Fibre/matrix adhesion of cellulose fibres in PLA,PP and MAPP: A critical review of pull-out test,microbond test and single fibre fragmentation test results

The present work deals with the practical fibre/matrix adhesion of regenerated cellulose fibres (lyocell) and bast fibre bundles (flax, kenaf) in different matrices (polylactide-PLA, polypropylene-PP, maleic-anhydride-grafted polypropylene-MAPP). The influence of different testing procedures (pull-out test, microbond test, fragmentation test) on the fibre/matrix characteristics is discussed. The results of the different tests showed the same trends, but the absolute values differ. Clearly higher interfacial shear strength (IFSS) for cellulose fibres was found in PLA and MAPP in comparison to PP due to higher polarity. In addition, bast fibres displayed higher apparent IFSS values compared to lyocell because of their rougher surface and their chemical composition. The apparent IFSS of the pull-out test resulted in higher values compared to results obtained from the fragmentation test. This phenomenon is explained by different stress distributions due to variable specimen geometry, different behaviour of failure and the friction which occurs between fibre and matrix during fibre pull-out in the pull-out test.     

Effect of additives on the interfacial strength of poly(l-lactic acid) and poly(3-hydroxy butyric acid)-flax fibre composites

The interfacial shear strength (IFSS), evaluated by single fibre pull-out tests was quantified for various biopolymer-flax fibre composites that were modified with additives. The additives included a plasticiser (glycerol triacetate) (GTA) absorbed onto/into the fibres, 4,4′-thiodiphenol (TDP) that is capable of forming hydrogen bonds between the matrix and cellulose from the fibres, and a hyperbranched polyester (HBP) to impart improved fracture toughness. Fibres were washed with acetone to remove the surface impurities and dried under vacuum before absorption of plasticiser and adsorption of thiodiphenol. It was found that the different additives significantly influenced the IFSS for the biopolymer-flax fibre systems while extraction with acetone had a no effect on the IFSS compared with the untreated fibres. The use of TDP imparted the most significant increase in IFSS whilst the HBP had an opposing effect. The use of ESEM corroborated with the findings of the single fibre pull-out tests.     

电晕处理对高性能PBO纤维的表面性能及其界面粘接性能的影响

对高性能PBO纤维表面进行了电晕处理,优化了其处理工艺。用XPS,FT-IR和SEM研究了处理前后纤维表面化学结构及物理结构的变化,通过单丝拔出试验和短梁剪切试验评价了PBO纤维与树脂基体的微宏观界面粘接性能。结果表明:经电晕处理后,PBO纤维表面含氧量增多,表面浸润性得到改善,单丝拔出的PBO-环氧界面剪切强度(IFSS)提高了25.6 ％,但短梁剪切强度(ILSS)的提高不明显。     

Determination of interfacial shear strength of white rot fungi treated hemp fibre reinforced polypropylene

Short untreated and white rot fungi treated hemp fibre, polypropylene (PP) and maleated polypropylene (MAPP) coupling agent were extruded and injection moulded into composite tensile test specimens. The tensile properties of untreated and treated fibre and their composites were measured. The fibre length distributions in the composite were obtained by dissolving the PP/MAPP matrix in boiling xylene to extract the fibre. Both the Single Fibre Pull-Out test and the Bowyer and Bader model were used to determine the interfacial shear strength (IFSS) of these composites. IFSS was found to be lower for the Single Fibre Pull-Out test, which was considered to be largely due to axial loading of fibre and the resulting Poisson’s contraction occurring during this technique. This suggests that the Bowyer and Bader model provides a more relevant value of IFSS for composites. The results obtained from both methods showed that IFSS of the treated fibre composites was higher than that for untreated fibre composites. This supports that the hemp fibre interfacial bonding with PP was improved by white rot fungi treatment.     

Visualization of dynamic fiber-matrix interfacial shear debonding

To visualize the debonding event in real time for the study of dynamic crack initiation and propagation at the fiber–matrix interface, a modified tension Kolsky bar was integrated with a high-speed synchrotron X-ray phase-contrast imaging setup. In the gage section, the pull-out configuration was utilized to understand the behavior of interfacial debonding between SC-15 epoxy matrix and S-2 glass fiber, tungsten wire, steel wire, and carbon fiber composite Z-pin at pull-out velocities of 2.5 and 5.0 m s^?1. The load history and images of the debonding progression were simultaneously recorded. Both S-2 glass fiber and Z-pin experienced catastrophic interfacial debonding whereas tungsten and steel wire experienced both catastrophic debonding and stick–slip behavior. Even though S-2 glass fiber and Z-pin samples exhibited a slight increase and tungsten and steel wire samples exhibited a slight decrease in average peak force and average interfacial shear stress as the pull-out velocities were increased, no statistical difference was found for most properties when the velocity was increased. Furthermore, the debonding behavior for each fiber material is similar with increasing pull-out velocity. Thus, the debonding mechanism, peak force, and interfacial shear stress were rate insensitive as the pull-out velocity doubled from 2.5 to 5.0 m s^?1. Scanning electron microscope imaging of recovered epoxy beads revealed a snap-back behavior around the meniscus region of the bead for S-2 glass, tungsten, and steel fiber materials at 5.0 m s^?1 whereas those at 2.5 m s^?1 exhibited no snap-back behavior.     

Evaluation of three in-plane shear test methods for advanced composite materials

This paper is concerned with the evaluation of three in-plane shear test methods for advanced carbon fibre composites for aerospace applications. To accomplish this goal, the losipescu, ± 45° tensile and 10° off-axis tensile shear test methods were evaluated for three advanced epoxy matrix materials (Narmco 5245C, Hexcel F584 and American Cyanamid Cycom 1806) reinforced with Hercules IM6 carbon fibres. The values of in-plane shear moduli obtained from the three test methods and three materials were then used with other previously determined elastic constants to predict the tensile moduli of (+45°/0°/−45°/90°)_6s laminates. Comparison of the predicted and experimental laminate tensile moduli showed that any one of the three shear test methods was appropriate for determining the in-plane shear modulus to predict tensile moduli of symmetric laminates which consist of equal numbers of 0°, +45°, −45° and 90° oriented laminae.     

The effect of moisture on the shear properties of carbon fibre composites

A study was made of the effect of moisture on the mechanical properties of composites (carbon fibre-reinforced epoxy resins) which are dominated by the matrix or matrix/fibre interface. Such properties are the interlaminar shear strength in unidirectional laminates and tensile strength in (± 45) laminates. Unidirectional material was either immersed in boiling water or aged in a hot-humid atmosphere and then the interlaminar shear strength was measured at room temperature in short beam bending. The values obtained were found to be independent of the mode of exposure but depended on the amount of moisture present in the composite. The (± 45) material was aged at 70°C and 95% relative humidity to accelerate the moisture uptake and then tested at 20°C, 70°C, 110°C and 130°C. At test temperatures above 70°C the tensile strength decreased as the composite absorbed moisture. Plasticization, swelling and debonding were identified as the factors affecting the failure mechanisms in these laminates.     

Transcrystallisation in PP/flax composites and its effect on interfacial and mechanical properties

The effect of flax fibre reinforcement on the crystallisation behaviour of polypropylene (PP) was investigated using a hot-stage polarising optical microscope. To follow the crystallisation kinetics, crystallisation temperature and time were varied. At crystallisation temperatures between 130 and 138 °C the most uniform and thickest transcrystalline layers were formed. The effect of transcrystallisation on the interfacial shear strength (IFSS) in micro-composites was studied by the fibre pull-out test method. It was found that the IFSS of the PP/flax system is slightly decreased with the presence of a transcrystalline interphase. Finally, the influence of the formation of a transcrystalline zone on the macromechanical properties of compression moulded PP/flax composites was studied.     

Synergy of matrix and fibre modification on adhesion between carbon fibres and poly(vinylidene fluoride)

Interfacial properties between carbon fibres and poly(vinylidene fluoride) (PVDF) were tuned by modifying both constituents. Atmospheric plasma fluorination (APF) was utilised to tailor the surface composition of carbon fibres, which resulted in an incorporation of up to 3.7 at.% of fluorine functionalities in to the fibre surfaces. The PVDF matrix was modified by blending pure PVDF with maleic anhydride (MAH) grafted PVDF. Both fibre and matrix modifications act in synergy with improvements of up to 50% in the apparent interfacial shear strength (IFSS) above the level of pure fibre or matrix modification. Modification of both constituents led to the formation of various interactions at the fibre/matrix interface namely dispersive and polar (H-bonds) between (modified) PVDF and the fluorine as well as oxygen functionalities on the fibre surfaces. The apparent IFSS between the modified fibres and matrix reaches a maximum of 42 MPa, which is almost the tensile strength of the pure PVDF. The improvements in apparent IFSS in single fibre model composites for both fibre and matrix modifications translated to a seven times improvement in the interlaminar shear strength of unidirectional composites.     

高性能有机纤维单丝复合体系界面粘结性能实验研究

采用单丝复合体系多次断裂法,通过对纤维单丝断点数的统计及其断点形貌的分析,考察了PBO纤维、芳纶Twaron纤维、超高分子量聚乙烯纤维(UHMWPE)3种高性能有机纤维与韧性环氧基体的界面剪切强度;并对比考察了界面剪切强度与对应复合材料单向板层间剪切强度之间的关系;结合XPS、SEM等手段分析了有机纤维表面物理化学特性对界面剪切强度的影响。结果表明,Twaron/环氧的界面剪切强度高于PBO/环氧,UHMWPE/环氧的界面粘结弱,该方法不能测试;上述体系界面剪切强度与对应的复合材料单向板层间剪切强度变化趋势是一致的;表面化学活性高的纤维对应的界面剪切强度高。     

Analysis of the single-fibre pull-out test by means of Raman spectroscopy: Part II. Micromechanics of deformation for an aramid/epoxy system

The single-fibre pull-out test has been analysed for Kevlar-49 fibres in a cold-cured epoxy resin by using both a conventional pull-out experiment and Raman spectroscopy. The interfacial shear strength (ISS) has been estimated from the pull-out force for fibres with a range of embedded lengths. Raman spectroscopy has been used to analyse the distribution of fibre strain in the pull-out test by mapping the variation of strain along an aramid fibre undergoing pull-out from the epoxy resin matrix. At low strains the behaviour follows elastic shear-lag analysis but, as the fibre strain is increased, debonding takes place at the fibre/matrix interface. It is found that this debond propagates along the interface until the entire fibre is debonded. The fibre is then pulled out of the resin matrix by a frictional pull-out process. It is shown that the conventional pull-out experiment produces only an apparent value of ISS and that through a partial-debonding model it is possible to use the interfacial parameters obtained from the Raman analysis to predict the data from the conventional test.     

Direct measurements of interfacial shear strength of multi-walled carbon nanotube/PEEK composite using a nano-pullout method

This paper presents a proposal of a simple and easy method to evaluate the interfacial shear strength (IFSS) of CNT-dispersed polymer composites. An individual multi-wall carbon nanotube (MWNT) was pulled out from a MWNT-dispersed/PEEK composite using a nano-pullout testing system installed in an SEM. The tensile load was measured using the elastic deformation of an AFM cantilever. The pull-out length was controlled by making a through-thickness hole near the specimen edge using a focused ion beam (FIB) system. The IFSS of a MWNT/PEEK composite was measured as 3.5-14 MPa, which agrees with the IFSS estimated from the macroscopic stress-strain behavior of the MWNT/PEEK composites.     

The glass fibre-polymer interface: II—Work of fracture and shear stresses

Pull-out experiments have been carried out on single production fibres under carefully controlled conditions. Four parameters were determined. The interfacial yield stresses, of about 9–14 MPa, were very much smaller than the shear strengths of the bulk polymers in the case of an epoxy, whether post-cured or not, and a non-post-cured polyester. Values for the work of fracture of the interface varied from 140 to 300 Jm^?2, and again were less than those of the polymer. Interface failure sometimes took place in the epoxy rather than at the fibre surface, whereas with the polyester it always took place at the fibre surface. After interface failure, pull-out was governed by friction, with maximum shear stresses of 7–10 MPa for polyester, and 21–34 MPa for epoxy, the higher values being obtained for the post-cured resins. Average frictional shear stresses were sometimes less than a half of the maximum shear stress, indicating that the fibre Poisson's shrinkage was playing an important role in the pull-out process. A silicone release agent reduced the frictional shear stresses to 2·5 MPa, with both resins.     

电晕处理对超高分子量聚乙烯纤维表面性能的影响

对超高分子量聚乙烯（UHMWPE）纤维表面进行了电晕处理,用XPS,FT-IR和SEM研究了处理前后纤维表面化学结构及物理结构的变化,通过单丝拔出试验和短梁剪切试验评价了UHMWPE纤维与树脂基体的微宏观界面粘接性能,结果表明：经电晕处理后,UHMWPE纤维表面含氧量增多,含氧基团数量与种类增加,表面浸润性得到改善,纤维与基体的界面粘结强度（Ts）提高幅度可达535％,短梁剪切强度TNOL提高了40％以上．     

Selection of an in-plane shear test method based on the shear sensitivity of laminate tensile modulus

The sensitivity of the tensile modulus for a number of Hercules AS4/3501-6 laminates to changes in the values of in-plane shear modulus was used to select the fibre orientations for four highly shear-sensitive laminates of the form [±θ₁,±θ₂]_3s. The in-plane shear moduli for the Hercules AS4/3501-6 composite material were then determined for 90° Iosipescu, 10° off-axis tensile and ±45° tensile specimens. These values were used with classical laminate plate theory to predict laminate tensile moduli. The best agreement between these predicted values and those which were experimentally measured was obtained when the ± 45° tensile test method was used to determine the in-plane shear modulus.     

Experimental and numerical investigation of the interface between epoxy matrix and hemp yarn

In the present work, the adhesion between an impregnated hemp yarn and the epoxy matrix was investigated. The micromechanical tests usually used to characterise the fibre/matrix interface were adapted to the yarn/matrix interface. Single yarn composite specimens with yarn axis at 0° were manufactured and submitted to fragmentation tests to determine the experimental interfacial shear strength (IFSS). Specific single yarn composite specimens with yarn axis at 90° from the loading direction were also tested to track by digital image correlation the strain fields in the yarn, in the resin and at the yarn/matrix interface. A finite element analysis was developed and optimised to simulate the fragmentation process and provides a conservative value of IFSS.     

Interfacial shear stress in SiC fibre-reinforced cordierite

An analytical model based on a consistent shear-lag theory was developed to predict the interfacial shear stress in single fibre pull-out tests. The calculations show that the stress is highly dependent on the specimen thickness and the method of testing. Data for the debond stress and the interfacial shear stress were measured for single SiC fibres embedded in a magnesium aluminium silicate (cordierite) matrix. The effect of fibre embedded length, processing schedule, and matrix toughening were investigated. For a fixed sample support configuration during testing, good agreement was obtained between the model predictions and experimental data.     

The effect of heat treatment temperature on the interfacial shear strength of C/C composites

This paper investigates the effect of heat treatment temperature on the interfacial shear strength (IFSS) of carbon/carbon composites reinforced with polyacrylonitrile-based fibers. A series of single fiber push-out tests were performed on specimens heat treated at 1800, 2100, and 2400 °C, using a nanoindenter with a flat ended conical tip. The microstructure was characterized using polarized light and transmission electron microscopy and the debonded fiber/matrix interface was examined using scanning electron microscopy. Wavelet analysis of the load–displacement data was used as an additional tool to investigate the initiation and progression of debonding. Compared to 1800 °C, heat treatment at 2400 °C was associated with a decrease in IFSS, from 12 to 7 MPa. Transmission electron microscopy study showed that the microstructure of the fiber/matrix interphase remained amorphous even with heat treatment at 2400 °C. The decrease in the IFSS can be partly attributed to the reorganization of the graphene sheets in the matrix in the vicinity of fiber/matrix interphase. The thermal expansion mismatch between fiber and pyrocarbon matrix is another possible reason for the observed decrease in the IFSS.     

Effects of fibre volume fraction on the stress transfer in fibre pull-out tests

The elastic stress transfer taking place across the fibre/matrix interface is analysed for the fibre pull-out test by means of both micromechanics and finite element (FE) analyses. A special focus has been placed on how fibre volume fraction, V_f, affects the interface shear stress fields in the model composites containing both single and multiple fibres. In a so-called ‘three-cylinder model’, where a fibre, a matrix and a composite medium are coaxially located, the constraint imposed on the central fibre due to the surrounding fibres is properly evaluated. It is shown in the FE analysis that the differences in stress distributions between the composite models containing single and multiple fibres become increasingly prominent with increasing V_f. The principal effect of the presence of surrounding fibres in the multiple-fibre composite model is to suppress effectively the development of stress concentration near the embedded fibre end and thus eliminate the possibility of debond initiation from this region for all V_f considered. This is in sharp contrast to the single-fibre composite model, in which the interfacial debond can propagate from the embedded end if V_f is larger than a critical value. These findings are essentially consistent with the results from micromechanics analysis on the same specimen geometry. The implications of the results for the practical fibre pull-out test as a means of measuring the interface properties are discussed.     

Three techniques of interfacial bond strength estimation from direct observation of crack initiation and propagation in polymer–fibre systems

Three techniques of bond strength determination in micromechanical tests—fibre strain profile analysis by means of Raman spectroscopy, “kink” force determination in a traditional pull-out test, and crack length monitoring in a microbond test—were used for investigation of interfacial debonding in epoxy–glass fibre and epoxy–aramid fibre systems. Crack propagation was characterised by local interfacial parameters—critical energy release rate, G_ic, and ultimate interfacial shear strength (IFSS), τ_ult. The comparison of the results showed good agreement both between different techniques and between stress-based and energy-based failure criteria. Sizing of glass fibres caused more pronounced variations in the IFSS than for aramid fibres due to different interfacial failure patterns. The strength of “real” epoxy–glass composites with sized and unsized fibres correlates well with the bond strength determined from the micromechanical tests.