Reactive and Nonreactive Binders in Glass/Vinyl Ester 

Composites 

by John C. Brody and John W. Gillespie, Jr. 

ARL-CR-552 September 2004 

prepared by 

University of Delaware 

Center for Composite Materials 

Newark, DE 19716 

under contract 

DAAD19-01-2-0005 

Approved for public release; distribution is unlimited.
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Army Research Laboratory 

Aberdeen Proving Ground, MD 21005-5069 

ARL-CR-552 September 2004 

Reactive and Nonreactive Binders in Glass/Vinyl Ester 

Composites 

John C. Brody and John W. Gillespie, Jr. 

Center for Composite Materials 

University of Delaware 

prepared by 

University of Delaware 

Center for Composite Materials 

Newark, DE 19716 

under contract 

DAAD19-01-2-0005 

Approved for public release; distribution is unlimited. 
ii

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4. TITLE AND SUBTITLE 

Reactive and Nonreactive Binders in Glass/Vinyl Ester Composites 

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622618.AH80 

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6. AUTHOR(S) 

John C. Brody* and John W. Gillespie, Jr.* 

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Composite Manufacturing Science Laboratory 

University of Delaware 

Center for Composite Materials 

Newark, DE 19716 

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ARL-CR-552 

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U.S. Army Research Laboratory 

ATTN: AMSRD-ARL-WM-MB 

Aberdeen Proving Ground, MD 21005-5069 

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13. SUPPLEMENTARY NOTES 

*University of Delaware, Center for Composite Materials, Newark, DE 19716. 

14. ABSTRACT 

This study characterizes and evaluates two types of preform binders—reactive thermosets and nonreactive thermoplastics. The 

interply adhesion between woven glass plies was measured as a function of binder type, concentration, and preforming 

conditions. It was found that reactive binders offer the potential to provide much larger interply adhesions between glass plies 

in a preform than thermoplastics and are thus superior choices for the fabrication of complex-shaped preforms requiring little or 

no springback. Laminated composite panels fabricated from preforms with varying binder concentrations were evaluated in 

regards to their interlaminar properties. It was found that both binder types degraded the interlaminar shear strength of a woven 

glass reinforced/vinyl ester composite. Additionally, composite laminates made from preforms and containing the thermoplastic 

binder showed decreases in the interlaminar fracture toughness of the composite by ~60%. However, composite laminates 

fabricated from preforms using the reactive epoxy binder showed an increase in fracture toughness by ~47%. Hence, it is 

concluded that a range of interlaminar properties can be achieved depending on the type of binder, the amount of binder, and the 

processing of the binder, and also that of the composite itself. 

15. SUBJECT TERMS

binder, preform, adhesion, interlaminar properties 

16. SECURITY CLASSIFICATION OF: 

19a. NAME OF RESPONSIBLE PERSON

John C. Brody 

a. REPORT 

UNCLASSIFIED 

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OF ABSTRACT 

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OF PAGES 

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(302) 831-6644 

Standard Form 298 (Rev. 8/98) 

Prescribed by ANSI Std. Z39.18
iii

Contents 

List of Figures iv

List of Tables v

1. Introduction 1

2. Experimental 3

2.1 Materials..........................................................................................................................3 

2.2 Preform Construction ......................................................................................................4

2.3 Composite Fabrication ....................................................................................................5 

2.4 Preform Characterization ................................................................................................5 

2.5 Composite Performance ..................................................................................................6 

3. Results and Discussion 7

3.1 Preform Analysis.............................................................................................................7 

3.2 Interply Adhesion of Preforms (T-Peel Test)..................................................................8 

3.3 Void Content Determination .........................................................................................10 

3.4 Binder Effect on Interlaminar Shear Strength...............................................................14 

3.5 Binder Effect on Interlaminar Fracture Toughness.......................................................15 

4. Conclusion 18

5. References 20

Distribution List 22 
iv

List of Figures 

Figure 1. DSC thermogram of ATLAC 363E showing glass-transition temperature and 

melting temperature. ..................................................................................................................4 

Figure 2. DSC thermogram of PRETEX 110 showing glass-transition temperature and 

melting temperature. ..................................................................................................................4 

Figure 3. SEM image showing binder coverage of 3 weight-percent (a) and 9 weight-percent 

(b) ATLAC binder on woven glass mat processed at 80 °C......................................................7 

Figure 4. SEM image showing binder coverage of 3 weight-percent (a) and 9 weightpercent (b) PRETEX binder on woven glass mat processed at 110 °C. ....................................8 

Figure 5. SEM micrographs showing the limited tow impregnation (a) of ATLAC binder 

processed at 80 °C and (b) PRETEX binder processed at 110 °C.............................................8 

Figure 6. Load-vs.-displacement curve for T-Peel test of 3-in-wide specimen of E-glass with 

6 weight-percent of varying binder type....................................................................................9 

Figure 7. Peel strength vs. binder concentration for ATLAC and PRETEX binders on woven 

E-glass mats. ............................................................................................................................10 

Figure 8. Comparison of T-Peel test specimens bound by ATLAC and reacted PRETEX 

binder on 0°/90° woven E-glass...............................................................................................11

Figure 9. SEM micrograph of fiber mat surface of 6 weight-percent reacted PRETEX peel 

specimen at magnification of 75×............................................................................................11 

Figure 10. SEM micrographs of fiber mat surface of (a) 6 weight-percent ATLAC peel 

specimen at 200× and (b) 6 weight-percent reacted PRETEX peel specimen at 250×. ..........12 

Figure 11. SEM micrograph of woven glass fiber vinyl ester DERAKANE 411-C-50 

composite laminate with no binder at 55× magnification........................................................13 

Figure 12. SEM micrograph of interlaminar void within composite laminates with (a) 

9 weight-percent PRETEX binder and (b) 9 weight-percent ATLAC at 60×. ........................13 

Figure 13. Interlaminar shear strengths of composite laminates manufactured from woven 

glass preforms of varying binder type and concentration.......................................................14 

Figure 14. Load vs. displacement of composite DCB specimens.................................................15 

Figure 15. Delamination curve showing R-curve behavior for glass-reinforced DERAKANE 

411-C-50 vinyl ester composites with varying binder.............................................................16 

Figure 16. Mode I propagation fracture toughness of composite laminates with varying 

binder type and concentration..................................................................................................16 

Figure 17. SEM micrographs of fracture surface of DCB specimen of composite laminate 

containing 9 weight-percent ATLAC (a) 150× (b) 100×.........................................................17 

Figure 18. SEM micrographs of fracture surface of DCB specimen of composite laminate 

containing 9 weight-percent PRETEX at (a) 75× and (b) 50×. ...............................................18 
v

List of Tables 

Table 1. Results of T-Peel test for 0°/90° woven E-glass tackified with ATLAC 363E and 

PRETEX 110 binders.................................................................................................................9 

Table 2. Fiber volume fraction and void content of glass-reinforced vinyl ester composite 

laminates with varying binder concentrations. ........................................................................12 

Table 3. Interlaminar shear strengths of glass reinforced vinyl ester composite laminates 

with varying binder concentrations..........................................................................................14 

Table 4. Mode I initiation fracture toughness of composite laminates, GIC, with varying 

binder type and concentration..................................................................................................17 
vi

INTENTIONALLY LEFT BLANK.
1

1. Introduction 

Liquid composite molding processes such as vacuum-assisted resin transfer molding (VARTM), 

resin transfer molding (RTM), and the Seeman composite resin infusion molding process 

(SCRIMP) have been recognized as low-cost methods in manufacturing large-size composites in 

the marine, transportation, and civil infrastructure industries. Such manufacturing processes 

usually require the reinforcement material, typically two-dimensional (2-D) fabrics layers, to be 

hand laid into a mold cavity prior to processing. This often requires multiple layers of 

reinforcement mat to be cut to shape, stacked, and aligned to conform to various curvatures of 

the mold cavity (1). In order to reduce production time and cost, preshaped reinforcement, or 

preforms are often employed. Preforms typically consist of multiple layers of dry reinforcement 

mat, bound together into a single, three-dimensional (3-D), net-shaped structure. 

Additional benefits of using preforms include easy handling and mold placement of the 

reinforcement material, control of fiber alignment, prevention of unwanted wrinkling of layers, 

the ability to control part thickness to meet dimensional tolerances, and the ability to control the 

fiber volume fractions that will be present in the final cured composite itself. 

Preforms can be fabricated by complex weaving processes and/or stitching of individual 

reinforcement plies. Preforms may also consist of layers of reinforcement mats, which have 

been bound together by polymeric materials, most often referred to as binders or tackifiers. The 

most common types of binders are typically low-melting thermoplastic polyester, or either 

catalyzed, or uncatalyzed thermosetting epoxies that are solid at room temperature (2–4). 

Thermoplastic and uncatalyzed binders are typically designed to be soluble in the infusing 

matrix, whereas reactive (catalyzed) binders are often designed to react and be compatible with 

the matrix resin. 

Binders can be applied to the reinforcement fabric surface in various methods. Common 

application methods use veils, solvent spray, and powder. Veils are placed between adjacent 

plies of reinforcement material, and ply stacks are fused together into a preform upon application 

of heat and pressure (2). In the case of spray application, the solid binder is dissolved into a 

solvent, commonly acetone, and applied by a spray gun to the fabric surface. Some researchers 

have found that this method of application provides for a more uniform coverage of the binder 

material (5); however, this is often times not feasible due to inherent health hazards and 

additional requirement for solvent removal. 

Another commonly used tackifier application approach is to use powders. Powdered preform 

binders are required to be distributed uniformly onto the surface of the fiber mat in order to 

ensure sufficient adhesion throughout the preform. Typical binder loadings range from 4% to 

7% of the weight of the reinforcement (2, 4, 6). After the binder is applied to the fiber mat 
2

surface, sufficient heat is next applied to the mat in order to melt the binder material. This is 

usually done with the use of infrared lamps or ovens. Then upon cooling, the binder resolidifies, 

adhering to the fiber mat surface. 

Preforms are then constructed from individual plies of binder-coated mats by any typical 

thermoforming process involving heat and pressure. The individual plies are stacked, aligned, 

and placed within a mold cavity. Pressure is typically applied by a mechanical press, or by a 

vacuum bag assembly. Again, adequate heat is applied to melt the binder, and react the binder in 

the case of reactive thermosetting binders. Heat is often applied via a heated tool or the mold 

being placed in an oven or autoclave. Once the binder is allowed to melt on the surface of the 

fiber mats, the assembly is allowed to cool while a constant pressure is maintained. Upon 

cooling, the binder resolidifies, and the individual plies are fused into a single, net-shaped 

preform. 

The use of preform binders introduces significant issues requiring attention, including 

springback, shape retention, permeability and wet-out of the preform; binder dissolution and 

migration; and affects on the matrix resin and overall performance of the composite. 

A few studies have addressed the effect of preform processing and binder type on the shape 

retention of preforms. Studies conclude that preform springback is dependent upon the binder 

modulus, ply surface area coverage, extent of binder reaction, and binder location (interply vs. 

intraply). Accordingly, higher binder modulus, surface coverage areas, and reactivity conversion 

all result in less springback (2, 4, 7). Additionally, the binder location has shown to affect both 

springback and interply adhesion. Studies have shown that both type of binder application 

(spray vs. powder) and performing conditions can influence whether the binder will penetrate 

within fiber tows or remain on the layer surface (2, 7, 8). Results from these studies indicate that 

preforms with binder inside fiber tows offer far less springback, whereas those with binder that 

remains outside fiber tows and solely on fiber mat surface offer superior interply adhesion. 

Another significant issue is the effect binder materials impart on the permeability and fiber 

wet-out. Studies indicate that permeability is affected more by the blockage of the larger gaps 

between the fiber tows (interlayer) as compared to the blockage of the smaller interstitial gaps 

within the tows (intralayer) (4, 7, 9). For preforms in which the tackifier remains outside the 

fiber tows, the permeability decreased as the tackifier concentration increased (4, 7). In contrast, 

for fabrics preformed at higher temperatures, in which the binder infiltrates within the fiber tows, 

the preform permeability increased as the binder concentration increased (7). However, in the 

case where binder is predominantly within the fiber tow, results indicate poor wet-out, and 

formation of voids within the tows (4). 

Additionally, it has been shown that binder dissolution can cause drastic increases in resin 

viscosity, and thus hinder mold filling as well (3, 9). Furthermore, uneven dissolution and binder 

migration can result in varying binder concentrations across the cured composite laminate (2, 3), 
3

which may result in uneven shrinkage and a distribution of reaction rates, mechanical properties, 

and thermal stresses within the composite part. 

Additional studies have shown that preform binders can have a drastic effect on the 

thermophysical and mechanical properties of the matrix resin and overall composite laminate. 

Studies have shown binder material may alter resin fracture toughness, tensile strength and 

strain, impact energy, and glass transition temperatures (2, 9–11). 

Additionally, the use of incompatible binders has been shown to have detrimental effects on a 

composite laminates interlaminar strength and toughness. It has been suggested to choose a 

compatible binder with similar chemistry to that of the parent resin matrix for best composite 

performance (2). Moreover, it has been shown that modifying binders with elastomer particles 

can provide for significant increases in interlaminar toughness (5, 6). 

In the present study, two types of preform binders are investigated: a reactive epoxy, and a 

nonreactive thermoplastic polyester. The interply adhesion between woven glass plies was 

measured as a function of binder type, concentration, and preforming conditions. Additionally, 

the effects of the respective binders on the interlaminar properties of a vinyl ester composite 

were addressed. 

2. Experimental 

2.1 Materials 

In this study, two different types of preform binders were evaluated. ATLAC*

 363E, a 

thermoplastic polyester, and PRETEX 110, a catalyzed epoxy with a heat activated curing agent. 

The reinforcement used in this study was E-glass Vetrotex 324 0°/90° woven roving with an 

aerial weight of 24 oz/yd2

. The sizing of the E-glass was Vetrotex product #611, which 

consisted of a vinyl ester/polyester-compatible silane coupling agent and an epoxy film former. 

The resin of interest was a vinyl ester, Dow DERAKANE† 411-C-50, containing 50% styrene 

monomer by weight. 

As seen from its respective dynamic scanning calorimetry (DSC) profile (figure 1), the ATLAC 

binder has a melting temperature at ~55 °C and a glass transition temperature of 47 °C. The 

reactive nature of the PRETEX binder is evident in its DSC profile (figure 2). From figure 2, it 

is seen that PRETEX has a melting temperature at ~60 °C, and upon further heating it is 

observed that an exothermic reaction is taking place, beginning at ~75 °C, and peaking at 

~115 °C. The resulting cross-linked polymer was found to have a glass-transition temperature at 

~110 °C. 

 *

 ATLAC is a registered trademark of Reichhold Chemicals. 

†

 DERAKANE is a registered trademark of the Dow Chemical Company. 
4

 

-10.0

-8.0

-6.0

-4.0

-2.0

0.0

30 35 40 45 50 55 60 65 70

Heat Flow Rate (J/sec.g)

Temperature, °C

First Ramp

Second Ramp

-10.0

-8.0

-6.0

-4.0

-2.0

0.0

30 35 40 45 50 55 60 65 70

Heat Flow Rate (J/sec.g)

Temperature, °C

First Ramp

Second Ramp

Figure 1. DSC thermogram of ATLAC 363E showing glass-transition temperature 

and melting temperature. 

Figure 2. DSC thermogram of PRETEX 110 showing glass-transition 

temperature and melting temperature. 

2.2 Preform Construction 

Preforms consisting of varying binder concentrations of 3, 6, and 9 weight-percent for both 

binders were constructed, where the weight percentage is based on that of the dry reinforcement 

-1.0

0.0

1.0

2.0

3.0

4.0

0 50 100 150 200

Heat Flow Rate, (J/sec.g)

Temperature, °C

Second Ramp

First Ramp
5

only. The powdered binder particles were first applied uniformly to the surface of individual 

fiber plies via a handheld sifter-type apparatus. Subsequently, the mats were placed in a 

noncirculating oven at 65 °C for ~10 min in order to adhere the binder particles to the mat 

surface. Next, individual binder-coated plies were stacked and aligned on one another and 

placed on a flat tool surface within a vacuum bag assembly. The assembly was then placed back 

in the oven and vacuum and heat were applied to fuse the plies into a flat-shaped perform. The 

heat allowed the binder to melt (and react in case of PRETEX), and the pressure served to 

consolidate the preform. Subsequently, the bag assembly was removed from the oven while 

vacuum pressure was maintained in order to maintain compaction until the binder cooled and 

resolidified. Preforms with the ATLAC binder were processed at a temperature of 80 °C for 

30 min, whereas those with the PRETEX binder were processed at 110 °C for 2 hr to ensure 

complete cross linking of the binder during preforming. 

2.3 Composite Fabrication 

Composite laminates were manufactured from the preforms using a VARTM technique. 

Preforms consisted of 8 plies of reinforcement at dimensions of 40 × 40 cm (15 × 15 in), with 

varying concentrations of 3, 6, and 9 weight-percent, or each respective binder. The preforms 

were placed on a flat mold surface within a vacuum bag assembly and infused with the vinyl 

ester resin at room temperature. Following complete infusion and cure of the resin, the 

composite laminates were demolded and postcured in an oven at 130 °C for 2 hr. 

2.4 Preform Characterization 

Preforms were analyzed for binder coverage, spread out, and tow impregnation at their 

respective processing specifications by a scanning electron microscope (SEM). Additionally, 

their interply adhesion was evaluated by a T-peel test in accordance to ASTM D 1876 (12). This 

test method determines the relative peel resistance of adhesive bonds between flexible 

adhedrands, where the material peel strength is measured as the force per unit width required to 

pull apart the two adherends. Preforms (12 × 12 in) were constructed, consisting of two layers of 

woven glass mat bound with binder material at varying concentrations of 3, 6, and 9 weightpercent. Specimens were sectioned from these preforms at dimensions of 7.6 × 30 cm (3 × 12 

in). Specimens manufactured with the ATLAC binder were preformed at a temperature of 80 °C 

for ~30 min. Two sets of specimens were manufactured with the PRETEX binder. The first set 

was processed at 110 °C for 2 hr and the second set at 65 °C for 30 min. Based on the binders 

melting and reaction temperatures of 65 and 110 °C, as determined from DSC, it is expected that 

the binder is fully reacted and cross linked in the first set of specimens, and little or no cross 

linking is achieved in the second set of specimens. The specimens were tested on an Inston 

tensile testing machine with a constant crosshead displacement of 25.4 cm (10 in)/min at ambient 

conditions. 
6

2.5 Composite Performance 

Following the fabrication of the composite laminates, their respective fiber volume and void 

contents were determined. Void content was calculated by determining the actual measured 

density of a composite and comparing it to a theoretical density. The volume of voids was 

computed from the following equation: 

V = ( Td - Md ) / Td, (1)

where V is the volume percent of voids within the composite and Md and Td are the measured and 

theoretical densities of the composite laminate. The measured density of the material was 

determined by the dry/wet weight method outlined in ASTM D 792 (13). The theoretical density 

was calculated based on the individual mass fractions of the constituents, in which the fiber mass 

fraction was determined by a burnout test, and the binder mass fraction was based on the original 

binder loading onto the glass mats during preforming. 

The apparent interlaminar shear strength of the composite specimens was determined in 

accordance to ASTM D 2344 (14), using a short beam shear test. The eight layers of glass ply 

resulted in a composite laminate with an approximate thickness of 0.5 cm (0.20 in). In order to 

ensure specimens fail in shear, it is recommended by the standard to use a length to thickness 

ratio of 7, for glass fiber reinforced composites. Thus, specimens were cut from the flat 

composite laminates at a length of 3.5 cm (1.4 in) and a width of 1.5 cm (0.6 in). A 

span-to-thickness ratio of 5 is suggested, thus a testing span of 2.5 cm (1.0 in) was used. 

Specimens were loaded in an Instron tensile testing machine fixture in three-point bending at a 

span of 2.5 cm (1.0 in) and a testing speed of 0.13 cm (0.05 in)/min. The apparent interlaminar 

shear strengths (SH) were calculated as follows: 

bd

P S B

H

0.75 = , (2) 

where, PB equals the failure load and b and d equal the width and thickness of the specimen, 

respectively. 

The Mode I interlaminar fracture toughness of the specimens was determined in accordance with 

ASTM D 5528 (15). Dual cantilever beam (DCB) specimens were machined from the 

prefabricated composite panels at dimensions of 25.4 cm (10 in) in length and 2.54 cm (1.0 in) in 

width. Kapton* film was used as the nonadhesive insert and provided an initial crack length of 

~6.4 cm (2.5 in). Opening forces were applied to the DCB specimen by means of loading blocks 

that were bonded with an epoxy adhesive to one end of the specimen. The DCB specimens were 

tested at ambient conditions with a screw-driven Instron tensile testing machine at a constant 

crosshead speed of 0.254 cm (0.10 in)/min. The opening crosshead displacement and load were 

recorded by the testing machine, whereas the propagating crack length was recorded by hand 

 *

 Kapton is a registered trademark of DuPont. 
7

with the aid of a traveling magnifying glass. The Mode I critical strain energy release rate, GIC, 

was calculated use modified beam theory by 

3

2 ( | |) IC

P G

b a

δ = + ∆ , (3) 

where P is the applied load, δ is the load point displacement, b is the width of the specimen, a is 

the crack length, and ∆ is a correction factor determined experimentally and is equal to the 

difference between the x intercept and x = 0 points on the least-square plot of cube root of the 

compliance (y-axis) as a function of delamination length (x-axis). 

3. Results and Discussion 

3.1 Preform Analysis 

Figures 3 and 4 show the surface of the fiberglass mat with varying binder loadings of 3 and 

9 weight-percent of ATLAC and PRETEX binders. As the binder loading is increased, the 

surface area coverage increases. It is seen that the two types of binders exhibit similar binder 

coverage and spread out, and the binder materials remain on top of the fiber mat surface. Figure 

5 displays the side view of the binder coated mats, where it is clearly seen that binder spread out 

is limited at these respective processing temperatures (80 °C for ATLAC and 110 °C for 

PRETEX), and the binder does not impregnate into the fiber tows. Additionally, it was found 

that preforms constructed with the PRETEX binder were much more stiff and “board-like” than 

those fabricated with the ATLAC binder. 

(a) (b) 

Figure 3. SEM image showing binder coverage of 3 weight-percent (a) and 9 weightpercent (b) ATLAC binder on woven glass mat processed at 80 °C. 
8

(a) (b) 

Figure 4. SEM image showing binder coverage of 3 weight-percent (a) and 9 weightpercent (b) PRETEX binder on woven glass mat processed at 110 °C. 

(a) (b) 

Figure 5. SEM micrographs showing the limited tow impregnation (a) of ATLAC binder 

processed at 80 °C and (b) PRETEX binder processed at 110 °C. 

3.2 Interply Adhesion of Preforms (T-Peel Test) 

The interply adhesion of the preforms was evaluated with a T-Peel test. Results of the test can 

be found in table 1 and figures 6 and 7. Typical load-vs.-displacement curve for the T-Peel test 

can be observed in figure 6. It was observed that the specimens exhibited a stick/slip type 

behavior, which is due to the uneven distribution of binder on the fiber mat surface and also 
9

Table 1. Results of T-Peel test for 0°/90° woven E-glass tackified with ATLAC 363E and 

PRETEX 110 binders. 

 Peel Strength, (N/cm) 

Binder Type 3 Weight-Percent 6 Weight-Percent 9 Weight-Percent 

PRETEX 110 reacted 7.85 ± 2.61 15.52 ± 3.87 24.50 ± 2.96 

PRETEX 110 unreacted 0.103 ± 0.028 0.166 ± 0.051 0.166 ± 0.026 

ATLAC 363E 0.653 ± 0.186 1.21 ± 0.354 1.64 ± 0.527 

Figure 6. Load-vs.-displacement curve for T-Peel test of 3-in-wide 

specimen of E-glass with 6 weight-percent of varying 

binder type. 

perhaps to the wavy architecture of the woven mat. Both factors would contribute to areas where 

the two plies do not perfectly adhere together. This stick/slip behavior became more pronounced 

at higher binder concentrations for each respective sample set. 

The results from the peel test show that interply adhesive strengths increase as the binder loading 

is increased. This can be attributed to higher surface area coverage of the binder material. 

Results from the T-Peel test show that there is a much greater interply adhesion (15× greater at 

9 weight-percent binder loading) for preforms constructed with the reactive epoxy (PRETEX) 

binder than those with a low-melting thermoplastic (ATLAC). It is believed that the 

thermoplastic binder simply provides a mechanical interlocking between adjacent plies, whereas 

if processed correctly, the reactive epoxy binder can provide an additional chemical adhesion 

with the fiber sizing. This, in turn, will result in much better interply adhesion, resulting in a 

more board-like preform with greater structural integrity. It was also found that specimens in 
10

Figure 7. Peel strength vs. binder concentration for ATLAC and PRETEX 

binders on woven E-glass mats. 

which the PRETEX binder was not reacted (processed at 65 °C for 30 min) exhibited very low 

adhesion. At this lower processing temperature, the binder material softens but is not allowed to 

flow and spread across the mat surface, or to undergo any crosslinking. Additionally, it was 

found that much of the binder could be easily brushed off the fiber mat surface due to poor 

adhesion. Thus, it is concluded that processing temperatures of 65 °C and lower are not adequate 

for preforms using PRETEX as the binder material. 

The difference in interply adhesion between the reacted PRETEX and ATLAC specimens is also 

portrayed in the respective specimens failure. Samples made with the ATLAC binder exhibited 

a clean separation, whereas those made with the reacted PRETEX binder did not. From figure 8 

it can be seen that the PRETREX specimens exhibited a “spider-webbing” type failure, resulting 

from the high adhesion that causes fiber bridging between plies. This bridging of fibers is also 

evident in the SEM image shown in figure 9. The SEM image in figure 10 also reveals that the 

predominant type of failure in both sets of specimens was an adhesive failure between the fiber 

and the binder material. Additionally, it appeared that ATLAC is a more brittle binder with the 

existence of fracture and cracking through the binder material. 

3.3 Void Content Determination 

Following the fabrication of the composite laminates, their respective fiber volume and void 

contents were determined. These factors are significant in that often times they influence the 
11

Figure 8. Comparison of T-Peel test specimens 

bound by ATLAC and reacted PRETEX 

binder on 0°/90° woven E-glass. 

Figure 9. SEM micrograph of fiber mat surface of 

6 weight-percent reacted PRETEX peel 

specimen at magnification of 75×. 

mechanical response of the composite laminate. The results of the void and fiber contents of the 

composites are summarized in table 2. 
12

(a) (b) 

Figure 10. SEM micrographs of fiber mat surface of (a) 6 weight-percent ATLAC peel 

specimen at 200× and (b) 6 weight-percent reacted PRETEX peel specimen at 

250×. 

Table 2. Fiber volume fraction and void content of glass-reinforced vinyl ester composite 

laminates with varying binder concentrations. 

 

ATLAC 363E PRETEX 110 

Binder Loading Vf % Vv % Vf % Vv % 

No binder 47.5 ± 0.5 1.78 ± 0.21 47.5 ± 0.5 1.78 ± 0.21 

3% 48.0 ± 0.6 1.63 ± 0.28 49.4 ± 2.4 2.11 ± 0.24 

6% 47.9 ± 0.9 1.99 ± 0.57 53.7 ± 1.6 4.64 ± 1.71 

9% 51.2 ± 1.9 3.00 ± 1.76 55.6 ± 0.4 3.26 ± 1.03 

The fiber volume fractions of the composite laminates are ~48%–50% with the exception of the 

two laminates containing 6% and 9% PRETEX binder, which are slightly higher. From table 2, 

it is also seen that the composite laminates containing 6 and 9 weight-percent PRETEX binder 

had the highest void contents, although the standard deviations are moderately high. This greater 

fiber volume fraction may be attributed to less preform springback during infusion with the 

PRETEX preforms than the ATLAC preforms, due to the high interply adhesion as previously 

mentioned. Additionally, the ATLAC binder was soluble in the infusing resin, whereas once 

cross linked, the PRETEX binder is not. 

SEM was also done to examine the void contents of the samples. The results from this analysis 

can be seen in figures 11 and 12. From the SEM micrographs, it can be seen that all of the 

composite samples contained some voids. It can be seen that the voids in the composite laminate 

without binder are relatively small in comparison to the larger voids in the laminates with binder 

material. As noted in the figures, the composites with 9 weight-percent PRETEX and 
13

Figure 11. SEM micrograph of woven glass fiber vinyl 

ester DERAKANE 411-C-50 composite 

laminate with no binder at 55× magnification. 

(a) (b) 

Figure 12. SEM micrograph of interlaminar void within composite laminates with (a) 

9 weight-percent PRETEX binder and (b) 9 weight-percent ATLAC at 60×. 

9 weight-percent ATLAC had large voids concentrated in the interlaminar regions and small 

voids within the fiber tows. The composite without binder also contained small voids within the 

fiber tows, but contained minimal interlaminar voids. This suggests that the binder material 

concentrated in the interlaminar regions (due to poor tow impregnation, figure 5) inhibits the 

proper filling of the resin, thus creating interlaminar voids. 
14

3.4 Binder Effect on Interlaminar Shear Strength 

The results of the short beam shear test are displayed in table 3, and figure 13. The results 

indicate that the incorporation of both binder types into woven glass-reinforced vinyl ester 

composite laminates results in lower interlaminar shear strengths. The effect becomes more 

pronounced as additional binder is used in the preform. Although both binders proved to be 

detrimental in regards to shear strength, the composite laminates with the PRETEX binder faired 

better. A laminate with 9 weight-percent ATLAC binder resulted in a reduction of interlaminar 

shear strengths by ~23%, whereas the laminate with 9 weight-percent PRETEX binder resulted 

in a reduction of ~15%. This reduction in interlaminar shear strengths is most likely due to the 

increased interlaminar void content resulting from the introduction of the binder as discussed 

earlier. 

Table 3. Interlaminar shear strengths of glass reinforced vinyl ester composite laminates 

with varying binder concentrations. 

 Interlaminar Shear Strength, (N/cm2

) 

Binder Loading ATLAC 363E PRETEX 110 

No binder 4615 ± 204 4615 ± 204 

3% 4407 ± 115 4463 ± 182 

6% 3967 ± 182 4139 ± 222 

9% 3576 ± 173 3921 ± 271 

Figure 13. Interlaminar shear strengths of composite laminates 

manufactured from woven glass preforms of varying binder 

type and concentration. 
15

3.5 Binder Effect on Interlaminar Fracture Toughness 

Figure 14 shows the load-vs.-displacement curve for three individual composite DCB specimens, 

that of the pure resin and glass fabric without binder, a composite laminate with 9 weight-percent 

(with respect to glass mat weight only) ATLAC binder and a laminate with 9 weight-percent 

PRETEX binder. These plots are representative of the other specimens tested in each respective 

sample set. As the resulting data shows, composites with the PRETEX binder showed higher 

fracture toughness values compared to the control composite panel (no binder), whereas the 

composites made from preforms using the ATLAC binder showed lower fracture toughness 

values. Additionally, from figure 14, it is seen that each specimen exhibited a crack propagation 

that followed a “stick-slip” type of failure indicated by the jagged peaks in the plot. However, as 

indicated in figure 14, it was noticed that the composite panels containing the PRETEX binder 

showed the most stable propagation, with many more smaller crack propagations during loading. 

The results of the testing can be seen in figures 15 and 16 and in table 4. Many samples 

exhibited an R-curve (resistance curve) behavior, although, this type of behavior was not seen 

with many of the specimens containing ATLAC binder. 

From the results, it is seen that the introduction of the ATLAC binder into the composite 

laminate caused detrimental effects on the Mode I interlaminar fracture toughness. There is 

nearly a 60% decrease in the GIC propagation, between the composite panel with no binder, and 

that with a 9 weight-percent loading of the ATLAC binder. On the other hand, it is seen that the 

introduction of the PRETEX binder has the opposite effect, and the interlaminar fracture 

toughness GIC propagation, is increased by ~50% at binder loadings of 6 and 9 weight-percent. 

Figure 14. Load vs. displacement of composite DCB specimens. 
16

Figure 15. Delamination curve showing R-curve behavior for glass-reinforced 

DERAKANE 411-C-50 vinyl ester composites with varying binder. 

Figure 16. Mode I propagation fracture toughness of composite laminates 

with varying binder type and concentration. 
17

Table 4. Mode I initiation fracture toughness of composite laminates, GIC, with varying binder 

type and concentration. 

Interlaminar Fracture Toughness 

(J/m2

) 

 Laminates With ATLAC Laminates With PRETEX 

Binder Concentration 

(Weight-Percent of Fibers) 

Initiation 

GIC

Propagation 

GIC

Initiation 

GIC

Propagation 

GIC

No binder 576 ± 142 855 ± 152 576 ± 142 855 ± 152 

3 455 ± 96 560 ± 140 928 ± 105 1126 ± 110 

6 291 ± 75 404 ± 112 1096 ± 154 1261 ± 177 

9 273 ± 60 357 ± 60 1033 ± 114 1257 ± 169 

The improved toughness of the composite laminates containing PRETEX binder is believed to be 

a result of the high interply adhesion developed during the preforming stages when the binder 

was cross linked and possibly chemically bound to the fiber sizing. For the case of preforms 

made with the thermoplastic polyester ATLAC binder, the interply adhesion is solely due to a 

mechanical interlocking. Thus, there was a much lower interply adhesion with preforms 

fabricated with this binder. Additionally, if the binder had not completely dissolved, it may act 

as a barrier between the matrix resin and fiber mat surface, inhibiting proper formation and 

chemical bonding at the fiber matrix interphase, and result in lower interply toughness. 

Subsequent to fracture toughness testing, an SEM was used to examine the fracture surfaces of 

the specimens. Figure 17 shows the fracture surface of the composite DSB specimen with 9 

weight-percent ATLAC loading. It can be seen that much of the failure was of a brittle cohesive 

type, with smooth and flat fracture surface through the bulk of the matrix. Additionally, it is 

seen that there exists a cohesive type failure between the fiber and matrix (or binder) interface as 

indicated by the fiber imprints in the resin. 

(a) (b) 

Figure 17. SEM micrographs of fracture surface of DCB specimen of composite laminate 

containing 9 weight-percent ATLAC (a) 150× (b) 100×. 
18

In the composite specimens consisting of PRETEX binder, the majority of the failure was 

cohesive between the individual fibers and the matrix (resin or binder) as shown in figure 18. 

In areas where the failure was through the matrix, the surface consisted of rough pocket-like 

dimples as shown in figure 18b. In contrast to the ATLAC specimens, this suggests a tougher 

ductile-type fracture. 

(a) (b) 

Figure 18. SEM micrographs of fracture surface of DCB specimen of composite laminate containing 

9 weight-percent PRETEX at (a) 75× and (b) 50×. 

4. Conclusion 

It is concluded that both the ATLAC 363E and PRETEX 110 binders can provide sufficient 

adhesion between adjacent plies of woven glass mat to construct preforms that are able to 

maintain their flat shape during handling. With the aid of SEM, it was determined that both 

binders exhibited similar fiber mat coverage and spread out at their individual processing 

parameters. SEM images also indicate that both binder materials appear to remain on the surface 

of the glass fabric, with little or no penetration into the fiber tows. 

Results from the T-Peel test show that there is a much greater interply adhesion (15× greater at 

9 weight-percent binder loading) for preforms constructed with the reactive epoxy (PRETEX) 

binder than for those with a low-melting thermoplastic (ATLAC). It is believed that the 

thermoplastic binder simply provides a mechanical interlock between adjacent plies, whereas, if 

processed correctly, the reactive epoxy binder can provide an additional chemical adhesion with 

the fiber sizing. This in turn, will result in much better interply adhesion, resulting in a more 

board-like preform with greater structural integrity. It can be concluded that reactive binders, 
19

which chemically interact with the fiber sizing, are better suited in applications where 

complex-shaped preforms with little springback are required. 

From the SEM analysis of the manufactured composite laminates, it was concluded that the 

introduction of binder material had led to higher void contents which were concentrated in the 

interlaminar regions of the composite. Additionally, short beam shear testing concluded that the 

binder had detrimental effects on the composites interlaminar shear strength. It was determined 

that this effect became more pronounced at higher preform binder loadings. A composite 

laminate fabricated from a woven glass preform containing 9 weight-percent ATLAC 363E 

binder exhibited a reduction of interlaminar shear strength by ~23 weight-percent when 

compared to that of the same laminate without binder. Likewise, laminates with the 

9 weight-percent PRETEX binder exhibited approximately a 15% reduction in interlaminar shear 

strength. This reduction in interlaminar shear strength is believed to be a result of the increase in 

interlaminar voids resulting from the binder. 

From the Mode I interlaminar fracture toughness testing, it was found that although composites 

of ATLAC bound preforms showed a decrease in fracture toughness, for composites of PRETEX 

bound preforms there were substantial improvements. The composite laminate with 

9 weight-percent ATLAC binder resulted in a reduction in Mode I propagation interlaminar 

fracture toughness by ~60%. However, the composites specimens tested with 9 weight-percent 

PRETEX binder resulted in an increase in fracture toughness by an impressive 47%. 

Additionally, it was found that the PRETEX specimens exhibited a much more stable fracture, 

whereas the ATLAC specimens exhibited a “stick-slip” type crack propagation. 

From the results, it was realized that one could get a significantly large variation in interlaminar 

strengths and toughness values by simply varying the binder type and concentration. Thus, this 

demonstrates the potential for using preform binders to tailor the interlaminar regions of a 

composite laminate in addition to the inherent benefits provided by the preforms themselves. 
20

5. References 

1. Shih, C. H.; Lee, L. Tackification of Textile Fiber Preforms in Resin Transfer Molding. 

Journal of Composite Materials 2001, 35 (21), 1954–1981. 

2. Kittelson, J. L.; Hackett, S. C. Tackifier/Resin Compatibility Is Essential for Aerospace 

Grade Resin Transfer Molding. Proceedings of the 39th International SAMPE Symposium, 

Anaheim, CA, 1994; pp 83–96. 

3. Chen, J.; Backes, D.; Jayarman, K. Dynamics of Binder Displacement in Liquid Molding. 

Polymer Composites 1996, 17 (1), 23–33. 

4. Rohatgi, V.; Lee, J. Moldability of Tackified Fiber Preforms in Liquid Composite Molding. 

Polymer Composites 1997, 31 (7), 720–744. 

5. Hillermeier, R. W.; Seferis, J. C. Interlayer Toughening of Resin Transfer Molding 

Composites. Composites: Part A 2001, 32, 721–729. 

6. Hillermeier, R. W.; Hayes, B. S.; Seferis, J. C. Processing and Performance of TackifierToughened Composites for Resin Transfer Molding Techniques. Proceedings of the 44th 

International SAMPE Symposium, Long Beach, CA, 1999; pp 660–669. 

7. Shih, C. H.; Liu, Q.; James, L. Tackified SCRIMP for Aerospace Applications. 

Proceedings of the 45th International SAMPE Symposium, Long Beach, CA, 2000. 

8. Knight, J. C; Backes, D.; Jayarman, K. Consolidation and Relaxation Behavior of 

Continuous Strand Random Glass Mats With Thermoplastic Binders. Polymer Composites

1996, 17 (3), 451–457. 

9. Backes, D.; Jayaraman, K.; Petty, C. SAE technical paper no. 930.175; Society of 

Automotive Engineers: Dearborn, MI, 1993. 

10. Huang, Y. J.; Horng, J. C. Effects of Thermoplastic Additives on Mechanical Properties and 

Glass Transition Temperatures for Styrene-Crosslinked Low-Shrink Polyester Matrices. 

Polymer 1998, 39 (16), 3683–3695. 

11. Brody, J. C. The Evaluation of Preform Binders in Laminated Composite Materials. 

Masters Thesis, University of Delaware, Newark, DE, 2003. 

12. ASTM D 1876. Standard Test Method for Peel Resistance of Adhesives 1993. 

13. ASTM D 792. Standard Test Method for Density and Specific Gravity of Plastics by 

Displacement 1991. 
21

14. ASTM D 2344. Apparent Interlaminar Shear Strength of Parallel Fiber Composites by 

Short-Beam Method 1984. 

15. ASTM D 5528. Standard Test Method for Mode I Interlaminar Fracture Toughness of 

Unidirectional Fiber-Reinforced Polymer Matrix Composites 1994a. 
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 M FATEH RDV 31 

 WASHINGTON DC 20590 

 3 CYTEC FIBERITE 

 R DUNNE 

 D KOHLI 

 R MAYHEW 

 1300 REVOLUTION ST 

 HAVRE DE GRACE MD 21078 

 1 DIRECTOR 

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 IANG TMT 

 2055 BOULDERS RD 

 CHARLOTTESVILLE VA 

 22911-8318 

 1 SIOUX MFG 

 B KRIEL 

 PO BOX 400 

 FT TOTTEN ND 58335 

 2 3TEX CORP 

 A BOGDANOVICH 

 J SINGLETARY 

 109 MACKENAN DR 

 CARY NC 27511 

 1 3M CORP 

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 3M CENTER BLDG 60 IN 01 

 ST PAUL MN 55144-1000 
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 1 DIRECTOR 

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 TA 5 

 K CRELLING 

 WASHINGTON DC 20310 

 1 ADVANCED GLASS FIBER YARNS 

 T COLLINS 

 281 SPRING RUN LANE STE A 

 DOWNINGTON PA 19335 

 1 COMPOSITE MATERIALS INC 

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 19105 63 AVE NE 

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 1 JPS GLASS 

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 PO BOX 260 

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 1 COMPOSITE MATERIALS INC 

 R HOLLAND 

 11 JEWEL CT 

 ORINDA CA 94563 

 1 COMPOSITE MATERIALS INC 

 C RILEY 

 14530 S ANSON AVE 

 SANTA FE SPRINGS CA 90670 

 2 SIMULA 

 J COLTMAN 

 R HUYETT 

 10016 S 51ST ST 

 PHOENIX AZ 85044 

 2 PROTECTION MATERIALS INC 

 M MILLER 

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 14000 NW 58 CT 

 MIAMI LAKES FL 33014 

 2 FOSTER MILLER 

 M ROYLANCE 

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 195 BEAR HILL RD 

 WALTHAM MA 02354-1196 

 1 ROM DEVELOPMENT CORP 

 R O MEARA 

 136 SWINEBURNE ROW 

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 NEWPORT RI 02840 

 2 TEXTRON SYSTEMS 

 T FOLTZ 

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 1449 MIDDLESEX ST 

 LOWELL MA 01851 

 1 O GARA HESS & EISENHARDT 

 M GILLESPIE 

 9113 LESAINT DR 

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 2 MILLIKEN RESEARCH CORP 

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 SPARTANBURG SC 29303 

 1 CONNEAUGHT INDUSTRIES INC 

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 1 ARMTEC DEFENSE PRODUCTS 

 S DYER 

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 COACHELLA CA 92236 

 1 NATL COMPOSITE CTR 

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 2000 COMPOSITE DR 

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 3 PACIFIC NORTHWEST LAB 

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 1 SAIC 

 M PALMER 

 1410 SPRING HILL RD STE 400 

 MS SH4 5 

 MCLEAN VA 22102 
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 1 ALLIANT TECHSYSTEMS INC 

 4700 NATHAN LN N 

 PLYMOUTH MN 55442-2512 

 1 APPLIED COMPOSITES 

 W GRISCH 

 333 NORTH SIXTH ST 

 ST CHARLES IL 60174 

 1 CUSTOM ANALYTICAL 

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 A ALEXANDER 

 13000 TENSOR LANE NE 

 FLINTSTONE MD 21530 

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 1745 JEFFERSON DAVIS HWY 

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 3 ALLIANT TECHSYSTEMS INC 

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 WV01 16 STATE RT 956 

 PO BOX 210 

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 26726-0210 

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 1 PRATT & WHITNEY 

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 400 MAIN ST MS 114 37 

 EAST HARTFORD CT 06108 

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 1100 WEST HOLLYVALE ST 

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 1 BRIGS COMPANY 

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 HERNDON VA 22071-2443 

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 L ZERNOW 

 425 W BONITA AVE STE 208 

 SAN DIMAS CA 91773 

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 2 GENERAL DYNAMICS OTS 

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 1 GKN WESTLAND AEROSPACE 

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 WALLINGFORD PA 19086 
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 5 SIKORSKY AIRCRAFT 

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 S GARBO MS S330A 

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 6900 MAIN ST 

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 1 AEROSPACE CORP 

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 ANAHEIM CA 92806 

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 SANTA CLARA CA 95052 

 1 UDLP WARREN OFC 

 A LEE 

 31201 CHICAGO RD SOUTH 

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 P JANKE MS 170 

 4800 EAST RIVER RD 

 MINNEAPOLIS MN 55421-1498 

 1 LOCKHEED MARTIN 

 SKUNK WORKS 

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 1011 LOCKHEED WAY 

 PALMDALE CA 93599-2502 

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 5537 PGA BLVD 

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 & SYSTEMS DIV 

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 1745A W NURSERY RD 

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 991 ANNAPOLIS WAY 

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 6 INST FOR ADVANCED 

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 I MCNAB 

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 C PERSAD 

 3925 W BRAKER LN STE 400 

 AUSTIN TX 78759-5316 

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 1233 SHELBURNE RD STE D8 

 SOUTH BURLINGTON VT 

 05403-7700 

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 409 W CATHERINE ST 

 BEL AIR MD 21014-3613 
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 1 SAIC 

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 8500 NORMANDALE LAKE BLVD 

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 BLOOMINGTON MN 55437-3828 

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 LOS ANGELES CA 90024-1597 

 2 UNIV OF DAYTON 

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 LOWELL MA 01854 

 1 IIT RESEARCH CTR 

 D ROSE 

 201 MILL ST 

 ROME NY 13440-6916 

 1 GA TECH RESEARCH INST 

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 P FRIEDERICH 

 ATLANTA GA 30392 

 1 MICHIGAN ST UNIV 

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 212 EARTH ENGR 

 SCIENCES BLDG 

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 1 STANFORD UNIV 

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 & AEROBALLISTICS 

 S TSAI 

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 1 UNIV OF MAINE 

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 R LOPEZ ANIDO 

 5793 AEWC BLDG 

 ORONO ME 04469-5793 

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 11100 JOHNS HOPKINS RD 

 LAUREL MD 20723-6099 

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 5 UNIV OF DELAWARE 

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 201 SPENCER LAB 

 NEWARK DE 19716 
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 SCIENCE & ENGRG 

 UNIV OF ILLINOIS 

 AT URBANA CHAMPAIGN 

 J ECONOMY 

 1304 WEST GREEN ST 115B 

 URBANA IL 61801 

 1 UNIV OF MARYLAND 

 DEPT OF AEROSPACE ENGRG 

 A J VIZZINI 

 COLLEGE PARK MD 20742 

 1 DREXEL UNIV 

 A S D WANG 

 3141 CHESTNUT ST 

 PHILADELPHIA PA 19104 

 3 UNIV OF TEXAS AT AUSTIN 

 CTR FOR ELECTROMECHANICS 

 J PRICE 

 A WALLS 

 J KITZMILLER 

 10100 BURNET RD 

 AUSTIN TX 78758-4497 

 3 VA POLYTECHNICAL 

 INST & STATE UNIV 

 DEPT OF ESM 

 M W HYER 

 K REIFSNIDER 

 R JONES 

 BLACKSBURG VA 24061-0219 

 1 SOUTHWEST RESEARCH INST 

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 J RIEGEL 

 6220 CULEBRA RD 

 PO DRAWER 28510 

 SAN ANTONIO TX 78228-0510 

 1 BATELLE NATICK OPERS 

 B HALPIN 

 313 SPEEN ST 

 NATICK MA 01760 

 3 DIRECTOR 

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 A FRYDMAN 

 2800 POWDER MILL RD 

 ADELPHI MD 20783-1197 

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 W C FRAZER 

 400 COLLERAN RD 

 APG MD 21005-5059 

 91 DIR USARL 

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 D LYON 

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 P PLOSTINS 

 A ZIELINSKI 

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 P CONROY 

 B FORCH 

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 C LEVERITT 

 R LIEB 

 R PESCE RODRIGUEZ 

 B RICE 

 AMSRD ARL WM BF 

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 J MCCAULEY 

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 L GHIORSE 

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 T BOGETTI 

 L BURTON 

 R CARTER 

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 G DEWING 

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 D HENRY 

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 R KASTE 

 L KECSKES 

 M MINNICINO 

 B POWERS 

 D SNOHA 

 J SOUTH 

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 AMSRD ARL WM MC 

 J BEATTY 

 R BOSSOLI 

 E CHIN 

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 D GRANVILLE 

 B HART 

 J LASALVIA 

 J MONTGOMERY 

 F PIERCE 

 E RIGAS 

 W SPURGEON 

 AMSRD ARL WM MD 

 B CHEESEMAN 

 P DEHMER 

 R DOOLEY 

 G GAZONAS 

 S GHIORSE 

 C HOPPEL 

 M KLUSEWITZ 

 W ROY 

 J SANDS 

 D SPAGNUOLO 

 S WALSH 

 S WOLF 

 AMSRD ARL WM RP 

 J BORNSTEIN 

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 AMSRD ARL WM T 

 B BURNS 

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 W BRUCHEY 

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 1 LTD 

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 316 ROUTE DE BAYONNE 

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 1 DEUTSCHE AEROSPACE AG 

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