Performance Enhancement of Concrete

Through the Use of Waste Injection

Molding Pellets: A Preliminary
Study of Viability
B. LENNON, V. M. KARBHARI* H. ALLEN
AND
Center for Composite Materials and Department of Civil Engineering
University of Delaware
Newark, DE 19716
ABSTRACT: The recycling of advanced polymers and composites is a major problem
facing the composites industry due not only to problems related to the actual process itself
but also to liability issues associated with reuse. This article presents the initial results of
an ongoing investigation aimed at the reuse of waste pellets as aggregate in concrete to in-
crease the compression strength and ductility of the resulting concrete. A variety of glass-
filled materials, including nylon, polycarbonate, and polypropylene—as well as unrein-
forced polymers such as PET and PEEK—were used. Materials were substituted for
traditional stone aggregate at a range of levels including complete replacement. Results
demonstrate the viability of such use, and the article discusses implications in terms of
future applications, as well as advances needed, in order to make this approach a reality.

KEY WORDS: composites, recycling, injection molding, pellets, flexure, toughness.

INTRODUCTION
FUTURE USE of advanced
polymers composites depend and
only will not
HE the achievement of designed
on materials profiles and high performance
levels at low cost but also on their ability to be recycled or reused. Today’s com-
petitive materials environment has already witnessed the increasing use of metals
in areas where composites were making inroads, due merely to the stigma of
composites not being &dquo;environmentally friendly.&dquo; Legislation is already in place
in both Europe and the United States that mandates the use of a certain percent-
age of recycled polymers in a number of industrial products. The European
Economic Community (EEC) has already decreed that by the end of 1993, 50 %
by weight of all plastics and composites used in automobiles must be recycled; on
the other hand, U.S. regulations are already being put into place mandating lower

*Author to whom correspondence should be addressed

Journal of THERMOPLASTIC COMPOSITE MATERIALS, Vol. 6- January 1993 49

0892-7057/93/01 0049-13 $6.00/0
@ 1993 Technomic Publishing Co , Inc.

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
50

amounts of recyclability. However, increasing pressure is being brought to bear

on governments and regulatory agencies to set up a materials recycling tax on the
suppliers, thereby severely restricting the use of non-recyclable or non-reusable
materials. This threatened tax is leading automobile manufacturers to ask suppli-
ers and subcontractors to commit to taking back parts after their useful life and,
in some cases - Nissan, for example - to reconsider the overall use of composites
in automotive components (McDermott, 1993). In a recent move, Ford Motor
Company published worldwide recycling guidelines to encourage design prac-
tices that ensure easy separation of materials and overall use of recyclable compo-
nents (Ford, 1993).
The recyclability of plastics and composites is a strategic issue of concern for
the entire industry. Although plastics make up only about 7 % of solid wastes at
present and are expected to account for 10 % of solid municipal waste by the year
2000, they are a very visible 30% by volume (Thayer, 1989). There is a growing
perception that plastics, and now composites, constitute a threat to the environ-
ment, with increasing concern being shown by the advanced composites industry
to existing and pending legislation. Although the current focus is on plastic pack-
aging and bottles, the actual problem lies in the significant amount of waste and
scrap generated in the fiber-reinforced composites industry. As yet, this problem
has not received major attention in the U.S., although the EEC has already made
significant strides in both technical and legislative efforts (Jutte and Graham,
1991). Of the advances made in the U.S., the primary thrust has come from the
SMC and BMC industries, which have taken an early and active role in defining
and determining novel, yet responsible, methods for reuse of their glass-
reinforced products (Jutte and Graham, 1991; Butler, 1991; SMC Automotive
Alliance, 1991; Hudec, 1991; Watt and Xu, 1991).
Generally, it can be argued that waste/scrap can be dealt with in one of four
ways-burning or incineration, burial in landfills, reuse or reprocessing, and
waste minimization (Rathje, 1989). Palmero (1982) has argued that at a more
specific level, options can be arranged in pyramid fashion listing the evolution of
materials from primary reuse to incineration and final disposal. For thermosets,
for example, the approaches can be outlined as a four-tiered pyramid. The first
tier, obviously the most desirable, consists of the reintroduction of waste into the
raw material stream itself. At the second tier, material is used as filler for lower-

grade materials. The third level consists of uses such as in asphalt and concrete,
whereas at the fourth and lowest level, the scrap/waste can be either pyrolyzed to
generate feed stock and oils or incinerated for energy recovery. Obviously, it
would be desirable if all waste could be used perpetually at levels one or two, but
failing that, if they were made to follow the pyramid structure in use as value-
added products through each level, the downward progression being driven by
each new life-cycle in a new form. The use of PET from soda bottles in carpet
backing is an example of this progression (Carreras, 1992). There are several
technical approaches to the disposal, recycling, or reuse of glass-reinforced com-
posites, among which the most often cited are incineration, chemical degradation
(hydrolysis, glycolysis, and saponification), pyrolysis, size reduction, and reuse
as a value-added product. The addition of carbon fiber to resin systems creates an

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
 51

entirely different set of issues related to recomposition and/or reuse and will be
addressed separately at a later date.
In this article, we describe the preliminary results of an approach aimed at
the value-added reuse of pellets as aggregate in cement concrete. The overall
objective of the program is to demonstrate and develop the use of composite
and polymer aggregate as value-added replacements for the stone aggregate
used traditionally in cements. The motivation was to find an alternative to dis-
posal of these materials in landfills while simultaneously improving the perfor-
mance of cement for specialized construction, as well as to present an approach
that may reduce the level of ASR (alkali silica reaction) degradation in concrete.
It is emphasized that the development of this concept requires knowledge of
both polymer and cement chemistry and must stress the use of low-cost routes
in order to be of value in the civil engineering arena. It is expected that a
majority of the audience will be from the plastics and advanced composites
arena; hence, a brief summary of cements and their chemistry is provided in the
next section.

CEMENT AND CONCRETE

Portland cements are inorganic powder compounds manufactured generically
by burning a mixture of limestone (usually a low-magnesium type), clay (low-
alkali variety) and some iron ore in a kiln at about 1450°C to produce a cement
&dquo;clinker&dquo; comprised mainly of C3S (alite-an impure tricalcium silicate), CZS
(belite-an impure dicalcium silicate), C3A (an aluminate phase consisting
mainly of tricalcium aluminate), and C4AF (a ferrite phase-tetracalcium
aluminoferrite). The nomenclature used follows that commonly used in the in-
dustry wherein the common oxides are denoted by their first letters: C CaO, =

S = Si02, A = A1203, and F Fe203. This mixture is mixed with about

=

3-5 % of gypsum and is ground to form Portland cement. Approximate composi-

tions and fineness ranges for the five major types of ASTM standard Portland ce-
ment are given in Table 1.
When Portland cement is mixed with water, a series of hydration reactions
occurs, the chemistry of which is complex and the exact mechanisms still
debatable (Tayler, 1990; Skalny, 1989). Approximately 80% of the cement is
made up through reactions of alite (a form of tricalcium silicate, C3S) and belite

Table 1. Standard composition of ASTM Portland cement (ACI 225 R-85).

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
52

Table 2. Ranges of compressive strengths as a

function of time.

(an impure dicalcium silicate, €28) at stoichiometries as below:

where C1,7 SH2 is the non-stoichiometric calcium silicate hydrate, and CH rep-
resents the calcium hydroxide. Hydration reactions are slow and can take years
to reach completion. However, under the appropriate conditions, the main setting
reactions can be completed within the first day, giving the concrete enough
strength and stiffness to support itself. Normally, tests are conducted at intervals
of 7, 14, and 28 days to assess strength; the latter figure is the time at which about
75 % of the alite reaction is completed. It should be noted that the hydration of the
CaO compounds to Ca(OH)2 and CaO-SiO2-H20 gels leads to the formation of
fibrils that hold the components of the cement paste together. The formation of
these fibrils and therefore of the transition zone is extremely critical for the
achievement of a high-strength mix. Sand is generally added as a strengthening
agent, along with stone aggregate, to form concrete. During setting, the original
pores filled with water are filled with solid hydrate reaction products, with the C-
S-H gels (CaO-Si02-H20) acting as binders having a high specific surface area
and a low degree of crystallinity.
Concrete mixtures must have an intricate balance among a number of factors,
often involving tradeoffs between workability and final performance. The water-
cement ratio is one such example: usually between 0.40 and 0.50, about 60% is
needed for the completion of hydration chemistry, the rest being adsorbed in the
C-S-H gel. Too much water causes porosity and a more permeable and weak con-
crete, whereas too little results in poor workability, insufficient expansion space
for the hydration of C-S-H, and poor concrete due to incomplete (or constrained)
hydration. Typical ranges of compressive strengths of traditionally moisture-
cured concretes are given in Table 2. The interested reader is referred to the ex-
cellent works of Taylor (1990) and Lea (1971) for further details on chemistry and
performance as related to the creation of a microstructure, which in many ways
is similar to that of a composite at the microscopic level.
Despite the long history and widespread use of concrete in various forms and

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
 53

chemistries, the limitations are rather severe, although most can be &dquo;designed
around.&dquo;The main limitations are listed below:
~ low tensile and flexural strengths
~ brittleness
~
potential for cracking during hydration due to excessive temperature gradients
formed due to heat-of-hydration
.
variability of aggregates
.
susceptibility to reactions between hydration product alkalis and the aggregate
.
susceptibility to attack by sulfates, acids and frost
Although the compressive strength of concrete is touted as its major advantage
over other materials, its tensile strength-less than 1000 psi on the average-is
negligible and, on overall comparison, fares poorly even when compared to alu-
minum (Table 3).
In fact, there are a number of applications where modifications to concrete/
cement slurries through better aggregate/additives would prove advantageous,
especially if they could be achieved without a significant increase in cost or
complexity of mix. The use of advanced fibers for increasing toughness and
tensile and flexural strength has been the focus of considerable attention
(Mobasher and Shah, 1989); however, the use of replacement aggregate has not
received the attention it deserves, beyond its use in &dquo;econocrete&dquo; and as the sub-
grade in pavements. Rather than consider the use of specifically tailored
&dquo;composite-aggregate,&dquo; we emphasize the use of waste as aggregates in this arti-
cle, focusing on the reuse potential of composite waste as value-added products
in concrete.
A major concern of late is the degradation of concrete structures due to alkali
reactions between the slurry and certain fine-grained silicate rock aggregates. In
alkali reactivity, sodium and potassium give rise to strong hydroxide solutions
that attack aggregate and dissolve silica, giving a hydrophobic silica gel as the by-
product. In the presence of water, the gel expands, cracking the concrete. Cur-
rently, additives are used in an attempt to control the reaction and reduce con-
crete degradation. Fly ash is often used as an additive and is reputed to be an
effective agent of alkali reaction retardation, as the alkalis react with the glass in
fly ash during curing and are effectively neutralized from further reaction. How-
ever, quality control and uniformity of fly ash mixed concrete is still question-
able. The use of glass-filled pellets may also help in decreasing alkali reaction

Table 3. Baseline properties.~ ~ ~~

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
54

degradation in addition to enhancing the performance (specifically in flexure) of

concrete.

MATERIALS AND FABRICATION OF TEST SPECIMENS

In this study, two unfilled and three glass-filled polymer-based systems were in-
vestigated for their potential as value-added aggregate in concrete. It should be
kept in mind that although injection molding is widely deemed to be the ideal
process for the of waste, the use of scrap and leftover feedstock in ther-
reuse

moplastic injection molding is typically limited to 10-15%, depending on the

polymer and the application (Tushie et al., 1988). An increase in this percentage
generally results both in processing difficulties and in drastic reduction in per-
formance levels such as in impact.
A basic 1:2:4:4 mix (water: cement: sand: coarse aggregate) of cement con-
crete was prepared with sufficient water to ensure workability. In all, five
materials-of which three were glass-fiber-reinforced and two were neat
polymers-were used in injection molding pellet form as aggregate. Details are
given in Table 4. For each material set, 50.8 mm x 50.8 mm x 50.8 mm
&dquo; &dquo;
(2 x 2 x 2 &dquo;) compression cubes were cast, with aggregate being replaced
by the pellets at 12.5 %, 20 %, 25 %, 50 %, 75 % and 100 % volume. For each
series, a control set of concrete was also cast. In addition, scale beams of size
&dquo; &dquo;
330.2 mm x 25.4 mm x 25.4 mm (13&dquo; x 1 x I&dquo;) were cast at each of the
replacement ratios using the PET pellets only. Specimens were vibrated during
casting according to standard procedure and allowed to cure for two days in the
molds before their removal and placement in a tank of water. Specimens were
allowed to remain in the tank for total times of 7, 14 and 28 days after pouring.
Care was taken to ensure that all sets, including the controls, were exposed to the
same cure conditions.

EXPERIMENTAL PROCEDURE AND RESULTS

Compression tests were performed on the 50.8 mm x 50.8 mm x 50.8 mm

(2 &dquo; x 2 &dquo; x 2 &dquo;) cubes following the loading rates prescribed in ASTM C39-86,

Table 4. Details of pellets used.

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
 55

Figure 1. Relative effectiveness of different pellets.

Vol. 4.02 (150 psi/sec for the first half of loading and 30-35 psi/sec for the second
half). Figure 1 shows the relative effectiveness of using the various materials as
a function of replacement percentage on the 28-day compressive strength. In

Figure 1, the first column represents results obtained with polycarbonate/glass;

the last, the results obtained with PET, with the polypropylene/glass,
nylon/glass, and PEEK pellet results being shown in between, in that order. All
results were the average of at least 6 specimens; the scatter was within 5-10 % .
In no case was the scatter of the samples made with pellets greater than that of
the control concrete specimens. It can be seen from Figure 1 that specific
strength ratios greater than 1 can be obtained for polycarbonate/glass, poly-
propylene/glass, and PEEK at the 25, 20 and 50% replacement levels, respec-
tively. It should be noted that in each case there was a lack of formation of a good
transition zone between the pellets and the cement slurry, formation of which
would have resulted in higher levels of efficiency. Figures 2 and 3 show the com-
parison based on densities. It would appear that if the adhesion problem could be
overcome, the use of the composite and/or polymer waste could provide one way
to obtain a lower weight simultaneous with enhanced performance. The use of
polymer additives and fillers as described above is hypothesized to also increase
the chemical resistance of the concrete both to alkali reactions and to other en-
vironmentally induced degradation. This aspect is now being investigated and
will be reported elsewhere. In light of the problem related to the formation of the
interface, it is interesting to compare specific ratios as the concrete cures from
the 7-day to the 28-day level as in Table 5.

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
 Figure 2. Densities due to the use of glass-reinforced systems.

Figure 3. Denslties due to the use of unfilled (PEEK and PET) systems.

56

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
 57

Table 5. Specific strength ratios as a function of time.

From the experimental results and microscopic investigation, it is clear that as

the hydration progresses with time, the alite completes its reaction, and the CaO-
Si02-H20 fibrils form stronger bonds between the constituents of the control con-
crete. However, due to the inert surfaces of the pellets, few to no bonds were
formed. Preliminary tests on surfactants have shown that the use of an anionic
surfactant actually increases the creation of fibrillar structure from the pellets,
giving improved results. It should be noted that similar degradation was observed
by Watt and Xu (1991) in the use of ground scrap SMC. However, at the 28-day
level, the ratio of compressive strength of the sample with 10% SMC replace-
ment to the compressive strength of the control at the 28-day level was 0.8,
whereas results for three of the five materials used in this investigation at the
12.5 % level are higher, as shown in Table 6.
Smith (1986) had attempted to use polyethylene as 50% and 100% replacement
in a similar concrete mix (water, cement, aggregate ratio). It is illuminating to
compare his results of compressive strength (only 7-day cure strengths were re-
ported) with those of the fiber materials used in this investigation. The results in
Table 7 are given in terms of compressive strength ratios-i.e., the ratio of the
compressive strength of the specimen containing the pellets to that of the control.
It is clear that the systems used in the current investigation are significantly better
in terms of compressive strength characteristics. Also the three glass-fiber-
reinforced systems do not show degradation when the replacement level is dou-

Table 6. Compressive strengths

at the 28-day level (12.5%).

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
58

Table 7. Comparison of compressive strength ratios.

bled, making these systems attractive for use in the further development of light-
weight and enhanced-performance concrete products.
In addition to the compression cube tests, flexural tests were conducted on
specimens with PET using 330.2 mm x 25.4 mm x 25.4 mm (13&dquo;X
1 &dquo; x 1 &dquo;) beams. The beams were tested in three-point flexure at the 28-day
strength level; the results are given in Table 8. The structural efficiency for the
flexural specimens was computed from the ratios of the maximum stress levels
and the respective densities. Figure 4 shows the comparison of structural efficien-
cies in compression and flexure. It is clear that the use of the pellets without any
surface treatment does not add to the performance in compression. However,
there is a significant increase of almost 50 % in efficiency in flexure at the 75 %
replacement level. The maximum stress was computed as S 3PLI(2bdl), =

where P is the maximum load determined through testing, L is the support span,
and b and d are the width and depth of the beam, respectively. The results here
are quite encouraging, especially at the 75 % level, where there is not only an in-
crease in flexural capacity but, more importantly, a significant drop in weight.

Figure 5 depicts the plots of load versus cross-head displacement for the control
and 75 % replacement samples. It can be seen that the addition of the PET in-
creases both the load-carrying capacity and the ductility of the material. This

Table 8. Results of three-point flexure tests.

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
Figure 4. Structural efficiencies in compression and bending through the use of PET ag-
gregate.

Figure 5. Comparison of the 75% PET filled and control specimens in flexure.

59

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
60

promises to be an avenue of considerable potential for the use of scrap polymer

and/or composites in applications such as slabs, pavements, etc. The increase in
possible deformation before the onset of failure greatly adds to the performance
of concrete, enabling further ductility when reinforced with steel without the sud-
den formation of tension cracks. A gain in deformation capability for the entire
set of PET beams was seen as compared to the control, which is directly trans-
latable to improvements in toughness of the concrete.

DISCUSSION AND CONCLUSIONS

The rapidly changing environmental awareness, as well as the increasing costs
of landfilling polymers and composites, is making it impossible to deal with large
amounts of waste following traditional approaches. Simultaneously, there is a
growing need from the construction industry for the formulation of lower weight,
higher strength, chemically resistant concretes. The mechanical properties of
concretes have been seen to reflect the inhomogeneities in terms of large pores,
weak solid phases, and stress concentrations, due to both geometry and differing
moduli. There is considerable interest in enhancing the performance of concrete,
especially in light of the detrimental effects mentioned earlier and their combined
effects on the deterioration of the infrastructure.
There exists the possibility of simultaneously solving-at least partially-the
problems of waste disposal and concrete deterioration/low performance through
the use of composite and polymer waste as aggregate in concrete. Results of the
preliminary study reported herein are encouraging, especially in flexure. Based
on studies of the transition zone, it is apparent that the main challenge is to create
a strong bond between the composite/polymer waste used as aggregate and the
cement slurry. The use of plasticizers and anionic surfactants is expected to
decrease this problem. Research indicates that the use of materials such as waste
PEEK may increase the ductility and toughness of the concrete and may find
potential application not only for higher strength concretes but also in construc-
tion, where increased ductility is necessary to offset seismic damage due to
dynamic loading. It is of interest to note that in their recent development of the
Living Environments House, GE used a plastic concrete that was similar to con-
ventional concrete except that 30 % of the aggregate was pre-treated waste and
scrap (including recycled) plastic and composites. The flexural strength of the
resulting concrete was more than 25 % higher than conventional concrete, but it
was too expensive for current use (Wilkinson, 1990). The flexural properties
shown by the concrete in this study rival those reported, with no addition in ac-
tual cost, which emphasizes that concrete can ecologically isolate composites
while simultaneously providing a reuse method removed from the controversies
of landfill and incineration.

ACKNOWLEDGEMENTS
The authors gratefully acknowledge the University of Delaware Center for
Composite Materials University/Industry Research Consortium for the support
of Bryan Lennon’s graduate research program during the 1992-93 academic year.

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015
 61

REFERENCES
1985 "Guide to the Selection and Use of Hydraulic Cements," ACI 225R-85, American Concrete In-
stitute
Butler, K 1991. "Recycling of Molded SMC and BMC Materials," Proceedings of the 46th Annual
SPI Conference, Session 18-B, pp. 1-8.
Carreras, E 1992. Private communication.
Hudec, P. O. 1991. "Reduction of Alkali Reactivity and De-Icing Salt Damage in Concrete by Addi-
tions of Pyrolysed Sheet Molding Compound," Proceedings 7th Annual ASM/ESD Conference, De-
troit, pp 611-614
Jutte, R B. and W D Graham 1991 "Recycling SMC," Proceedings of the 46th Annual SPI Confer-
ence, Session 18-A, pp. 1-6.
Lea, F. M. 1971. Chemistry of Cement and Concrete, 3rd Edition
, Chemical Publishing
Mobasher, B and S P. Shah 1989. "Test Parameters for Evaluating Toughness of Glass Fiber Rein-
forced Concrete Panels," ACI Materials Journal
, 86(5) 448-458
McDermott, J S 1993 "Automotive Applications," Proceedings of the JTEC Workshop on Advanced
Manufacturing Technology for Polymer Composite Structures in Japan, February, 1993 , pp.
103-109.
Palmero, J. 1992 "Recycling Phenolics," Proceedings of the 8th Annual ASM/ESD Advanced Compos-
, November, pp. 253-260.
ites Conference, Chicago

Rathje, W. L. 1989 "Rubbish," The Atlantic Monthly (December):2.

Skalny, J. O , ed. 1987. "Concrete Durability A Multi-Billion Dollar Opportunity," NMAB-437, Na-
tional Materials Advisory Board, National Research Council.
SMC Automotive Alliance 1991 "Pyrolysis as a Means of Recycling Thermoset Composites," Pro-
ceedings of the 46th Annual SPI Conference, Session 18-D, pp. 1-2
Smith, B. 1986. "A Preliminary Report on an Ongoing Investigation into the Use of Plastics Refuse
and Scrap as a Replacement for Sand and/or Gravel in Portland Cement Mixtures," Proceedings of
, pp. 1465-1470.
ANTEC
Taylor, H. F. W. 1990. Cement Chemistry
. London, England: Academic Press
Thayer, A. M 1989. "Solid Waste Concerns Spur Plastic Recycling Efforts," C & EN, pp 7-15.
Tushie, D. R., G. A. Jensen, and N. F Beasley 1988 "Thermoplastic Injection Molding," in En-
gineered Materials Handbook, Vol 2, ASM International
, pp 309.
Watt, D. F. and J. Z Xu 1991 "On the Use of Pyrolysed SMC as a Concrete Additive," Proceedings
of the 7th Annual ASM/ESD Conference, pp 615-619.
Wilkinson, J. F. 1990. "Superior Materials Are in the Offing," ENR (October 4):33-36.

Downloaded from jtc.sagepub.com at MICHIGAN STATE UNIV LIBRARIES on February 25, 2015