via calcium and phosphorous ions measurements, showed that the biocomposites had enhanced ability to accelerate the mineralization of calcium phosphate layer on their surfaces. FT-IR and SEM-EDAX post-immersion confirmed that the CPP/polymeric composites containing chitosan or chitosan–gelatin matrix had ability to induce a bone-like apatite layer onto their surfaces. Finally, a novel CPP/polymeric biocomposites have good bioactivity and suitable mechanical properties; therefore, they could be used in bone grafting and tissue engineering applications in future.     

Influence of heat treatment on the heat distortion temperature of poly(lactic acid)/bamboo fiber/talc hybrid biocomposites

Influence of heat treatment and fillers on the heat distortion temperature (HDT) of poly(lactic acid) hybrid biocomposites was intensively studied through HDT testing, polarizing microscope (POM), differential scanning calorimetry (DSC), and dynamic mechanical analysis (DMA). With loading 20 wt % BF or 20 wt % talc, improvement of HDT in PLA composite was about 10°C comparing with neat PLA after heat treatment. Moreover, there was a great improvement (above 45°C) of HDT in PLA composites with loading 20 wt % BF and 20 wt % talc simultaneously after heat treatment. Transcrystallization was observed during heat treatment and isothermal crystallization of PLA composites with loading BF and talc simultaneously. There was no similar phenomenon in other PLA composite with loading only one filler. The possible mechanism of forming transcrystallization was proposed. DSC and DMA were also used to clarify the variation in HDT before and after heat treatment, and the results suggest that the crystallinity, modulus and glass transition changed, especially formation of transcrystallization played a key role in improvement of HDT in PLA composites. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Preparation and properties of tung oil-based composites using spent germ as a natural filler

Novel biocomposites have been prepared by the free radical polymerization of a tung oil-based resin using spent germ, the coproduct of wet mill ethanol production, as a filler. The effect of filler particle size, amount of filler, amount of crosslinker, and molding pressure on the resulting composites has been investigated. When compared to the pure resin, an increase in storage modulus is observed when filler is added to the matrix. The thermal stabilities of the resulting composites lie between the stabilities of the resin and the spent germ. Decreasing the particle size results in an increase in both the storage modulus and the mechanical properties of the composites. As the amount of crosslinker, divinylbenzene, increases, an improvement in the thermal stabilities and mechanical properties is observed. The composites prepared are mainly composed of renewable resources, possess good thermal and mechanical properties, and have potential applications in the construction and automotive industries. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Effect of fiber volume fraction on the thermal and mechanical behavior of polylactide‐based composites incorporating bamboo fibers

Biodegradable composites reinforced with natural fibers are emerging as advanced materials in structural applications. In this work, green biocomposites are fabricated using hot pressing molding technique, polylactic acid selected as a matrix. The samples are prepared with different fiber volume fractions (30%, 40%, and 50%). Tensile tests are conducted on the specimens to investigate the composite mechanical behavior, and the influences of fiber content on the morphological and thermomechanical properties are evaluated using scanning electron microscopy, differential scanning calorimetry, and thermogravimetric analysis. There are higher tensile modulus and lower elongation at break for composites with increasing fiber content, respectively. Much variation in the tensile strength is observed when the fiber content is varied, which could be attributed to fiber agglomerations that affect the dispersion of fibers in the matrix, as evidenced by fracture surfaces. Thermal tests demonstrate that the increment of fiber content enhances the glass transition temperature and crystallization temperature of composites. Besides, a comparative analysis of the composites is performed, and the properties of the treated fiber composites are found to be improved compared to those from untreated fibers. Detailed analysis confirms the possibility of the addition of bamboo fibers to a biodegradable matrix for a specific application. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46148.     

Jatropha deoiled cake filler‐reinforced medium‐density polyethylene biocomposites: Effect of filler loading and coupling agent on the mechanical,dynamic mechanical and morphological properties

This work focuses on the performance of Jatropha deoiled cake (JOC) as filler for medium‐density polyethylene. The biocomposites were prepared using a melt‐compounding technique. Maleated polyethylene (MPE) was used as a reactive additive to promote polymer/filler interfacial adhesion. The mechanical, thermodynamic mechanical and morphological properties of the resultant composites were investigated. The results show that the incorporation of JOC into the matrix reduced tensile, flexural, and impact strengths compared with the pure matrix. Moreover, tensile and flexural moduli were increased. The composites prepared with MPE had better mechanical properties and lower water uptake, indicating an enhancement in the interfacial interaction between JOC and polyethylene systems. The storage modulus was increased by the increase in filler loading and decreased when MPE was used. The composites loss modulus curves revealed two glass transitions indicating partial miscible blends. Scanning electron microscopy analysis for maleated composites showed a relatively homogeneous morphology with few left cavities, and the filler particle size is smaller compared to nontreated composites. POLYM. COMPOS., 2013. © 2013 Society of Plastics Engineers     

Effect of filler surface treatment on the properties of recycled high‐density polyethylene/(natural rubber)/(Kenaf powder) biocomposites

Biocomposites were prepared from a kenaf core powder and recycled high‐density polyethylene/(natural rubber) blend by using an internal mixer at 165^oC and 50 rpm. The effect of the filler content and the filler surface treatment was studied. Chemical modification of kenaf filler was performed with alkali pretreatment followed by treatment with silane. Scanning electron microscopy and infrared spectroscopy studies confirmed changes in the chemical compositions and structural characteristics induced through the modification. It was found that treated biocomposites offered higher tensile strength and tensile modulus, but lower elongation at break compared with untreated biocomposites. Lower water absorption and higher thermal stability of the resultant biocomposites were also obtained when treated fillers were used. J. VINYL ADDIT. TECHNOL., 20:218–224, 2014. © 2014 Society of Plastics Engineers     

Preparation and morphological,thermal, and physicomechanical properties of polypropylene‐potato peel biocomposites

Potato peel powder (POPL), which is biodegradable, has been used as filler material in polypropylene (PP) matrix in varying concentration from 10 to 40% by weight to prepare biocomposites and investigated water absorption, physicomechanical and thermal properties. Scanning electron microscopy and X‐ray diffraction has been used for morphological characterization and crystallization studies. Flexural modulus of biocomposites increased by 40% compared with neat PP at 30% loading of POPL. Flexural strength also increased with increasing filler loading. Tensile strength of biocomposites has been observed to be comparable with neat PP up to 20% filler loading and increase in tensile modulus up to 40% was seen in biocomposites with 20% filler loading. Impact strength of biocomposites up to 20% filler loading was found to be at par with neat PP. Use of MA‐g‐PP compatibilizer in the biocomposites yielded better physico‐mechanical and thermal properties than biocomposites without compatibilizer. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42445.     

“True” biocomposites with biopolyesters and date seed powder: Mechanical,thermal, and degradation properties

Biopolymers have gained research focus due to enhanced property profiles as well as need to replace the fossil fuel based polymeric materials. The generation of biocomposites with functional biofillers can lead to further enhancement of their potential. In this study, composites of date seed powder with biopolyesters poly(butylene adipate‐co‐terephthalate) (PBAT) and poly‐l ‐lactide (PLA) have been demonstrated. The composites exhibited individual degradation peaks for the components in the thermogravimetric analysis (TGA), but still had suitable thermal performance confirmed by the dynamic TGA. The filler also modified the crystalline morphology of the polymers differently. The tensile modulus of the PBAT‐based composites had enhancement of more than 300% in the composite with 40% filler content. The PLA composites also enhanced the modulus marginally till 20% filler content, however, it was still significant due to the very high modulus of PLA as compared to PBAT. The rheological properties indicated the polymer still had viscous behavior even when high amount of filler was added. The storage and loss modulus of the composites enhanced with filler fraction, the PLA composites with 30 and 40% content, however, exhibited very high values probably due to filler aggregates and low filler‐polymer interfacial interactions. The filler particles were observed to be uniformly distributed in the polymer matrices, though some filler aggregates were also observed in the composites with higher filler fractions. After embedding in compost soil, the composites had significantly enhanced extent of biodegradation as compared to pure polymers, thus, confirming the “true” biocomposite nature. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40816.     

Preparation and characterization of chitosan/KSF biocomposite film

Chitosan–clay biocomposites have been prepared in which KSF‐montmorillonite (KSF) is used as filler and diluted acetic acid is used as solvent for dissolving and dispersing chitosan and montmorillonite, respectively. The effect of KSF loadings in biocomposites has been investigated. The characterization with different methods (FTIR, DSC, TGA, SEM, and XRD) on chitosan/KSF biocomposites systems was examined. Morphology and properties of chitosan biocomposites have been studied compared with those of pure chitosan. The FTIR and SEM results indicated the formation of an intercalated‐and‐exfoliated structure at low KSF content and an intercalated‐and‐flocculated structure at high KSF content. The thermal stability and the mechanical properties of the composites were also examined by DSC, TGA/DTG, and tensile strength measurements, respectively. The dispersed clay improves the thermal stability of the matrix systematically with the increase of clay loading. Tensile strength of a chitosan film was enhanced until the clay ratio up to 2 wt% and elongation‐at break decreased with addition of clay into the chitosan matrix. The XRD results confirmed the intercalation of the biopolymer in the clay interlayer by the decrease of 2θ values while the chitosan–clayratio increases. POLYM. COMPOS., 2009. © 2008 Society of Plastics Engineers     

Properties of silanized nypa fruticans filled polylactic acid/recycled low density polyethylene biocomposites

The biocomposites of Nypa Fruticans (NF) and Polylactic acid (PLA)/recycled low density polyethylene (rLDPE) were prepared using Brabender EC PLUS. The effect of NF content and silane coupling agent on mechanical, thermal, and morphological properties were studied. The results show that addition of NF in PLA/rLDPE biocomposites have decreased the tensile strength, elongation at break, and crystallinity of biocomposites. The Young's modulus of biocomposites and thermal stability increased with the increasing NF content. The surface of NF fillers were silanized to improved the interfacial adhesion between the NF filler and PLA/rLDPE matrix. It was found that the tensile strength, Young's modulus, crystallinity of PLA, and thermal stability of silanized biocomposites higher as compared to untreated biocomposites. The enhancement of the properties of biocomposites with silane treatment was proven by SEM studied. The silanized biocomposites showed better interfacial interaction and adhesion between NF and PLA/rLDPE matrix. POLYM. ENG. SCI., 55:1733–1740, 2015. © 2014 Society of Plastics Engineers     

Reinforcement effect of biomass carbon and protein in elastic biocomposites

Biomass carbon (BC) and soy protein (SP) were used to reinforce natural rubber (NR) biocomposites. The particle size of BC was reduced and characterized with elemental analysis, X‐ray diffraction, infrared spectroscopy, and particle size analysis. The rubber composite reinforced with the BC/SP and the composite reinforced with the BC of higher carbon content show useful tensile properties at an optimum filler fraction. The model analysis of the stress–strain behaviors provides insight into filler network characteristics. For the highly filled composites, the BC have less constraint on the polymer chains as shown by the temperature and frequency dependent modulus as well as the model analysis of stress softening effect. The presence of NR protein improves the filler–polymer adhesion for the composites reinforced with BC/SP. POLYM. COMPOS., 2013. © 2013 Society of Plastics Engineers     

The Influence of Green Surface Modification of Oil Palm Mesocarp Fiber by Superheated Steam on the Mechanical Properties and Dimensional Stability of Oil Palm Mesocarp Fiber/Poly(butylene succinate) Biocomposite

In this paper, superheated steam (SHS) was used as cost effective and green processing technique to modify oil palm mesocarp fiber (OPMF) for biocomposite applications. The purpose of this modification was to promote the adhesion between fiber and thermoplastic. The modification was carried out in a SHS oven at various temperature (200–230 °C) and time (30–120 min) under normal atmospheric pressure. The biocomposites from SHS-treated OPMFs and poly(butylene succinate) (PBS) at a weight ratio of 70:30 were prepared by melt blending technique. The mechanical properties and dimensional stability of the biocomposites were evaluated. This study showed that the SHS treatment increased the roughness of the fiber surface due to the removal of surface impurities and hemicellulose. The tensile, flexural and impact properties, as well as dimensional stability of the biocomposites were markedly enhanced by the presence of SHS-treated OPMF. Scanning electron microscopy analysis showed improvement of interfacial adhesion between PBS and SHS-treated OPMF. This work demonstrated that SHS could be used as an eco-friendly and sustainable processing method for modification of OPMF in biocomposite fabrication.     

Interfacial interactions in calcium carbonate–polypropylene composites. 2: Effect of compounding on the dispersion and the impact properties of surface-modified composites

This study was carried out to investigate the influences of compounding process and surface treatment on calcium carbonate (CaCO₃) filled polypropylene. The compounding process is discussed with reference to a twin-screw extruder and an internal mixer. The calcium carbonate filler was surface-treated with a liquid titanate coupling agent (LICA 12) and stearic acid. Composites of different weight fractions were prepared by both compounding processes, and their impact properties were evaluated. The notched Izod impact strength increased with CaCO₃ content up to a maximum at about 10 vol%, and then decreased. Surface treatment of CaCO₃ filler generally yielded composites of higher impact strength than untreated system. Though LICA 12 was more effective than stearic acid in modifying the filler, the low-cost stearic acid proved to be more effective when dealing with the impact properties of composites. Moreover, the composites from a Brabender Plasti-corder exhibited better gross uniformity than that from the twin-screw extruder. However, good filler dispersion and uniform microscopic morphology, as revealed by SEM microscopy, was observed in the samples from the twin-screw extruder. Polym. Compos. 25:451–460, 2004. © 2004 Society of Plastics Engineers.