Effect of Autoclave Pressure On Interfacial Properties at Micro-And Macro - Level in Polymer-Matrix Composite Laminates
Effect of Autoclave Pressure On Interfacial Properties at Micro-And Macro - Level in Polymer-Matrix Composite Laminates
Effect of Autoclave Pressure On Interfacial Properties at Micro-And Macro - Level in Polymer-Matrix Composite Laminates
Abstract: Variable autoclave pressures were applied on polymer-matrix composite to evaluate the effects on interfacial shear
strength (IFSS) and interlaminar shear strength (ILSS) in [0]10 T800/X850 composite laminates. The characterizations of
microstructure of the laminates were obtained using optical digital microscope and scanning electron microscope. The IFSS
and ILSS were measured by fiber push-in and short beam three-point bending tests respectively. Results have shown that
there exists an optimum range of autoclave pressure. The delamination and voids are mainly located at the plies of laminates,
where the shapes of voids are changeable. The number and size of voids decrease as the pressure increases, while the
impregnation of resin on fibers is improved continuously, leading to an increase for the fiber volume fraction. The IFSS and
the ILSS are related with the pressure all in the polynomial increasing models. For void contents are above 1 %, the ILSS
increases progressively as the pressure increases. Conversely, when void contents are less than 1 %, the changes of ILSS are
negligible and the ILSS is insensitive to the voids. For T800/X850 composite, the autoclave pressure in the range of 0.4 MPa
to 0.6 MPa is recommended.
Keywords: Polymer composites, Autoclave pressure, Void content, Fiber volume fraction, Interfacial properties
1614
Pressure on Interfacial Properties of Composites Fibers and Polymers 2017, Vol.18, No.8 1615
as the increase of the pressure, and the mechanical properties composite panels cured at different autoclave pressure
can be increased by reducing the amount of voids. But the conditions using a precision diamond saw. The samples were
in-situ effect of autoclave pressure on the microscale fiber/ filled in an epoxy resin to facilitate the polishing. Surfaces
matrix interfacial properties is not considered, and its perpendicular to fibers were polished with a series of the
relationship with interlaminar shear failure is rarely mentioned. silicon carbide abrasive papers of 600, 1000, 1500 grit size,
A better understanding of these effect is crucial to optimize then finished with 1 µm diamond paste, followed by a
the autoclave pressure conditions in an autoclave process of ultrasonic cleaning. The distribution, the number and the
composites. Analysis of their failure mechanisms provides a size of the internal defects in composite laminates were
good basis for multiscale modelling. observed using the optical digital microscope (ODM, model:
In this paper, the fiber/matrix interface shear strength OLYMPUS DS×500, Japan). The spatial distribution and
(IFSS) and the interlaminar shear strength (ILSS) were volume fraction of fibers in the intraply treated by spray-
investigated by push-in and short-beam tests. The influence gold were analyzed using the scanning electron microscope
mechanism of autoclave pressure on microscopic defects (SEM, model: TESCAN MIRA3 LMU, Czech).
and structure state of composite were analyzed in detail using
optical digital and scanning electron microscopic techniques, Mechanical Testing
respectively. The quantitative evaluations of the relationship Interlaminar Shear Strength Test (ILSS)
between autoclave pressure, microscopic characteristics and To assess the effects of autoclave pressure on the
the interfacial properties were established. Moreover, the interlaminar interface properties of composite laminates, the
interfacial failure modes of composites under different interlaminar shear strength tests were selected according to
autoclave pressure were also discussed. Chinese standard JC/T 773-2010. Samples of 20 mm (length)×
10 mm (width), and the thickness was the full thickness of
Experimental cured laminates, were cut from the center of the composite
panels and tested using the three-point short-beam bending
Material method with a span ratio of 7:1, as is shown in Figure 1. Five
The experimental composite material under research was tests for each group of samples were performed under the
the T800/X850 carbon fiber reinforced epoxy prepreg stoke control at a constant speed of 1 mm/min using the
(purchased from Commercial Aircraft Co., Ltd., China). The CMT5105 tensile testing machine (produced by Sansi Taijie
Cytec’s CYCOM X850 is a solvent-free epoxy resin which Co., Ltd., China). The interlaminar shear strength (ILSS,
has been added the thermo-plastic particles to enhance the MPa) of the composite samples was determined according to
fracture toughness and impact properties, applied to the equation (1),
aviation fiber prepreg manufacturing. The carbon reinforcement
3 Pmax-
used in the prepreg is a high strength carbon fiber of T800 τILSS = --- × --------- (1)
4 bh
with a fiber diameter around 5.1 µm. The initial resin
content of 35 % and the 190 g/m2 prepreg areal density were where Pmax is the maximum load (N), b is the sample width
all offered by the manufacturer. (mm) and h is the sample thickness (mm). The fracture
modes of samples after ILSS tests were examined by optical
Fabrication of Unidirectional Composite Laminates digital microscope (OLYMPUS DS×500, Japan) to analyze
In order to investigate the effect of autoclave pressure on the main fracture mechanism.
microscopic structures and interfacial properties of the Interfacial Shear Strength Test (IFSS)
composites. Four unidirectional composite laminates were In order to understand the effects of autoclave pressure on
fabricated by different kinds of the external pressure in the fiber/matrix interface properties of composite, fiber
autoclave process. The pressures were set as 0.0 MPa, 0.2 MPa, push-in tests were conducted by a triboindenter instrument
0.4 MPa and 0.6 MPa respectively. Under a given temperature (model: Hysitron TI 950, US) with a diamond flat punch of
cycles, the laminates were heated to the 180 oC at the rate of 5 µm in diameter. Micromechanical tests were performed
1.5 oC/min, and then were held for 150 min. Finally it was under displacement control at the 40 nm/s with the
cooled down to room temperature by means of air cooling. maximum displacement of 1200 nm and then unloading was
Each kind of pressure was controlled precisely by the preset conducted to the original position. The schematic and the
program of the autoclave system, and began to boost when experimental setup for the push-in test are shown in Figure
the temperature was reached to 30 oC. The dimension of the 2. The sample was inspected under the optical microscopy to
cured square panels was 100 mm×100 mm, and the final find the position of typical fiber packing patterns. Afterwards,
thickness of these panels was approximately 2.0±0.2 mm. the sample was moved beneath the low-load with maximum
load of 120 mN indenter probe. The in-situ images are
Microstructure Observation obtained by raster scanning the low-load indenter probe over
Samples of 10×10 mm2 were cut from each piece of the sample surface to allow for precise test placement and
1616 Fibers and Polymers 2017, Vol.18, No.8 Tengfei Chang et al.
Figure 1. (a) Schematic diagram of the three point bending method and (b) experimental setup with the ILSS test.
Figure 2. (a) Schematic of the fiber push-in test [12] and (b) experimental setup with the Hysitron TI950 Triboindenter.
Figure 3. (a) Optical micrograph of composite cross-section and (b) in-situ imaging showing the detail of one hexagonal packing before and
after fiber push-in tests.
microstructure identification. Afterwards, the sample was by its six nearest neighbors, as is show in Figure 3. The
tested under the high load indenter probe with maximum interfacial shear strength (IFSS, MPa) was determined
load of 950 mN to obtain the critical load Pc at the onset of according to equation (2) based on the shear-lag model [11,12],
interface failure. nP
For experimental comparison, samples with size of τIFSS = ----------c-2 (2)
10 mm×10 mm×2 mm were embedded into epoxy resin to 2πr
conduct the IFSS tests. Over 15 fibers per sample groups where Pc is the critical load at the onset of interface failure
were tested and these fibers were performed with a typical (mN), r is the fiber diameter (µm), and n is a parameter that
hexagonal packing pattern formed by one fiber surrounded depends on the fiber/matrix elastic properties and the
Pressure on Interfacial Properties of Composites Fibers and Polymers 2017, Vol.18, No.8 1617
and the equation was as follows, specimens was enhanced obviously. When the autoclave
pressure increased from 0 MPa to 0.2 MPa, the measured
σ
Presin = Pvoid – -------- (5) value of ILSS increased from 58.65 MPa to 86.75 MPa and
Mlv
the ILSS increased by up to 47.91 %. From Figure 7, the
where Presin is the pressure of resin, Pvoid is the internal ILSS values still increased significantly as the value of
pressure of bubbles, σ is the surface tension between resin autoclave pressure increased from 0.2 MPa to 0.4 MPa. But
fluid and bubbles, Mlv is the bubble ratio of volume to compared with the growth range of the autoclave pressure
surface area. Equation (5) demonstrated that the internal increased from 0 MPa to 0.2 MPa, the ILSS was grow
pressure of bubbles was related to the resin pressure. And slowly. In which the value of ILSS increased from 86.75 MPa
the higher of the autoclave pressure, firstly, it would enforce to 96.51 MPa and the ILSS increased by 11.25 %. However,
the resin to withstand the pressure greater and the internal when the autoclave pressure was higher than 0.4 MPa or
bubbles were dissolved more in the resin, resulting in the more, the difference of the ILSS were not significant. And
voids decreased further; secondly, the pressure difference of the values of ILSS increased from 96.51 MPa to 98.15 MPa
resin was greater that accelerated the excess resin to compact with the autoclave pressure increased from 0.4 MPa to
out of the composites under low void content, and led the 0.6 MPa, while the value of their growth range was only
compactness degree of fibers closely more. Therefore, in 1.69 %. It can be seen in Figure 7, the corresponding fitted
term of the experimental composite, a good interface quality curve for the trend of the ILSS with the aotuclave pressure
and lower void content can be obtained within the autoclave had shown the relationship between the autoclave pressure
pressure range of 0.4-0.6 MPa. and the ILSS was basically in line with the polynomial
increasing relationship, which was inversely proportional to
Interfacial Properties Analysis the relationship between the autoclave pressure and the void
Interlaminar Shear Strength Analysis content (as shown in Figure 5).
It has been pointed out in the previously literature that the To further investigate the influence mechanism of autoclave
void leads to the marked reduction in composite mechanical pressure on the ILSS of the specimens, the ODM micrographs
properties, especially those dominated by the resin failure of the interlaminar failure modes under different autoclave
behavior like the interlaminar shear strength [15,16]. Thus, pressures were shown in Figure 8. As can be seen from it,
the autoclave pressure should produce the better mechanical the failure cracks of the tested specimens distributed mainly
properties by reducing the voids of composites and the in the interlayer, and extended along the void direction when
hypothesis was tested by evaluating the ILSS of the laminates the range of the autoclave pressure was from 0 MPa to
cured under different autoclave pressure. The corresponding 0.2 MPa. Reasons resulting in such phenomena may be
measured values of ILSS with the different autoclave pressure affected by the numbers and sizes of voids between the plies.
were shown in Figure 7, and the lowest value of ILSS was Because when the bending load was applied on the specimens,
58.65 MPa with the autoclave pressure of 0 MPa. As the the stress concentration often occurred in the voids easily,
increasing of the autoclave pressure, the ILSS of the especially in the big void region. Therefore, the crack began
to develop from the big voids and then extended between the
piles, which illustrating the void could affect the initial stage
and evolutional stage of the ILSS failure. However, when
the autoclave pressure reached to 0.4 MPa or more, the crack
appeared in the intralayer of laminates and there were no
difference about the failure modes of ILSS. This is due to the
void content was less than 1 % under conditions of the
higher autoclave pressure (exceed 0.4 MPa), the numbers
and sizes of the voids were negligible and the interlaminar
interfaces between the piles were bonded closely. In these
circumstances, the voids were no longer the main cause for
the failure of ILSS and the crack was concentrated in the
interfacial layer between the fibers and the resin. ILSS with
autoclave pressure over 0.4 MPa are almost constant.
Therefore, with pressure over 0.4 MPa, it would help to
eliminate the voids of composites, and obtain higher values
of ILSS.
Interfacial Shear Strength Analysis
Figure 7. Relationship between interlaminar shear strength and The interfacial shear strength measured by push-in test can
autoclave pressure. be used to characterize the bonding strength of the fiber-
1620 Fibers and Polymers 2017, Vol.18, No.8 Tengfei Chang et al.
Figure 8. The ODM micrographs of the fracture modes of specimens tested to measure the ILSS; (a) 0.0 MPa, (b) 0.2 MPa, (c) 0.4 MPa, and
(d) 0.6 MPa.
Figure 9. (a) Load-indentation depth curves vs. autoclave pressure and (b) schematic diagram of critical load calculation.
matrix interface at the microscopic scale level, which is was followed by a linear region (with slope S0) after the full
affected by different fiber packing density and polymer contact due to the elastic deformation of the fiber and the
morphology cross-link density [17]. Figure 9(a) showed the matrix; And thirdly, with the increase of the indenter load,
typical load-depth curves of single fiber debonding process the non-linear region between loading and fiber displacement
obtained by push-in tests for different autoclave pressure. As was followed which illustrated the onset of fiber debonding
can be seen from it, these curves presented an S shape failure. All of these curves presented the same initial elastic
similarly. Firstly, there was initially an imperfect contact stiffness, shown in Figure 9(a), but the non-linear regions
process between the indenter and the fiber; Secondly, this followed were different. The difference demonstrated that
Pressure on Interfacial Properties of Composites Fibers and Polymers 2017, Vol.18, No.8 1621
the critical load, which enforced the failure of the fiber- Figure 11 showed the in-situ scanning images of the fiber
matrix interface, increased with the increasing of the indentation produced by push-in tests for each sample under
autoclave pressure. The determination of the critical load different autoclave pressures. Figure 11(a) showed that the
was based on the shear-lag model [12]. In which, two fiber indentation was shallowest under the autoclave pressure
parallel lines with the initial stiffness S0 as the slope were of 0 MPa, indicating the fiber loaded had the largest amount
drawn with offset displacement of 2 % and 10 %, shown in of rebound. This meant that the impregnation of resin on the
Figure 9(b), then two points intersected between the two fibers was poor and the adhesion between the fiber and the
parallel lines and the load-depth curve were formed a line, matrix was very weak, which lead to the most non-obvious
and last the point regarded as the critical load was identified fiber indentation and the weakening of the IFSS. Upon the
by the intersection of the line and the curve. Therefore, the application of autoclave pressure, the external pressure were
values of IFSS with different autoclave pressure can be loaded along the thickness direction of the laminates and
calculated from the experimental results of Figure 9(a) and forced most of the internal resin to infiltrate the fibers
equation (2). continuously. Figure 11(b) showed the typical fiber indentation
The results of IFSS of the specimens under different with the autoclave pressure of 0.2 MPa, which meant the
autoclave pressure were shown in Figure 10, clearly indicating infiltration of the resin on the fibers had been improved and
the value of IFSS increases with the increase of the autoclave the fiber volume fraction in the intraply was increased,
pressure. As is shown in Figure 10, the IFSS was the lowest leading to the better of the IFSS. But there were still parts of
with the autoclave pressure of 0 MPa and its value was voids due to the inadequate pressure. When the autoclave
56.38 MPa. As the autoclave pressure increased from 0 MPa pressure reached to 0.4 MPa, the internal voids of composites
to 0.2 MPa, the IFSS increased significantly, their values were almost eliminated and the compactness degree of fibers
increased from 56.38 MPa up to 66.72 MPa and the IFSS was more uniform (as shown in Figure 4(b)). This confirmed
increased by 18.34 %. When the autoclave pressure increased that the high pressure which drove the resin flow to
from 0.2 MPa to 0.4 MPa, the value of IFSS increased from impregnate the fiber would bring a good bonding of fiber-
66.72 MPa to 69.39 MPa and the IFSS increased only by matrix interface and the improvement of the IFSS. Therefore,
4.00 %. But with the increasing of the autoclave pressure, the fiber indentation was obvious as well (Figure 11(c)).
the rising trend of IFSS increased rapidly. Compared the As the autoclave pressure increased to 0.6 MPa, shown in
IFSS with the autoclave pressure of 0.4 MPa, the value Figure 11(d), the fiber indentation was the deepest. This
increased to 76.89 MPa as the autoclave pressure reached to indicated that the fibers were impregnated completely by the
0.6 MPa and the IFSS increased by 10.81 %. In order to resin and the fiber-matrix bonding interface had been
show the trend of the IFSS with the autoclave pressure, the
fitted curve had been existed in the Figure 10. It can be seen
from Figure 10, the relationship between the autoclave
pressure and the IFSS was in good agreement with that of
the polynomial increasing model, which was consistent with
the effect of autoclave pressure on the fiber volume fraction.
improved further. But the higher autoclave pressure may However, if the magnitude of pressure exceeds the
also force the excess resin flowed so fast to exclude out of standard cure pressure, it leads to excess resin flowing out of
the laminates, and the compactness degree of fibers was composite and potential lean glue defects. For T800/X850
oversized. In which, the possibility of forming the lean composite, the autoclave pressure in the range of 0.4 MPa to
defects in local region would increase and the IFSS 0.6 MPa was recommended.
increased sharply. Therefore, for fabricating the high-quality
composite components, the autoclave pressure which is in Acknowledgements
the range of 0.4 MPa to 0.6 MPa is recommended. But too
much pressure may produce the new defects in some local The authors would like to gratefully acknowledges the
areas of components, such as lean defect, which should not funding from the National Key Basic Research Program of
be also ignored. China (973 program) under Grant No. 2014CB46502, Project
of Innovation-driven Plan in Central South University,
Conclusion 2015CX002 and State Key Laboratory of High-performance
Complex Manufacturing under Grant No. ZZYJKT2016-04.
Unidirectional laminates of a T800/X850 polymer matrix The authors would like to gratefully acknowledge the
composite were manufactured using variable autoclave composite research team members of Central South University
pressures. The influence of autoclave pressure on the micro- for their support and useful discussions in this research.
and macro- interfacial properties was assessed. Firstly, a
better characterization of the internal defects and the References
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