Evaluation of interlaminar-toughened poly(etherlmide)-modified epoxy/carbon fiber composites

Amorphous poly(ether imide) has been used as interlaminar toughening particulate agent in laminated carbon fiber/epoxy composites. Mode I and Mode II delamination fracture toughness was characterized using the double cantilever beam (DCB) and end-notched flexure (ENF) specimens. The delamination surface was examined using a scanning electron microscopy (SEM) to investigate relationships between the morphology and properties. The results revealed that the PEI-modified composites exhibited a significantly increased fracture toughness, which increased with the PEI content. G_IC was improved from 165 to 540 J/m² (at 1 mm/min crosshead speed). G_IIC was improved more significantly from 290 to 1300 J/m². It is believed that these values could be further improved if the processing cycle were to be optimized.     

Effect of physical aging on the toughness of carbon fiber-reinforced poly(ether ether ketone) and poly(phenylene sulfide) composites. I

The effect of physical aging on the penetration impact toughness and Mode I interlaminar fracture toughness of continuous carbon fiber (C.F.) reinforced poly(ether ether ketone) (PEEK) and poly(phenylene sulfide) (PPS) composites has been investigated by using an instrumented falling weight impact (IFWI) technique and a double cantilever beam (DCB) test. Composite materials studied are aged below their glass transition temperature (T_g) at various periods. Initiation force and energy of damage, failure propagation energy, impact energy and ductility index (D.I.) are reported. The Mode I critical value of strain energy release rate (G_IC) of the unidirectional carbon fiber-reinforced PEEK (APC-2) composites is obtained. Results show that aging has a significant effect on the toughness of both composite materials. Energy absorbed during impact decreases with the increase of aging temperature and period. The PEEK/C.F. composites exhibit a higher retention of impact toughness than that of the PPS/C.F. composites after aging; however, the PPS/C.F. composites show a much higher ductility index. The Mode I fracture mechanism of the APC-2 composite is a combination of stable and unstable failure and shows a “stick-slip” behavior. Owing to the formation of a relative rigid structure, the fracture toughness (G_IC) of APC-2 decreased with the increase of aging temperature and period.     

Mode I and Mode II delamination resistance and mechanical properties of woven glass/epoxy–PU IPN composites

The effect of polyurethane on the mechanical properties and Mode I and Mode II interlaminar fracture toughness of glass/epoxy composites were studied. Polyurethanes (PU) synthesized using polyols and toluene diisocyanate were employed as modifier for epoxy resin by forming interpenetrating polymer network. The PU/Epoxy IPN was used as matrix material for GFRP. PU modified epoxy composite laminates having varying PU contents were prepared. The effect of PU content on the mechanical properties like interlaminar fracture toughness (Mode I, G_1c and Mode II, G_IIc), tensile strength, flexural strength, and Izod impact strength were studied. The morphological studies were conducted on the fractured surface of the composite specimen by scanning electron microscopy (SEM). Tensile strength, flexural strength, and impact strength of PU‐modified epoxy composite laminates were found to increase inline with interlaminar fracture toughness (G_1c and G_IIc) with increasing PU content to a certain limit and then it was found to decrease with increase in PU content. It was observed that toughening of epoxy with PU increases the Mode I and Mode II delamination toughness up to 17 and 120% higher than that of untoughened composite specimen, respectively. POLYM. COMPOS., 2008. © 2008 Society of Plastics Engineers     

Rubber modification of low temperature cure cyanate ester matrices and the performance in glass fabric composites

Low temperature cure cyanate ester resin systems were developed and modified with epoxy‐terminated butadiene acrylonitrile rubber (ETBN) and impregnated into woven glass fabric. Mode I and mode II interlaminar fracture toughness values of the cured laminates were evaluated as a function of rubber concentration. Mode I fracture toughness increased to almost twice that of the unmodified system, while mode II fracture toughness remained essentially unchanged. Composite samples were subjected to aging experiments in water and the absorption/desorption behavior was investigated as was the effect on thermal performance. The presence of rubber was found to reduce the rate of matrix deterioration but also caused a substantial increase in water uptake. It was found that although the addition of rubber to the matrices decreased the unconditioned (dry) T_g all specimens showed the same reduction in T_g, after equilibrium water absorption.     

Effect of graphene oxide on the interlaminar fracture toughness of carbon fiber/epoxy composites

Graphene oxide (GO) nanoparticles were introduced in the interlaminar region of carbon fiber–epoxy composites by dispersing it in a thermoplastic polymer carrier such as polyvinylpyrrolidone (PVP). Mode‐I fracture toughness (G_IC) was investigated using double cantilever beam testing to evaluate the effect of the GO on the delamination behavior of the composite. The GO content was varied from 0% to 7% by weight as a function of the PVP content. Improvement of ～100% in the Mode I fracture toughness (G_IC) was observed compared to composites with no GO. The optimum amount of nanoparticles for improving the interlaminar fracture toughness was found to be ～0.007% by weight of the composite. The increase in the value of flexural strength value was also observed. Scanning electron microscopy of fracture surfaces, X‐ray diffraction, and transmission electron microscopy, and reflectance Fourier transform infrared spectra, as well as Raman spectroscopy results, are presented to support the conclusions. POLYM. ENG. SCI., 59:1199–1208 2019. © 2019 Society of Plastics Engineers     

Temperature and Loading Rate Effects on the Fracture Behaviour of Adhesively Bonded GFRP Nylon-6,6

The combined effect of varying test temperature and loading rate on the Mode II fracture toughness of plasma-treated GFRP Nylon-6,6 composites bonded using a silica-reinforced epoxy adhesive has been studied. End notch flexure tests have shown that the adhesive system used in this study offers a wide range of fracture energies that are extremely sensitive to changes in temperature and loading rate. Increasing the test temperature resulted in a substantial reduction in the Mode II fracture toughness of the adhesive, with the value of G_IIc at 60°C being approximately one-half of the room temperature value. In contrast, increasing the crosshead displacement rate at a given temperature has been shown to increase the value of G_IIc by up to 250%. Compression tests performed on bulk adhesive specimens revealed similar trends in the value of [sgrave]_y with temperature and loading rate. In addition, it was found that the plasma treatment employed in this study resulted in stable crack propagation through the adhesive layer under all testing conditions.

A more detailed understanding of the effect of varying temperature and loading rate on the failure mechanisms occurring at the crack tip was achieved using the double end notch flexure (DENF) geometry, which was considered in tandem with the fracture surface morphologies. Here, changes in the degree of matrix shear yielding and particle-matrix debonding were used to explain the trends in [sgrave]_y and G_IIc.     

Tetraglycidyl epoxy resins and graphite fiber composites cured with flexibilized aromatic diamines

Studies were performed to synthesize new ether modified, flexibilized aromatic diamine hardeners for curing epoxy resins. The effect of moisture absorption on the glass transition temperatures of a tetraglycidyl epoxy, MY 720, cured with flexibilized hardeners and a conventional aromatic diamine was studied. Unidirectional composites, using epoxy-sized Celion 6000 graphite fiber as the reinforcement, were fabricated. The room temperature and 300°F mechanical properties of the composites, before and after moisture exposure, were determined. The Mode I interlaminar fracture toughness of the composites was characterized, using a double cantilever beam technique to calculate the critical strain energy release rate, G_IC.     

Mechanical Behavior and Fracture Toughness of Poly(L‐lactic acid)‐Natural Fiber Composites Modified with Hyperbranched Polymers

Summary: The use of hyperbranched polymers (HBP) with hydroxy functionality as modifiers for poly(L ‐lactic acid) (PLLA)‐flax fiber composites is presented. HBP concentrations were varied from 0 to 50% v/v and the static and dynamic tensile properties were investigated along with interlaminar fracture toughness. Upon addition of HBP, the tensile modulus and dynamic storage modulus (E′) both diminished, although a greater decline was noticed in the static modulus. The elongation of the composites with HBP showed a pronounced increase as large as 314% at 50% v/v HBP. The loss factor (tan δ) indicated a lowering of the glass transition temperature (T_g) due to a change in crystal morphology from large, mixed perfection spherulites to finer, smaller spherulites. The change in T_g could have also resulted from some of the HBP being miscible in the amorphous phase, which caused a plasticizing effect of the PLLA. The interlaminar fracture toughness measured as the critical strain energy release rate (G_IC) was significantly influenced by HBP. At 10% v/v HBP, G_IC was at least double that of the unmodified composite and a rise as great as 250% was achieved with 50% v/v. The main factor contributing to high fracture toughness in this study was better wetting of the fibers by the matrix when the HBP was present. With improved ductility of the matrix, it caused ductile tearing along the fiber‐matrix interface during crack propagation.

ESEM photograph of propagation region of the interlaminar fracture toughness specimens with 30% v/v of HBP.     

The effect of silicon carbide whiskers on the Mode I interlaminar fracture of carbon fiber composites

This paper reports on the Mode I interlaminar fracture toughness improvement of carbon fiber-epoxy composites as a result of incorporating SiC whiskers in the epoxy matrix. Five laminates of unidirectional carbon fiber-epoxy composites at different weight fractions of SiC whiskers were manufactured using hand layup vacuum bagging process. Optical and scanning electron microscopic analysis were conducted to give an insight into the fracture morphogoloy, failure mechanisms, and the energy dissipation mechanisms created by the presence of the whiskers in the composite. Experimental results showed that composites containing 5 wt% whiskers exhibited 67% increase in the crack initiation interlaminar fracture toughness G_IC, whereas it exhibited 55% increase in the maximum G_IC compared to pristine composite. The optical and SEM fractographs revealed a strong relation between the microstructure of the fractured surfaces and the energy release rate trend of the composites.     

Thermal Properties,Fracture Toughness and Water Absorption of Epoxy-Palm Oil Blends

Epoxidized palm oil (EPO) was blended with cycloaliphatic epoxide, epoxy novolac and diglycidyl ethers of bisphenol-A. The fracture toughness and thermal properties of epoxy/EPO blends were characterized using single-edge notched bending tests and differential scanning calorimetry. Increased EPO loading improved the fracture toughness (K _IC ) of the epoxy blends. The epoxy blends with higher EPO loading exhibited higher degree of conversion. The glass transition temperature (T _g ) of the epoxy blends shifted to higher temperature as the increasing of DSC heating rate. Water absorption caused T _g reduction of epoxy blends but it was determined that the water molecules absorbed were totally reversible.     

Synthesis and characterization of fluorinated poly(etherimide)s toughening for carbon fiber‐reinforced epoxy composites

Novel‐fluorinated poly(etherimide)s (FPEIs) with controlled molecular weights were synthesized and characterized, which were used to toughen epoxy resins (EP/FPEI) and carbon fiber‐reinforced epoxy composites (CF/EP/FPEI). Experimental results indicated that the FPEIs possessed outstanding solubility, thermal, and mechanical properties. The thermally cured EP/FPEI resin showed obviously improved toughness with impact strength of 21.1 kJ/m² and elongation at break of 4.6%, respectively. The EP/FPEI resin also showed outstanding mechanical strength with tensile strength of 91.5 MPa and flexural strength of 141.5 MPa, respectively. The mechanical moduli and thermal property of epoxy resins were not affected by blending with FPEIs. Furthermore, CF/EP/FPEI composite exhibited significantly improved toughness with Mode I interlaminar fracture toughness (G_IC) of 899.4 J/m² and Mode II interlaminar fracture toughness (G_IIC) of 1017.8 J/m², respectively. Flexural properties and interlaminar shear strength of the composite were slightly increased after toughening. POLYM. COMPOS., 2010. © 2009 Society of Plastics Engineers     

Impact fracture behavior of continuous glass fiber-reinforced nylon 6

The impact fracture toughness of nylon 6/continuous glass fiber composites at four levels of fiber content has been studied. The composites were produced by anionically polymerizing caprolactam within a glass mat using a vacuum injection technique. Application of linear elastic fracture mechanics to characterize the impact fracture toughness of the composites, using an energy approach (G_IC), has been found to be applicable provided that a correction is made for the size of the damage zone. The concept of J_c, fracture energy per unit ligament area, has also been applied to the composites and agreement between G_IC and J_c has been found to be reasonably satisfactory. The ratio of crack propagation energy to the total energy absorbed (ductility index) has also been calculated. The ductility index was found to be close to one for the composites, indicating that additional energy is involved in propagating the fracturing cracks probably due to fiber debonding and/or crack blunting and fiber pullout. Fractographic examination of the impact fracture surface confirmed the presence of these features.     

Effect of silica nanoparticle size on toughening mechanisms of filled epoxy

The addition of silica nanoparticles (23 nm, 74 nm, and 170 nm) to a lightly crosslinked, model epoxy resin, was studied. The effect of silica nanoparticle content and particle size on glass transition temperature (T_g), coefficient of thermal expansion (CTE), Young's modulus (E), yield stress (σ), fracture energy (G_IC) and fracture toughness (K_IC), were investigated. The toughening mechanisms were determined using scanning electron microscopy (SEM), transmission electron microscopy (TEM) and transmission optical microscopy (TOM). The experimental results revealed that the addition of silica nanoparticles did not have a significant effect on T_g or the yield stress of epoxy resin, i.e. the yield stress and T_g remained constant regardless of silica nanoparticle size. As expected, the addition of silica nanoparticles had a significant impact on CTE, modulus and fracture toughness. The CTE values of nanosilica-filled epoxies were found to decrease with increasing silica nanoparticle content, which can be attributed to the much lower CTE of the silica nanoparticles. Interestingly, the decreases in CTE showed strong particle size dependence. The Young's modulus was also found to significantly improve with addition of silica nanoparticles and increase with increasing filler content. However, the particle size did not exhibit any effect on the Young's modulus. Finally, the fracture toughness and fracture energy showed significant improvements with the addition of silica nanoparticles, and increased with increasing filler content. The effect of particle size on fracture toughness was negligible. Observation of the fracture surfaces using SEM and TOM showed evidence of debonding of silica nanoparticles, matrix void growth, and matrix shear banding, which are credited for the increases in toughness for nanosilica-filled epoxy systems. Shear banding mechanism was the dominant mechanism while the particle debonding and plastic void growth were the minor mechanisms.     

Effect of cooling rate and crack propagation direction on the mode 1 interlaminar fracture toughness of biaxial noncrimp warp‐knitted fabric composites made of glass/PP commingled yarn

The mode 1 interlaminar fracture toughness of biaxial (±45°) noncrimp warp‐knitted fabric composites made of glass/PP commingled yarn was investigated. The crack propagation along the warp and weft directions, respectively, was considered for the composites cooled at two different rates during laminate molding. The interlaminar fracture toughness was characterized by determining the critical strain energy release rate (G_IC) of initiation and propagation measured from the double cantilever beam tests. In the case of a slow cooling rate (1°C/min), most specimens possess pure interlaminar crack propagation and direction‐independence characteristics. Nevertheless, the high‐cooled (10°C/min) specimens fractured in both directions suffer extensive intraply damage (crack branching, debonding, and bridging of 45°‐oriented interfacial yarns) and knit thread breakage, leading to G_IC of propagation two times higher than that of the slow‐cooled specimens, and the clear difference in the G_IC values of initiation between the two directions may be due to the contribution of the knit thread breakage to the fracture energy. POLYM. COMPOS., 2008 © 2007 Society of Plastics Engineers     

PET interleaving veils for improved fracture toughness of glass fibre/low‐styrene‐emission unsaturated polyester resin composites

The use of interleaved polyethylene terephthalate (PET) veils to increase the interlaminar fracture toughness of glass fiber‐reinforced, low‐styrene emission, unsaturated polyester resin composites, was investigated. PET, being chemically similar to the unsaturated polyester resin, was expected to exhibit good wetting and strong interaction with the matrix. Composite laminates were manufactured by hand lay‐up, with the veil content varying up to 7%. The effects of PET veils on the interlaminar shear strength, flexural strength, flexural modulus, glass transition temperature, damping parameters, and Mode‐I interlaminar fracture toughness of the composite were studied. The veils were found to enhance most of these properties, with only minor negative effects on flexural stiffness and T_g. The PET/resin bonding did indeed prove to be strong, but the enhancement of fracture toughness was not as much as expected, because of the weaker glass/resin interface providing an alternative crack propagation path. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 42877.     

Fracture toughness of silica particulate‐filled epoxy composite

The relationship between the postcuring conditions and fracture toughness on three silica particulate‐filled epoxy composites was investigated. The glass transition temperature, T_g, and the fragility parameter, m, derived from the thermo‐viscoelasticity, were used to characterize the composites, which were postcured under various conditions. The glass transition temperature and fragility both depended on both of the curing conditions and the volume fraction of silica particles. The glass transition temperature increased with the postcuring time and temperature, while the fragility generally decreased as the volume fraction increased. There was no direct correlation between the glass transition temperature and fragility. The fracture toughness depended on both the glass transition temperature and fragility. The composites with a high glass transition temperature and low fragility had high fracture toughness. These results indicate that the glass transition temperature and fragility are useful parameters for estimating the fracture toughness of the silica particulate‐filled epoxy composites. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 2261–2265, 2002     

Mechanical properties and fracture behaviors of epoxy composites with phase‐separation formed liquid rubber and preformed powdered rubber nanoparticles: A comparative study

Epoxy composites filled with phase‐separation formed submicron liquid rubber (LR) and preformed nanoscale powdered rubber (PR) particles were prepared at different filler loading levels. The effect of filler loading and type on the rheological properties of liquid epoxy resin suspensions and the thermal and mechanical properties of the cured composites as well as the relative fracture behaviors are systematically investigated. Almost unchanged tensile yield strength of the cured epoxy/PR composites is observed in the tensile test compared with that of the neat epoxy; while the strength of the cured epoxy/LR composites shows a maximum value at ∼4.5 wt% and significantly decreases with increasing LR content. The glass transition temperature (T_g) of the cured PR/epoxy has shifted to the higher temperature in the dynamic mechanical thermal analysis compared with that of the cured pure epoxy and epoxy/LR composites. Furthermore, the presence of LR results in highly improved critical stress intensity factor (K_IC) of epoxy resin compared with the corresponding PR nanoparticles. In particular, the PR and LR particles at 9.2 wt% loading produce about 69 and 118% improvement in K_IC of the epoxy composites, respectively. The fracture surface and damage zone analysis demonstrate that these two types of rubber particles induce different degrees of local plastic deformation of matrix initiated by their debonding/cavitation, which was also quantified and correlated with the fracture toughness of the two epoxy/rubber systems. POLYM. COMPOS., 36:785–799, 2015. © 2014 Society of Plastics Engineers     

“Ex situ” concept for toughening the RTMable BMI matrix composites,Part I: Improving the interlaminar fracture toughness

Aerospace‐grade bismaleimide matrix composites was toughened based on a novel ex situ resin transfer molding (RTM) technique using a special manufactured ES? carbon fabrics. The toughening mechanism and toughening effect by the technique are studied using thermoplastic PAEK as toughener. Mode I fracture toughness (G_IC) of the composites toughened by ex situ RTM technique increased up to three times higher than that of the control system, and Mode II fracture toughness (G_IIC) increased two times higher as well. The composite without toughening was denoted as control system. The microstructure revealed that a reaction‐induced phase decomposition and inversion happened in the interlaminar region, which resulted in a particles morphology that showed the thermosetting particles were surrounded with the PAEK phase. The plastic deformation and rupture of the continuous PAEK phase are responsible to the fracture toughness improvement. And the influence of PAEK concentration on toughness improvement was also investigated. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Toughening of epoxy hybrid nanocomposites modified with silica nanoparticles and epoxidized natural rubber

Silica nanoparticles (SN) and epoxidized natural rubber (ENR) were used as binary component fillers in toughening diglycidyl ether of bisphenol A (DGEBA) cured cycloaliphatic polyamine. For a single component filler system, the addition of ENR resulted in significantly improved fracture toughness (K_IC) but reduction of glass transition temperature (T_g) and modulus of epoxy resins. On the other hand, the addition of SN resulted in a modest increase in toughness and T_g but significant improvement in modulus. Combining and balancing both fillers in hybrid ENR/SN/epoxy systems exhibited improvements in the Young’s modulus and T_g, and most importantly the K_IC, which can be explained by synergistic impact from the inherent characteristics associated with each filler. The highest K_IC was achieved with addition of small amounts of SN (5 wt.%) to the epoxy containing 5–7.5 wt.% ENR, where the K_IC was distinctly higher than with the epoxy containing ENR alone at the same total filler content. Evidence through scanning electron microscopy (SEM) and transmission optical microscopy (TOM) revealed that cavitation of rubber particles with matrix shear yielding and particle debonding with subsequent void growth of silica nanoparticles were the main toughening mechanisms for the toughness improvements for epoxy. The fracture toughness enhancement for hybrid nanocomposites involved an increase in damage zone size in epoxy matrix due to the presence of ENR and SN, which led to dissipating more energy near the crack-tip region.     

The influence of cooling rate on the fracture properties of a glass reiforced/nylon fiber-metal laminate

The effect of varying cooling rate on the microstructure and resulting mechanical properties of a novel fiber-metal laminate (FML) based on a glass fiber-reinforced nylon composite has been investigated. Polished thin sections removed from plain glass fiber/nylon composites and their corresponding fiber-metal laminates indicated that the prevailing microstructure was strongly dependent on the rate of cooling from the melt. Mode I and Mode II interlaminar fracture tests on the plain glass fiber reinforced nylon laminates indicated that the values of G_Ic and G_IIc averaged approximately 1100 J/m² and 3700 J/m² respectively at all cooling rates. The degree of adhesion between the aluminum alloy and composite substrates was investigated using the single cantilever beam geometry. Here, the measured values of G_c were similar in magnitude to the Mode I interlaminar fracture energy of the composite, tending to increase slightly with increasing cooling rate. The tensile and flexural fracture properties of the plain composites and the fiber metal laminates were found to increase by between 10% and 20% as the cooling rate was increased by two orders of magnitude. This effect was attributed to over-aging of the aluminum alloy plies at elevated temperature during cooling. Finally, fiber metal laminates based on glass fiber/nylon composites were shown to exhibit an excellent resistance to low velocity impact loading. Damage, in the form of delamination, fiber fracture, matrix cracking in the composite plies, and plastic deformation and fracture in the aluminum layer, was observed under localized impact loading. Here, the fast-cooled fiber metal laminates offered superior post-impact mechanical properties at low and intermediate impact energies, yet very similar results under high impact energies.