Life Extention For Composite

2.
33
Life Cycle Engineering of
Composites
Y. LETERRIER
Ecole Polytechnique Federale de Lausanne, Switzerland
2.33.1 INTRODUCTION TO LIFE CYCLE ENGINEERING 2

2.33.1.1 Sustainable Resource Management 3
2.33.1.2 Loop Closing of Composite Materials 3
2.33.1.3 The Criteria and Analyses of Durability 4
2.33.1.3.1 Limiting factors to composite durability 4
2.33.1.3.2 Durability analyses of polymer composites 4
2.33.1.3.3 The life cycle approach to composite durability 5
2.33.1.3.4 Priorities in life cycle engineering 5
2.33.2 THE LIFE CYCLE OF POLYMER COMPOSITES 6
2.33.2.1 The Nature of Material Constituents 6
2.33.2.1.1 Polymer matrices 6
2.33.2.1.2 Fiber reinforcements 6
2.33.2.1.3 Interface 7
2.33.2.2 Brief Review of Aging and Degradation Phenomena 7
2.33.2.2.1 Process-induced degradation 7
2.33.2.2.2 Service-induced degradation 8
2.33.2.2.3 Viscoelasticity and aging during service 9
2.33.2.2.4 Coupling effects in durability analysis 10
2.33.2.3 Health Monitoring and Protective Measures 11
2.33.3 LIFE CYCLE ENGINEERING IN PRODUCT DEVELOPMENT 12
2.33.3.1 Ecoefficiency and Product Development 12
2.33.3.2 The Role of Design in the Life Cycle of Composites 12
2.33.3.2.1 Design for disassembly 12
2.33.3.2.2 Design for recycling 12
2.33.3.3 Reduction of Material Intensity 13
2.33.3.3.1 Weight reduction 13
2.33.3.3.2 Process and material integration 13
2.33.3.4 Life Extension of Composite Products 13
2.33.4 RECYCLING AND RECOVERY OF POLYMER COMPOSITES 14
2.33.4.1 Chemical Routes to Recycling 15
2.33.4.2 Mechanical Recycling and Quality Insurance 15
2.33.4.2.1 Thermoplastic composites 15
2.33.4.2.2 Thermoset composites 17
2.33.4.2.3 Fiber reinforcements 18
2.33.4.3 Incineration and Energy Recovery Routes 18
2.33.5 INTRODUCTION TO LIFE CYCLE ASSESSMENT OF COMPOSITES 18
2.33.5.1 What is Life Cycle Assessment? 18
2.33.5.1.1 Goal definition, scope, and functional unit 19
2.33.5.1.2 Inventory analysis 19
2.33.5.1.3 Impact assessment 19
2.33.5.1.4 Improvement analysis 19
1
2 Life Cycle Engineering of Composites
2.33.5.1.5 Key issues in life cycle assessment 19

2.33.5.1.6 Active and passive applications 19
2.33.5.2 Life Cycle Assessment of Recycling 20
2.33.5.3 Case Study of Components for Transportation Applications 20
2.33.5.3.1 Materials selection and functional unit 21
2.33.5.3.2 Energy and CO2 21
2.33.5.4 Case Study of Glass-fiber and Natural-fiber Reinforced Thermoplastics 23
2.33.5.4.1 Materials selection and functional unit 23
2.33.5.4.2 Impact assessment and sensitivity analysis 24
2.33.6 CLOSURE AND PERSPECTIVES 25
2.33.7 REFERENCES 26
2.33.1 INTRODUCTION TO LIFE CYCLE resources turnover, from cradle to cradle, as

ENGINEERING sketched in Figure 1. Much effort is never-
theless required to link product design to com-
For decades, the development of polymer posite science and technology, and to
composites has been driven almost exclusively environmental science: recyclable does not
by performance criteria such as high specific necessarily imply recycled, and recycled
stiffness. It is only in recent years that life does not necessarily imply environment-
cycle considerations have become prominent friendly. This work is, therefore, an attempt
features in the design of composite-based pro- to provide rational understanding of the key
ducts, with a gradual increase of recycling factors involved in such interplay.
efforts, and growing interest for durability ana- This section introduces the overall frame-
lyses. The issues of loop-closing, resource effi- work for life cycle engineering. It establishes
ciency, waste reduction, and life-extension are links to the underlying issue of sustainable
to be seen as many facets of the life-cycle en- resource management and emphasizes the
gineering concept, developed as an integrated need for durability analyses of composites. It
method to design, manufacture, use, and re- also defines the main routes towards loop-
cover materials and products for optimal closing and sets the main priorities in life cycle
Figure 1 Life cycle engineering addresses both resource efficiency and waste minimization, in order to
optimize resource intensity during the whole life cycle (adapted from Lundquist et al., 2000; APME, 1999).
Introduction to Life Cycle Engineering 3
Table 1 Material intensities (MI) of abiotic resources (i.e., nonrenewable) and water
needed to produce selected materials (extract from Wuppertal Institute database
Version 1.3c). The values do not include transport-related MI.
Material MI abiotic resources MI water

(t/t) (t/t)
Fiber-reinforced composite 2.91 49.1

Kaolin 3.05 2.50
E-glass fiber 6.22 94.5
Aramid fiber 37.0 940
Carbon fiber 61.1 2411.5
Polyethylene 5.40 64.9
PVC 8.02 118
Polyester thermoset 5.40 209
Epoxy resin 13.7 290
Aluminum (primary) 85.4 1380
Aluminum (secondary) 3.45 60.9
Steel 6.35 46.8
Diamond 5 260 000
Table 2 Markets for glass-fiber reinforced compo- 1988, Weizsacker et al., 1997, Gardner and
sites. Sampat, 1998). This imbalance is expressed as
the ratio between the amount of resources and
Application field Market sharesa Lifetime the weight of materials and products, thor-
(%) (years) oughly studied by the Wuppertal Institute and
termed material intensity (MI) (e.g., Schmidt-
Consumer goods 12 110
Electrical industry 19 550 Bleek, 1993). Table 1 reports several MI values
Industrial equipment 20 550 for composite constituents, together with sev-
Transportation 21 10 eral other materials. It is evident that for all
Building 16 >30 materials, the MI values are by far greater than
Others 12 1, and are larger for raw materials such as fibers
or polymers than for semifinished products
Source: Bowen, 1994 such as fiber-reinforced composites. The in-
a
Total world market 1986: 10 Mtons; projected market 2000: 100 creasing economic and environmental costs of
Mtons.
this excessive direct or indirect use of materials
trigger a number of strategies to reduce both
engineering. The subsequent sections are orga- resource consumption and waste generation.
nized as follows: Section 2.33.2 reviews the Synthetic polymers represent a mere 4% of
influences of the life cycle on the durability of crude oil applications, and their composites are
polymer composites; Section 2.33.3 describes therefore based on nonrenewable resources. As
the main approaches for product design in the indicated in Table 2, the lifetime of various ap-
context of life cycle engineering; Section 2.33.4 plications for polymer composites ranges from a
describes state-of-the-art recycling processes for few years in the case of consumer goods, up to
polymer composites; Section 2.33.5 introduces over 50 years, particularly in the building sector.
the life cycle assessment methodology, with case In the competition with alternative low-weight
studies. Finally, Section 2.33.6 closes the var- materials with a clearer environmental strategy,
ious topics discussed in the preceding sections. not to say aluminum, life extension of nonre-
newable polymer composites has become a
major issue. The following highlights the rea-
sons for this need, and indicates routes towards
2.33.1.1 Sustainable Resource Management increased durability of the resources used to
manufacture polymer composites.
For centuries, human activities have grown
based on a linear economy, considering unlim-
ited resources and an infinite sink to absorb all 2.33.1.2 Loop Closing of Composite Materials
wastes. Worldwide efforts are underway to re-
duce the large imbalance in resource Besides dematerialization, loop closing of
productivity, in the global context of sustain- resources is one of the key criteria towards
able development (see, for instance, WCED, sustainability. The extent to which a resource
loop is closed depends on the respective dur- composite part is not accessible, one may dis-
ability of the material and the corresponding tinguish the following three main causes:
resource, and is attainable through: (i) in- (i) Aging and degradation of the material con-
creased durability, (ii) increased use of renew- stituents. These phenomena which lead,
able resources, and (iii) increased reuse of depending on the field of application, to struc-
products and recycling of materials (Lundquist tural or functional failure of the composite
et al., 1999a, 1999b). part, are described in Section 2.33.2. These
Which route, or combination thereof, would typically include premature failure of the pro-
provide the optimal solution in terms of sus- duct due for instance to excessive levels of
tainability, that is, for economic, technological, internal stresses.
and environmental criteria, is not always evi- (ii) Improper design and processing cycle.
dent. It often requires trade-offs, as we have This situation involves primarily drastic limita-
learned from examples in recent years. Increas- tions to part re-use as well as material recycling
ing the durability of a product could have resulting from the inherent complexity of the
adverse effects on developing novel products constituent assembly, and therefore difficulties
with lowered environmental burden: a typical in disassembly.
example is that of cars. Increasing the use of (iii) Product obsolescence. The third limiting
renewable resources might imply increasing the factor to composite durability finds its causes in
use of hazardous substances for cultivation and the rapid technological progress, mostly within
processing, and would considerably impede the the area of computer goods and telecommuni-
number of times the material can be recycled. cations. It further results from changing con-
Finally, increasing the recycling level of materi- sumer patterns, where a typical example is that
als goes along with well-recognized drawbacks, of sports goods which use more and more poly-
including the drop in quality of used materials, mer-based composite materials. This topic is
which imply, when recycling, an overdesign to beyond the scope of this chapter, and the reader
compensate for such a drop, with a clear eco- is referred to the works of, e.g., Giarini and
nomic implication. Stahel (1993), Lemer (1996), or Kimura et al.
(1998).
2.33.1.3 The Criteria and Analyses of

Durability
2.33.1.3.2 Durability analyses of polymer
Durability is a key concept for the develop- composites
ment of polymer composites, since uncertainties
Three main axes for durability analysis have
about long-term behavior of these materials
been identified to analyze and predict the long-
often translate into conservative design. There
term evolution of polymer composites under a
is, however, no general definition of durability,
complex interplay of mechanical, thermal, and
since it obviously depends on the application to
environmental factors. These were reviewed by
be used in an unknown future. Typically, it is in
Cardon (1996b), and extensively developed in
the case of aircraft structures, 12 000 h in a
several publications devoted to this topic (Car-
supersonic regime, under cyclic loads and tem-
don and Verchery, 1991; Wetherhold, 1994;
peratures up to 175 8C (Arnold-McKenna and
Cardon et al., 1996; Cardon, 1996a; Reifsnider
McKenna, 1993) or, in the case of composite
et al., 1998).
hulls for submersible intended for 6000 m depth,
(i) The reduced time approach promoted by
several years with pressure cycles beyond 600
Schapery (1969, 1996) allows extrapolations of
bars, in a marine environment (Davies et al.,
long-term response from short-term tests, using
1996). Similarly, flexible piping systems for off-
timetemperature, timeaging time, and other
shore applications are expected to resist to op-
timemoisture superposition principles. This
erating pressures of 690 bars, temperatures of
approach stems from a thermodynamic formu-
145 8C, depths exceeding 1500 m, and extremely
lation of nonlinear viscoelastic and viscoplastic
aggressive production fluids (Quigley et al.,
constitutive equations. It is used for instance to
1998).
model structural recovery and moisture effects
in high-performance composites (Brinson,
1991; Brinson and Gates, 1995).
2.33.1.3.1 Limiting factors to composite (ii) The damage mechanics approaches of
durability Talreja, Allen, Ladeveze, Tamusz, and Nairn,
to cite only a few (Talreja, 1985, 1994), relate
Although an exhaustive list of factors con- the composite stiffness reduction to the pro-
tributing to reaching the end of the life of a gressive development of microdefects such as
Introduction to Life Cycle Engineering 5
Figure 2 Schematics of the drop in durability of materials at each life cycle step.
matrix transverse cracking in laminates. The With this approach in mind, the objective of
literature is rich in works devoted to the mod- life cycle engineering may be seen as maintain-
eling of these ubiquitous phenomena, and most ing the durability of the constituent materials
refer to the notion of internal variables, in the shown in Figure 2 to the highest possible level
thermodynamic sense, to describe the state of during the whole life cycle.
damage.
(iii) The critical element approach intro-
duced by Reifsnider and co-workers (Reifsnider
and Stinchcomb, 1986; Reifsnider, 1991; Reifs- 2.33.1.3.4 Priorities in life cycle engineering
nider et al., 1996), where the failure of the
composite is controlled by that of a critical Life cycle engineering puts priority on pre-
representative volume affected by a defined vention principles, which should be activated in
failure mode, identified from laboratory tests. the early stages of the design process (Luttrop
This approach has been implemented into the and Zust, 1998). As shown in Figure 3, the top
MRLife computer code to predict the remain- priority in terms of resource sustainability is to
ing strength and life of polymer composites. substitute a service to a product, which has been
termed dematerialization (Wernick et al., 1996).
Examples of dematerialization range from low-
ering weight of containers or cars, for which
2.33.1.3.3 The life cycle approach to composite low-weight composite structures play a central
durability role, to substitution of paper by electronic for-
mats, although the influence of the latter on
Figure 2 sketches the influence of the life dematerialization is still unclear. Similarly, high
cycle steps on the durability of a material, priority is to be given to all life extension
such as any of the constituents of a polymer options, including maintenance, repair, and
composite. It is evident that the durability of reuse, providing that no alternative product or
the material drops at each individual step. The service with less impact on the environment can
three main factors leading to such a drop were be used.
introduced in the previous section. There is Recycling, including mechanical recycling
widespread agreement that insufficient know- and chemical recycling, brings the durability
ledge about aging and degradation mech- of the constituents back to a higher value. It is
anisms, and particularly about the coupling nevertheless a lower priority option, particu-
between phenomena, is a central concern in larly when it requires larger material and energy
durability prediction of polymer composites. inputs compared to the preceding life extension
Improved processing cycles and understanding alternatives. Finally, feedstock recycling, where
of the long-term behavior of this class of the polymer constituent is recovered back into
materials would translate into less overdesign, fuel-like products, and energy recovery, are to
minimized maintenance efforts, and extended be considered as low-value alternatives. It
lifetime. Besides, improvements in design, should, however, be made clear at this point
material selection, and assembly practices that which recycling or recovery alternative, or
would benefit from incentives to recover combination thereof, will provide the optimal
individual parts in complex assemblies at all environmental benefit has to be evaluated. This
stages of the life cycle of the composite. topic will be addressed in Section 2.33.5.
Figure 3 Priorities in life cycle engineering.
According to this hierarchy, incineration towards equilibrium of amorphous glassy poly-

without energy recovery and dumping into mers translates into additional time-dependent
landfill are not considered as viable alternatives effects termed physical aging (Struik, 1978;
to resource management, as these bring the Hutchinson, 1995). These three key character-
durability of the resource to zero. istics of polymer materials with associated phe-
nomenology are summarized in Table 3.
2.33.2 THE LIFE CYCLE OF POLYMER

COMPOSITES 2.33.2.1.2 Fiber reinforcements
Most of the fibers used to reinforce polymer
2.33.2.1 The Nature of Material Constituents matrices, including glass, boron, and carbon,
The following summarizes the features of the are brittle, their mechanical strength being lim-
constituents of polymer composites relevant to ited by surface flaws. Fiber attrition in viscous
the influence of the life cycle on their durability. polymer melts during extrusion compounding,
and fiber/fiber wear, particularly in textile
technology, are typical concerns. As brittle
2.33.2.1.1 Polymer matrices materials, the strength of fiber filaments is
defect-controlled and as such, is dependent on
Polymers are organic materials. As such, they the length of the fiber. Probability distributions
tend to degrade under thermomechanical loads, accounting for surface flaw dependent strength
and degrade even more in the presence of oxy- have traditionally been associated with the Wei-
gen, moisture, and radiation such as ultraviolet, bull function (Weibull, 1951). It was used ex-
to which they are generally poor barriers tensively to derive the strength of carbon and
(Brown, 1993; Clough et al., 1996). Biodegra- glass fibers tested at various gauge lengths
dation of polymers is a further topic related to (Asloun et al., 1989; Padgett et al., 1995; Dibe-
the life cycle of organic materials, which none- nedetto et al., 1997; Tagawa and Miyata, 1997;
theless is beyond the scope of the present work, Wang and Xia, 1997), or indirectly, using single-
and the reader is referred to the compilations of fiber composite (Curtin, 1994; Goda et al.,
Lenz (1993) and Albertsson and Huang (1995). 1995) or acoustic emission (Okoroafor and
Polymers are also macromolecular assemblies, Hill, 1995; Clough and McDonough, 1996).
characterized by unique time-dependent prop- Besides being brittle, glass fibers are also sus-
erties, resulting in a variety of so-called viscoe- ceptible to hydrolysis, which affects their
lastic phenomena including creep and lack of mechanical strength (Thomas, 1960; Aslanova,
dimensional stability (Aklonis et al., 1972; 1985; Bansal and Doremus, 1986; German and
Ferry, 1980; Christensen, 1982). Moreover, Yannacopoulos, 1997; Vauthier et al., 1998), as
polymers are seldom in thermodynamic equil- shown, for instance, in Figure 4. Similarly ara-
ibrium. Crystalline structures frozen-in during mid fibers are sensitive to moisture with
the cooling stage of a processing cycle may reported creep rate increase (Dillard et al.,
evolve towards higher crystallinity, particularly 1991). Particular mention should finally be
in the presence of plastification agents such made of the case of lignocellulosic fibers
as moisture. Besides, the slow recovery back which, by contrast with synthetic fibers, are
The Life Cycle of Polymer Composites 7
Table 3 Factors contributing to aging and degradation of polymer matrices.
Nature of polymers Aging and degradation factors Phenomenology
(i) Organic matter . Temperature (pyrolysis) . Molecular scission

. O2 (oxidation) . Yellowing, embrittlement
. Radiation, incl. UV (oxidation) . Discoloration, embrittlement
. Solvents, incl. H2O (solvolysis) . Plastification
. Biodegradation . Enzymatic/bacterial action
. Mechanical load; melt state . Extensional degradation;
Shear and viscous heating
(ii) Macromolecular . Sorption of gases and liquids . Swelling and drop in Tg
organization
. Mechanical load; solid state . Yield, fatigue failure
. Time, temperature, stress . Viscoelasticity (creep, lack of
dimensional stability)
(iii) Nonequilibrium . Time and temperature . Cross-linking of network;
state Recrystallization
. Time, temperature, stress . Structural recovery and physical
aging
Figure 4 Variation of percentage tensile strength of pristine glass with exposure time at 0 (black dots) and
100% (white dots) relative humidities (reproduced by permission of the Society of Glass Technology from
Phys. Chem. Glasses, 1960, 1, 418).
particularly moisture- and temperature-sensi- 2.33.2.2 Brief Review of Aging and

tive (Bledzki et al., 1998). Degradation Phenomena
Process-induced degradation (i.e., high tem-
perature) and service-induced degradation (i.e.,
2.33.2.1.3 Interface low temperature) are treated in separate sec-
There is no need to remind the reader about tions in the following, although several features
the key role played by fillermatrix interfaces are common to both phenomena. As was illu-
and plyply interfaces on composite perfor- strated in Figure 2, it is also important to stress
mance, through their stress transfer capability, that the latter phenomena are greatly influ-
as detailed in several publications (Ishida, 1990; enced by the former, which becomes obvious
Gorbatkina, 1992; Akovali, 1993; Kim and in the case of closed-loop recycling.
Mai, 1998). Only few studies, however, have
specifically addressed the relation between the
type of interactions, the internal stress state, and 2.33.2.2.1 Process-induced degradation
the degradation processes germane to the inter-
facial region (e.g., Morii et al., 1991; Meyer Matrix degradation and fiber attrition are
et al., 1994; Bradley and Grant, 1995; Eriksson the two main causes responsible for degrada-
et al., 1996a; Tsotsis and Lee, 1998), by contrast tion of polymer composites during a processing
with ceramic matrix composites or metaloxide operation. On the one hand, all commercial
interfaces. polymer matrices are protected with antioxi-
dant additives, as the dominant polymer degra- thermosetting and thermoplastic composites
dation mechanism is the thermally activated during long-term environmental exposure, as
oxidative degradation (Zweifel, 1998), in concluded by Parvatareddy et al. (1995). Addi-
which the action of oxygen at high tempera- tional information can be found in the review of
tures leads, depending on the polymer type, to a Tant et al. (1995), devoted to the high tempera-
decrease of molecular weight and/or cross- ture properties and applications of polymers
linking. Viscous or adiabatic heating of the and polymer composites.
polymer melt, due to the combination of intense Sorption of small penetrants by the polymer
shear rates and low thermal conductivity, matrix, particularly water, often plasticize or
further contribute to such degradation phe- swell and induce microcracks in the polymer. It
nomena. Other chemical degradation processes may also damage the interface through osmotic
involve thermal degradation and solvolysis re- pressure effects and eventually degrade the fiber
actions such as hydrolysis, which is a main reinforcement, for instance, through hydrolysis
concern in the processing of natural fiber com- of glass. Mensitieri et al. (1995) and Weitsman
posites, as reviewed by Bledzki et al. (1998) in (1998) have reviewed the salient features of
the case of thermoplastics reinforced with wood moisture and solvent sorption in polymer ma-
fillers. Besides, mechanical degradation of the trices, particularly epoxy, polyester, and PEEK.
polymer may occur in particularly severe elon- Chemical resistance of glass fibers is well docu-
gational fields which provoke unfolding and mented (Bansal and Doremus, 1986) and is
scission of the macromolecules. largely dependent on their composition. For
On the other hand, fiber attrition is a central instance, Ghosh and Bose (1995) investigated
issue in processes involving shear flow of highly the higher hygrothermal resistance of N-glass
viscous polymers, typical of thermoplastic ex- fibers compared to E-glass fibers, in spite of the
trusion compounding and molding techniques. lower mechanical strength of the former.
It is the consequence of the limited bending Schutte (1994) reviewed the various character-
strength of the fibers, as was studied for exam- istics of moisture degradation of polymer com-
ple by Mittal et al. (1988), Wolf (1994), Ramani posites. Further information is found in the
et al. (1995), and Eriksson et al. (1996b), as a works of Selzer and Friedrich (1995) and Vau-
result of multiple reprocessing. thier et al. (1998), as well as in the compilation
of Chiang and McKenna (1996), and in the
studies of the effects of non-Fickian water dif-
2.33.2.2.2 Service-induced degradation fusion in fiber-reinforced composites of Cai and
Weitsman (1994), to cite only a few. Due to the
Similarly to the high-temperature regime re- considerable development of this class of mate-
levant to most processing operations, thermo- rials for structural marine applications, the spe-
oxidation is a key feature responsible for cific role of seawater has also been extensively
service-induced degradation of polymer com- studied, for instance, by Bradley and Grant
posites. Seferis and co-workers have investi- (1995) and Davies et al. (1998).
gated the degradation processes of this class Coupling and sizing agents were correlatively
of materials through weight loss measurements developed to improve interfacial adhesion and
taking into account their inherent anisotropy durability, as studied by Fraser et al. (1975).
and heterogeneity (Hayes and Seferis, 1996; The influence of the chemistry and morphology
Salin and Seferis, 1996). Tsotsis (1995) and of coupling agents on glass fibers on the dur-
Tsotsis and Lee (1998) report comprehensive ability of the interfacial region was reviewed by
analyses of the thermo-oxidative degradation Schutte (1994). It was analyzed by McKnight
of carbon-fiber reinforced epoxy composites, and Gillespie (1997) in the case of glass fibers,
which demonstrate the respective importance by Helmer et al. (1995) in the case of carbon
of matrix and interface degradation, matrix fibers, and by Bledzki et al. (1998) and Gauthier
toughness, ply interaction, and edge effects. et al. (1998) in the case of natural fillers. Alter-
Correa et al. (1996) found that the thermal native surface treatments have been developed,
resistance of aramid fiber reinforced compo- such as electrochemical, ozone, and cryogenic
sites was greater than that of carbon fiber re- fiber modifications studied by Rashkovan and
inforced composites or the pure matrix Korabelnikov (1997), using the single-fiber
polymer, due to improved interfacial interac- composite adhesion test to determine their
tions. Furthermore, environmental aging com- efficiency. The relation between the strength
bines the action of oxygen in the air, light, of individual filaments and that of the rein-
moisture and temperature, and, possibly, me- forced composite has further motivated a
chanical loads. The action of oxygen appears to large body of research. Recent works on that
be the dominant factor in the evolution of the topic include studies of Phoenix et al. (1997),
mechanical response of both fiber-reinforced devoted to statistical analysis of the strength of
Figure 5 Schematics of the shift of the viscoelastic relaxation time spectrum during aging time.
unidirectional composites, and of Curtin and characterized by a distribution of relaxation

Takeda (1998) and Shikula (1998). times, back towards equilibrium, has been
The issue of biodegradation of composites is termed structural recovery and extensively stu-
beyond the scope of this chapter, but one may died in the case of polymers since the late
cite the work of Gatenholm et al. (1992) and 1950s (Kovacs, 1958, 1963). The consequences
Gatenholm and Mathiasson (1994) who have of the recovery phenomenon can be found in
for instance processed biocomposites based on the evolution of mechanical, electrical (Li and
cellulose and biodegradable polymers, particu- Unsworth, 1994), and optical properties, and,
larly bacteria-produced polyester copolymers in general, in any property which is a function
(polyhydroxyhutyrate-hydroxyvalerate, PHB- of molecular mobility. Practically, an increase
HV) reinforced with wood cellulose. An excel- in the Young's modulus and yield stress or a
lent dispersion of cellulose fibers was achieved decrease in the creep rate have been reported
in the PHB matrix compared with such syn- as a result of structural recovery. Such time-
thetic matrices as polystyrene or polypropylene. dependent evolution of properties came to be
coined physical aging and was extensively stu-
died by Struik (1978) in the case of amorphous
2.33.2.2.3 Viscoelasticity and aging during and semicrystalline polymers and other glassy
service materials.
To our knowledge, Kong (1981) was the first
The time dependence of polymer composites to report investigations about the physical
has received increasing attention in the 1990s aging of polymer composites, with studies of
(e.g., Tuttle et al., 1995) (see Chapter 2.10, this the long-term behavior of epoxy/carbon lami-
volume). Particularly, their nonlinear viscoe- nates. In the 1990s, significant efforts were
lastic behavior has been modeled based on devoted to in-depth analyses of the phenomena,
Schapery's hereditary integral (Schapery, in a large variety of thermoset and thermoplas-
1969, 1996), whereas nonlinear viscoplastic tic-reinforced materials (e.g., Ma et al., 1990;
effects were treated using for instance Zapas Haidar and Vidal, 1996; Maddox and Gillham,
and Crissman (1984) derivations, both consti- 1997). Modeling of the evolution of the viscoe-
tutive formulations being implemented in clas- lastic behavior of these materials was proposed
sical lamination theory to characterize the by Sullivan (1990) and Sullivan et al. (1993)
response of laminated composites. Viscoelasti- using an effective time theory, which provided
city is described by a relaxation spectrum good agreement with a large variety of compo-
which is likely to evolve throughout the life site systems and, more recently, by Leterrier
of the composite, as a result of the various and co-workers, accounting for internal stresses
phenomena described above, similarly to what (Wyser, 1997; Leterrier et al., 1999). Interest-
is depicted in Figure 5. ingly, Armistead and Snow (1995) found no
Upon cooling from above the glass tran- evidence of aging upon adhesion properties in
sition temperature to below it, which is the model composites, besides the effects of inter-
case of most processing operations, amor- nal stresses. This result finds additional support
phous polymers depart from thermodynamic in the studies of Mendels et al. (1999a, 1999b).
equilibrium. The slow evolution of the none- These authors demonstrate that change in ad-
quilibrium state of the viscoelastic material, hesion is entirely attributed to the change in the
Figure 6 Evolution of the isochronous interfacial shear strength between a glass fiber and an epoxy matrix
after aging at Tg 7 5 8C. Three different models are compared, as indicated on the graph. The most accurate
model couples the thermoviscoelastic relaxation of internal stresses to the structural recovery of the polymer
matrix (after Mendels et al., 1999b).
internal stress state resulting from the aging 2.33.2.2.4 Coupling effects in durability
process, as shown in Figure 6 in the case of a analysis
glass fiberepoxy interface, aged below the
glass transition temperature of the polymer According to a survey made after several
matrix. years of expertise on damage composite parts
Several authors have refined the modeling by the French Technical Center for the
efforts by combining effective time theories Mechanical Engineering Industries (CETIM),
together with classical laminate theory, includ- 41% of failures in composite materials during
ing Brinson, Gates, and co-workers (Brinson, service that were not attributed to manufactur-
1991; Brinson and Gates, 1995; Bradshaw and ing defects result from coupled processes.
Brinson, 1997a, 1997b; Gates et al., 1997; Mon- Figure 7 summarizes the various causes for
aghan et al., 1994; Veazie and Gates, 1997) and failure, as reviewed by Perreux (1999) from a
Dillard and co-workers (Wang et al., 1995; survey of the French Association for Compo-
Parvatareddy et al., 1995, 1998; Pasricha et al., site Materials (AMAC). By definition, coupling
1997). The latter researchers have also ac- of phenomena occurs when the overall compo-
counted for oxidative degradation processes in site aging cannot be determined from the sum
adhesive joints. Similarly, Mijovic (1985) had of individual processes resulting from the var-
examined the coupling between physical and ious aging mechanisms taken separately. A
chemical aging in epoxy/carbon composites, typical coupling situation arises when a struc-
and numerical analyses were recently per- ture degraded under an oxidative atmosphere is
formed by Huang (1998). A summary of the simultaneously loaded in fatigue: the mechan-
theoretical developments relevant to the above- ical load induces further damage in the mate-
mentioned phenomena can be found in the rial, which, in turn, facilitates the diffusion of
work of Chow (1996). oxygen, hence, accelerates the degradation.
It is evident that the numerous degradation Coupled phenomena systematically accelerate
and aging processes described above, with their damage of the composite material, and their
own timescales, all act together in complex analysis requires investigation of the character-
interplay. This remark calls for a need to ana- istic timescales of the various aging factors
lyze coupling effects between these different acting altogether. It should be pointed out
factors. that the effect of temperature, at the exception
Figure 7 Statistics of composite failure, related to environmental causes (a) and life cycle causes (b) (after
Perreux, 1999).
of any change in the material state such as work based training introduced by Luo and
additional cross-linking for example, is to accel- Hanagud (1997) for real-time flaw detection.
erate the aging processes, and, as such, is not A variety of advanced structural health mon-
considered as a factor of coupling. Neverthe- itoring techniques for composites have been
less, the presence of thermal transitions in poly- reported. These include the use of active carbon
mers, together with the multiplicity of processes tows (Tamiatto et al., 1998), piezoelectric trans-
with different activation energies, render accu- ducers developed by Moulin et al. (1997) and
rate analysis of the acceleration effect of tem- Lichtenwalner et al. (1997), and wafer thin
perature very difficult. A comprehensive microsensors used initially to characterize in
analysis of coupled phenomena appears to be situ the processing state of polymers (Kran-
presently out of reach, and much research buehl et al., 1996).
efforts are still needed. As an alternative, Protection against aging and degradation of
several protective measures are being devel- polymer composites has traditionally been as-
oped, which are summarized in the following. sociated on the one hand with protection of the
composite constituents, and, on the other, with
the use of protective coatings. The former deals
mainly with stabilization of the polymer matrix
2.33.2.3 Health Monitoring and Protective and the development of tougher fibers, includ-
Measures ing specific sizing agents to protect the fiber
reinforcement. The latter are essentially paints,
Besides the theoretical analyses of the dur- which, as will be addressed in Section 2.33.4,
ability of polymer composites, efforts are direc- may be detrimental to the quality of the re-
ted towards health monitoring and protective ground material. Hard coatings find consider-
measures. The former involve embedded health able interest in tribological applications. They
sensors and self-monitoring of the composite, are also used as barrier layers to protect
otherwise termed intrinsically smart materi- carboncarbon composites from oxidation
als, through the continuous measurement of under extreme temperatures. Similarly,
electrical resistance which is a function of struc- although to a far lesser extent, oxygen and
tural damage, as reviewed by Chung (1998). moisture barrier coatings have been employed
According to Kranbuehl et al. (1996), em- to protect polymer composites. To prevent
bedded devices not only offer the capability to thermo-oxidative degradation, protective coat-
allow in situ measurements, but are also sound ings resistant to high-temperature and based on
alternatives to aging models, which lack relia- vapor deposition techniques have been success-
bility as they should predict an uncertain fu- fully developed and analyzed by Harding et al.
ture. In that sense, health sensors keep (1994) and Miller and Gulino (1994). Accord-
predictions on track. Recent developments in ing to Wyser (1997) and Wyser et al. (in press),
this direction include sophisticated neural-net- such thin coatings might further present the
advantage not to limit the recycling potential of product life extension, to ease maintenance and
the composite. repair operations, and also for material recov-
ery into useful applications, and turns out to be
a key challenge in the life cycle design of com-
plex products such as composites. Typical
2.33.3 LIFE CYCLE ENGINEERING IN guidelines stress common sense issues to
PRODUCT DEVELOPMENT ease the disassembly operation, by providing
easy access to assembly points and easy identi-
2.33.3.1 Ecoefficiency and Product fication of the type of material. Using fewer
Development dissimilar materials, and fewer subassemblies,
Ecoefficiency is, simply put, about producing benefits to both material recovery rate by in-
more with less resources and less pollution, and creasing material capture, and recovery eco-
for more insight, the reader is referred to work nomics, by decreasing disassembly time. In
of Fiksel (1994) and to the publications of the this sense, design for disassembly complies
World Business Council on Sustainable Devel- with design for assembly practices going for
opment (WBCSD, 1995). Life cycle design tools product simplification, which, in turn, is in
allow the linking of traditional design practices favor of improved reliability. In the case of
with environmental issues by showing what the plastic products, design guidelines often target
environmental issues are and the priorities that metal inserts, clamps, and screws, which should
need to be addressed. A considerable amount of be built to be easily separable, or even avoided
computer-aided tools are available to reduce and replaced by snap-fit systems. Similarly,
the environmental impact of a product, from Tome et al. (1999) propose substituting metallic
cradle to grave, some of which were compared inserts by local fiber-reinforcement areas. Inte-
by Hertwich et al. (1997). These tools encom- gration of such functions calls for novel proces-
pass design for recycling, design for disassem- sing approaches to composite manufacture,
bly, design for remanufacture, or design for which will be briefly addressed in a later section.
energy efficiency, and obviously make large
use of life cycle assessment methods. They
also consider waste minimization, including ha-
zardous waste, and compliance with regulations 2.33.3.2.2 Design for recycling
and standards. Initial efforts were mostly end-
of-pipe approaches to help designers avoiding Design for recycling targets the same features
waste and toxic substances. By contrast, in as design for disassembly. It addresses more
recent years, activities orient more and more specifically the selection of materials and sets
towards optimizing the product within sustain- their recycling rate. It further points out the
able boundaries (White, 1994). need to form recycled materials into new pro-
ducts. Particularly, fewer dissimilar materials in
assemblies, or in subassemblies of products de-
signed for disassembly, will improve the possi-
2.33.3.2 The Role of Design in the Life Cycle of bilities of material life extension. The German
Composites association Verein Deutscher Ingenieure
(VDI) has developed design for recycling guide-
The development of integrated components lines, classified into three distinct stages of re-
such as composite parts in light of the life cycle cycling: recycling during production, during
engineering concept should consider the var- use, and after use (Dowie and Simon, 1995;
ious topics discussed in the preceding sections, see also the standard VDI2243, VDI, 1993).
particularly issues of material reduction and life The all-PP (PP, polypropylene) dashboard
extension of products. This section emphasizes promoted by automotive tier-suppliers is an
the importance of accounting for composite innovative concept described by Braunmiller
durability and reliability in design strategies. et al. (1999) to develop a recycling friendly
Examples of existing design methodologies complex composite product. The structure of
such as design for disassembly and design for the instrument panel comprises a PP foam,
recycling and products and processes designed sandwiched in between a glass-mat reinforced
with these issues in mind are given. PP frame (GMT) and a TPO-PP/EPDM dec-
orative foil. This close-to monomaterial solu-
tion contrasts with the classical dashboard
2.33.3.2.1 Design for disassembly structure, including a metallic or GMT frame,
a polyurethane foam, and an ABS/PVC or
Disassembly of multimaterial products into similar vinyl foil. Designed for recycling, the
monomaterial constituents is a prerequisite for PP-based structure does not require costly
Life Cycle Engineering in Product Development 13
separation of the three main layers. Great ef- polymer composite parts (Bourban et al.,
forts are nevertheless needed to develop effi- 1998, 1999), and, from a life cycle perspective,
cient closed-loop recycling of this class of would also be beneficial for material recovery
materials, as will be dealt with in Section 2.33.4. purposes.
2.33.3.3 Reduction of Material Intensity

2.33.3.4 Life Extension of Composite Products
2.33.3.3.1 Weight reduction
Before considering end-of-life treatments de-
In many instances, ecoefficiency is reached veloped to extend the life of material constitu-
when using lightweight materials such as alu- ents, life extension of composite products
minum and polymer composites. The latter, should have a high priority in the design pro-
with unique specific stiffness and strength cess, as was illustrated in Figure 3. This in
(ASM, 1987; Tsoumis, 1991), are particularly practice implies fast and cost-effective mainte-
efficient in environmentally-active applications, nance and repair operations, based on design
such as transportation. An example of this is for assembly and disassembly approaches.
found in the case of the environmentally-aware Specific computer-aided design tools have
design of the Copenhagen S-train, developed in emerged to incorporate issues of life extension
the 1990s by the Danish Railway (DSB) where into the traditional development of composites.
the reduction of the weight was the main con- Russell et al. (1998) have, for example, simu-
cern. In comparison with the generation of S- lated the manufacture of filament-wound com-
trains from 1986, the weight per seat has been posites to provide complete material balance to
reduced by 46%, due to a large extent to the use design engineers. Extensive use is also made of
of light materials. computer-based techniques for stress analysis
of composite assemblies including strength and
life prediction (Reifsnider et al., 1996), and an
2.33.3.3.2 Process and material integration example for laminates specifically designed for
aircrafts can be found in the study of Madenci
Composite laminates are widely used as fa- et al. (1998). In the field of construction engi-
cing materials in structural sandwich applica- neering, there have been an increasing number
tions, in which they are bound to a low-density of developments where the design of composite
core, such as a foam or a honeycomb material. structures emphasized durability rather than
The benefits of such material integration is only mechanical criteria such as strength and
obvious, including weight savings, despite stiffness (e.g., studies of Meatto and Pilpel,
main drawbacks related for instance to the 1998, Iskander and Hassan, 1998, and Ishai
repair of the sandwich, and to the recovery of and Lifshitz, 1999). The same applies for mar-
the different constituents. The example of the ine applications, where composite technology is
traditional sandwich structure reveals the key claimed to offer significant life cycle cost sav-
trade-off between increased functional integra- ings thanks to reduced maintenance (Bhasin
tion which goes along with multimaterial inte- et al., 1998). However, according to Mouring
gration, and increased recycling potential (1998), design and analysis, fabrication, envir-
which, on the contrary, requires single-material onmental effects, repair, and joining are still
products. weak points in the further development of com-
Innovative technologies have emerged to re- posites in this field. In aircraft applications,
solve to a certain extent this trade-off in the case issues of maintenance and repair of structural
of thermoplastic composites. This class of ma- composites motivate considerable efforts. Cole
terials include neat and short-fiber reinforced (1998) has summarized the main achievements,
grades developed for injection molding pro- resulting from the creation of the Commercial
cesses, as well as continuous fiber reinforced Aircraft Composite Repair Committee in 1991,
composites processed by compression molding to establish an international forum to standar-
or autoclave bagging operations. The former dize various aspects of operating commercial
possesses high design freedom, but limited stiff- aircraft with composite components. Along si-
ness, which is opposite to the latter. Wakeman milar lines, several projects to ease maintenance
et al. (1999a, 1999b) developed methods for operations with diagnostic techniques have
process integration of flexible, semiconsoli- emerged, for instance the scanning laser Dop-
dated fiber tows with high stiffness into a neat pler vibrometer method of Castellini and To-
polymer substrate part. Combination of pro- masini (1998) or the laser-ultrasonic technique
cess integration and material integration has of Monchalin et al. (1998) used to inspect ad-
proven to be a cost-effective technology for vanced aircraft made of composite materials.
Figure 8 Recycling technologies (adapted from Lundquist et al., 2000).
In the field of repair, Lopata et al. (1998) composites. This class of materials, particu-
have investigated alternative routes for compo- larly those based on thermosetting matrices, is
sites such as traditional thermal cure or electron often considered not to be recyclable, and, con-
beam processing, and established the relevance sequently, should be phased out in favor of
of the latter technique. Polymer composites homogeneous materials. Such a statement
have also proven to be useful as patches to tends to ignore the overall life cycle environ-
reinforce damaged metallic aircraft structures, mental impacts as will be addressed in the next
as detailed by Rastogi et al. (1998). Reuse and section, but nevertheless explains to a certain
remanufacturing are additional routes to ex- extent the gradual replacement of thermoset
tend the life of products or their components composites by thermoplastic composites, be-
(Guide et al., 1997; Parker, 1997), particularly sides other advantages such as reduced process
in the case of environmentally passive applica- and storage costs. The main sources of polymer
tions, as detailed in Section 2.33.5. Material life composites in the waste stream are from the
extension through recycling is treated in the electric and electronic (E&E) industry, includ-
following section. ing the consumer market such as household
To be implemented successfully in an indus- electrical equipment and the automotive indus-
trial context, the technical and design ap- try which has become a clear target in the past
proaches to the life cycle of composites few years. The autoshredder residue (ASR)
discussed above, or, more generally, resource contains, for instance, about one-third of syn-
and waste management issues, should be envi- thetic materials (Disler and Keller, 1997). In all
saged in a broad framework of organizational these fields, the waste composites possess inter-
changes, where strategic, economic, and envir- esting economic value for recycling, and current
onmental factors strongly interfere. Towards efforts to recover this value are detailed as
this end, Environmental Management Systems follows.
(EMS) have emerged, and have already been Three main recycling techniques are available
implemented in a number of large-scale com- for polymers and their composites: (i) recovery
panies. The topic of EMS goes beyond the of materials by chemical processes, (ii) incor-
scope of this chapter, and the reader is referred poration of regrind during compounding, and
to general texts, such as that published by the (iii) energy recovery through incineration.
World Industry Council for the Environment Figure 8 summarizes the various recycling
(WICE, 1994). routes developed for plastics (Ehrig, 1992;
Cornell, 1995); the specific processes and lim-
itations relevant for composites are developed
2.33.4 RECYCLING AND RECOVERY OF in the following. It is obvious that, besides
POLYMER COMPOSITES technical requirements, the success of recycling
also depends on initial design, logistics of col-
To paraphrase Nadis and McKenzie (1993), lection, and eventually on the market for the
one may say the recycling problem in a word: secondary application.
Recycling and Recovery of Polymer Composites 15
2.33.4.1 Chemical Routes to Recycling 2.33.4.2 Mechanical Recycling and Quality

Insurance
Chemical recycling, which includes feed-
stock recycling, is essentially applied to the Mechanical recycling of polymers and poly-
polymer fraction, and can be broken down mer-based composites is in constant progress,
into four classes (Reinink, 1993; Wanjek and driven by tight legislation in the field of waste
Stabel, 1994): (i) solvolysis, (ii) oxidative pro- treatment. However, a systematic drop in qual-
cesses, (iii) pyrolysis and similar thermal de- ity occurs as a result of the reprocessing opera-
composition processes, and (iv) reductive tion. Quality assessment of the recycled
processes. Solvolysis is a generic term which material thus requires thorough analyses of
includes glycolysis, methanolysis, alcoholysis, its durability and reliability. Efforts in this
ammonolysis, and hydrolysis, as it involves direction are reported in the following, in the
reactions with the corresponding solvents. case of thermoplastic and thermoset matrix
The solvolysis process is used mainly to depo- composites.
lymerize condensation-type polymers such as
PET, PA, PMMA, and PC, plus a few addi-
tion-type polymers such as polyurethanes, 2.33.4.2.1 Thermoplastic composites
back into oligomers and original monomers,
which, subsequently, can be repolymerized Limiting factors to the performance of re-
into virgin materials. Addition-type polymers cycled thermoplastic composites are essentially
including polyolefins can be treated according related to process-induced matrix degradation
to the three other processes. Specific achieve- and fiber attrition, and the subsequent service-
ments concern for instance recycling of auto- induced degradation and aging of the polymer
motive shredder residues, for which Abrams matrix that has undergone several process cy-
et al. (1997) present a catalytic extraction pro- cles (see Chapter 2.25, this volume). Additional
cess to produce gas for electricity generation performance drop could result from contami-
and inert oxides that can be incorporated with nation by, for example, fragments of cross-
construction materials. Since methanolysis or linked paint coating or incompatible polymer
glycolysis of PET has been developed, Rebeiz fractions. As a tool for quality assessment,
et al. (1993a, 1993b) have studied PET recy- which is crucial to the market acceptance of
cling in composites. Similarly, Aslan et al. recycled materials, modeling efforts have arisen
(1997) have reacted products resulting from with the aim of predicting the properties of
the glycolysis of PET used in soft drink bottles mixtures of virgin and reprocessed fiber-rein-
with mixtures of saturated and unsaturated forced polymers (e.g., Bernardo et al., 1993,
acids yielding unsaturated polyester suitable 1996; Throne, 1987). Parametric studies of Ber-
as a matrix for fiber-reinforced composites, nardo et al. (1996) indicate for instance that, for
with toughness improvement. Efforts have glass-fiber-reinforced thermoplastics, the data
been directed by Patel et al. (1993) towards on the degradation of fiber lengths and me-
recycling of sheet molding compounds (SMC) chanical properties help understanding of the
through solvent extraction, hydrolysis, and effect of reprocessing on the fibermatrix inter-
pyrolysis. The latter process yields oily organic action. Most of the research and development
residues potentially interesting as nonreactive of recycled thermoplastic composites examine
extenders for epoxies and inorganic residues to specific cases, as reported in the following.
be used as fillers in a variety of polymer Recycling of glass-fiber reinforced polyamide
systems. Innovative studies examine reversible developed for a car air intake manifold, radia-
cross-linked networks, such as epoxies and tor end-caps, and similar under-the-bonnet ap-
unsaturated polyesters, which would be appro- plications has particularly motivated research
priate for recovery purposes (Sastri and Te- efforts in recent years. Dzeskiewicz et al. (1993)
soro, 1990; Tesoro and Sastri, 1990). Simon examined the recycling potential of glass fiber
and Kaminsky (1998) have recycled produc- reinforced polyamides, and measured a sys-
tion wastes of different polytetrafluoroethy- tematic drop in mechanical properties (tensile
lene (PTFE) compounds containing carbon strength, elongation, and impact) after one and
black, glass fibers, and bronze by pyrolysis in two regrinding and injection molding opera-
a fluidized-bed reactor, yielding tetrafluor- tions. Eriksson et al. (1996a, 1996b) performed
oethylene (TFE) and hexafluoropropene an in-depth study of recycling and durability of
(HFP) monomers for the production of fluor- 30 wt.% short glass fiber reinforced polyamide
opolymers. The potential and unique benefits 66. It was found that fiber length distribution,
of chemical recycling, and promising research and not matrix or interfacial thermal degrada-
directions, have been outlined by Tesoro and tion, controls the overall short-term perfor-
Wu (1995). mance of the recycled composite. The same
Figure 9 Critical concentration vs. critical diameter of simulated impurities (glass beads) based on
maintained tensile strength of glass fiber reinforced polyamide 66 (reproduced by permission of the Society
of Plastic Engineers from Polym. Eng. Sci., 1998, 38, 749756).
authors established that fiber attrition domi- tylene terephthalate cyclic thermoplastic com-
nates during initial compounding and first in- posite with 58.7 wt.% fibers has been investi-
jection molding, whereas it is less severe during gated by Steenkamer and Sullivan (1997a)
further regrinding and remolding and that, using a grinding, compounding, and injection
below 50 wt.% regrind, the short-term strength molding process. The authors found that the
remains within design limits. The specific roles recycled composite had similar properties to a
of oxidative degradation (Eriksson et al., commercially available short fiber reinforced
1997a, 1997b), of coolant aging, and of thermoplastic composite, with, however, a
EPDM rubber impurities (Eriksson et al., 25% drop in elongation at break. Czvikovszky
1998b) on embrittlement of the composite and Hargitai (1997) examined the recycling of
were identified. A negative influence of the polypropylene copolymers from automobile
glass fibers on the polyamide oxidative stability bumpers by reinforcing with eight different
was found (Eriksson et al., 1998c). The dete- types of high-strength fibers, using reactive
rioration rate of recycled composites containing modification (low-energy electron beam) of
up to 25 wt.% regrind was similar to that of the fibermatrix interface. The recycled mate-
virgin samples during thermal aging but slightly rial could be extruded and injection-molded
faster during coolant aging (Eriksson et al., into fiber-reinforced thermoplastic of enhanced
1998a). Finally, critical sizes and concentra- bending strength, increased modulus of elasti-
tions of impurities below which a safe mechan- city, and acceptable impact strength. Similarly,
ical behavior is achieved were also determined, Wiegersma et al. (1997) used glass fibers to
as shown in Figure 9. reinforce and improve the impact strength of
Chu and Sullivan (1996) have established recycled PET. These various results all support
that recycled fiber-reinforced polycarbonate the development of design for recycling
possesses properties as good as or better than reported earlier, such as that of Braunmiller
a comparable commercial composite. Injection et al. (1999).
and extrusion compression molding yielded An alternative to mechanical grinding, which
recycled composites with good tensile proper- is systematically associated with mechanical
ties, at the expense of impact strength, whereas recycling, has been promoted by Papaspyrides
the opposite was true for compression molded and co-workers since the late 1970s, using
samples, as a result of corresponding fiber selective dissolution of the polymer fraction,
orientation distributions. Recycling studies of followed by filtration under pressure to recover
polyether-ether-ketone (PEEK) composites separately the fibers from the polymer solution
reinforced with 10 wt.% and 30 wt.% short (Papaspyrides and Poulakis, 1997; Papaspyr-
carbon fibers by Sarasua and Pouyet (1997) ides et al., 1995). The technique allows removal
revealed degradation of fibers and matrix dur- of contaminants and degraded species such
ing recycling, with subsequent reductions in as cross-linked molecules. The authors also
Young's modulus and strength, as well as indicate that it offers the advantage of yielding
impact strength. The recyclability of a polybu- controlled amounts of residual polymer
Recycling and Recovery of Polymer Composites 17
Table 4 Mechanical properties of composites containing recycled SMC fractions.
Composite Modulus Strength Elongation at break

(GPa) (MPa) (%)
Reference SMC (25% glass fibers)a 14 86 0.9

Reference BMCb 13.1 27.9 0.44
BMC + 20% SMC coarse regrindb 9.2 14.5 0.34
BMC + 20% SMC fine regrindb 10.2 16.1 0.14
PP + 9% chopped glassb 2.00 37.9 3.45
PP + 30% SMC coarse regrindb 2.20 21.0 2.34
PP + 30% SMC fine regrindb 2.07 20.9 2.47
Epoxy + 20% (GF and CaCO3 from SMC)c 35.0 3.0
a b
Sources: Dana (1991); Farissey (1992); c Patel et al. (1993).
attached to the recovered fibers (Poulakis et al., best SMC recycling approach was claimed by
1997a). This polymer coating acts as a compa- Jost (1995) to be grinding waste composite into
tibilizer, thus improving dispersion in case of filler and fiber fractions. Developing markets
reprocessing into virgin resins, such as polypro- include construction, friction materials, putty,
pylene. It leads to the formation of a unique and reinforced thermoplastic and other thermo-
interphase, that was found to be beneficial for set industries. Current research programs de-
modulus and strength of the composite, but voted to SMC recycling stress the need for
detrimental to impact strength (Poulakis and quality insurance of the recycled materials to
Papaspyrides, 1997; Poulakis et al., 1997b). avoid downcycling. To this end, Bledzki et al.
Ramakrishna et al. (1997) have compared the (1995) proposed an experimental design plan to
selective dissolution technique with a commu- analyze the mechanical performance of such
nition technique in the case of a carbon fiber materials. The ERCOM composite recycling
reinforced PEEK, the latter eventually found to organization was founded in 1991, targeting
be the most efficient. Theoretical treatment of the suppliers of the automotive and electrotech-
the dissolution rates for highly filled polymers nical fields. The program is based on the prin-
was recently developed by Cao et al. (1998). ciple of recycling by grinding used materials
down to fiber-rich fractions suitable for mixing
with new SMC materials as fillers and rein-
forcements; the fact that the resin does not
2.33.4.2.2 Thermoset composites melt proved to be an advantage in terms of
compatibility (Kelderman, 1995; Schaefer,
A prerequisite to reusing thermoset resins 1995, 1997). Additional information about
and their composites as regrind is to reduce SMC recycling can be found in Chapter 2.22,
by shredding and grinding the size of the parts this volume. Table 4 reports data extracted
into flakes or powder fractions with controlled from the literature relating to the mechanical
sizes (Farissey, 1992) (see Chapter 2.19, this performance of SMC, BMC, and composites
volume). The techniques developed for this containing SMC regrind fractions.
are capable of generating a large variety of Besides the SMC recycling activities, dedi-
regrind fractions containing defined fiber cated projects were developed for specific ther-
length distributions, as indicated by Kelderman moset composite recycling, such as glass-fiber
(1995). In the 1980s, the regrind was mostly reinforced polyester/PUR sandwich structures
used as filler, either in uncured thermoset resins developed for building applications, for which
or in virgin thermoplastics. It was also used Mlecnik (1997) emphasized the need for design
with adhesive binders, where a large fraction for reuse tools. An Internordic program en-
of regrind is bound together with a small titled Recycling of Thermoset Composites
amount of adhesive. Later on, the potential of was launched by the Swedish Institute for Com-
the regrind fraction as reinforcement has been posites (NUTEC-SICOMP), with several pro-
explored. Major efforts have been directed to jects related for example to the recycling of
recycling sheet molding compounds (SMC) and boats (Pettersson and Nilsson, 1997). Another
bulk molding compounds (BMC), which repre- example was reported by Vasut et al. (1999)
sent ca. 50% of all composites. One may cite the who have studied the recycling of automotive
SMC Automotive Alliance aiming at develop- wastes, such as rubber-thermoplastic reinforced
ing commercial processes to convert composite composites, into noise abatement structures
scrap into new automotive applications. The along highways.
2.33.4.2.3 Fiber reinforcements reinforced concrete, and compression molded

panels. The suitability of the pyrolysis process
This section mainly concerns the recycling of for recycling SMC has been investigated as an
general-purpose glass into fibers to be used as alternative to the mechanical recycling route by
reinforcements in polymer composites. Studies Demarco et al. (1997). Studies have shown that
have shown that the performance of unsatu- temperatures in the range of 400500 8C are the
rated polyester structural composites rein- most suitable for recycling SMC by pyrolysis. In
forced with A-glass (primarily composed of the case of a glass fiber reinforced orthophthalic
soda lime silicate) recycled fibers is comparable polyester SMC, gas yields of 813 wt.% can be
to that of reference composites reinforced with sufficient to provide the energy requirements of
traditional E-glass, providing the A-glass fiber the process plant. Liquid yields of 916 wt.%
fraction is increased to offset their lower me- are nonpolluting liquid fuels with a high gross
chanical strength compared with the E-glass calorific value of 36.8 MJ kg71. About 40 wt.%
fibers (Steenkamer and Sullivan, 1997b). Ken- of such liquids could be used as petrols, and the
nerley et al. (1998) propose using a fluidized- remaining 60 wt.% could be mixed with fuel
bed process to recover glass fibers from SMC oils. The solid residues of 7282 wt.% can be
composites scrap. Glass fibers recovered at recycled in BMC with no detrimental effect on
450 8C using this process, whose strength is the BMC mechanical properties.
reduced to about half that of virgin fibers, To summarize this section devoted to recy-
have been used as partial and full replacement cling technologies, it turns out in general that,
for virgin fibers in a dough molding compound as was evidenced by Buggy et al. (1995), an
(DMC). A drop in mechanical strength was optimal recycling strategy has to be defined
noticed at recycled fiber fractions above 50%, for each specific material combination. These
whereas the flexural and Young's moduli were authors have shown that solvent recycling was
found to remain unaffected. appropriate for carbon fiber/PEEK APC-2,
whereas mechanical recycling was interesting
in the case of polyester/glass prepreg off-cuts,
2.33.4.3 Incineration and Energy Recovery and solvent swelling was used for an aramid
Routes fiber/epoxy composite. In the case of mechan-
ical recycling, most studies tend to indicate that
Incineration significantly reduces the volume fiber attrition is the dominant factor contribut-
of waste materials and, as such, has been pro- ing to a drop in mechanical properties, at least
moted as an alternative to the prevalent method in the short-term. In the long-term, however,
of disposal into landfills, nowadays prohibitive the durability of mechanically recycled compo-
due to increased cost, negative public opinion, sites depends, to a larger extent, to the degrada-
and legislation. Clearly, these two waste man- tion state of matrix and interface. The
agement routes lead to a total loss of the mate- development of reliable components using com-
rial value, and are further not free from posite regrind is not free of costs, and clearly
environmental impacts. By contrast, when com- requires in-depth quantitative performance as-
bined with energy recovery, incineration of sessments. The final statement follows Tesoro
waste finds increasing support as a viable recy- and Wu (1995), who clearly emphasize the need
cling method. For more information on the for long-range programs devoted to design for
energy recovery of plastics, the reader is re- recycling on the one hand, and multidisciplin-
ferred to the documents published by Mark ary research programs to develop a new gen-
and Vehlow (1998) under the auspices of the eration of polymers with built-in recovery
APME. potential, on the other.
Most of the efforts devoted to energy recov-
ery of polymer composites can be associated
with studies on automotive shredder residues
2.33.5 INTRODUCTION TO LIFE CYCLE
(ASRs). Since 1990, the SMC Automotive Alli-
ASSESSMENT OF COMPOSITES
ance, with 30 suppliers of the auto industry,
promotes the combination of pyrolysis pro- 2.33.5.1 What is Life Cycle Assessment?
cesses with mechanical recycling as the most
realistic mid-term disposal options for ASR Environmental life cycle assessment (LCA) is
(see, for instance, Automotive Engineering, a tool to assess the environmental impact of
1994). Unser et al. (1996) have explored recov- products over the whole product life cycle, and
ery methods for composites, which convert the is usually performed in three phases (SETAC,
polymer matrix to lower chain hydrocarbons 1993) followed by an improvement assessment
and fuel gas leaving behind fibers, used with or interpretation procedure (Jolliet and Crettaz,
success in bulk molding compounds panels, 1997). According to Ryding (1994), LCA is
Introduction to Life Cycle Assessment of Composites 19
mainly applied to internal analyses of products, 2.33.5.1.3 Impact assessment

to achieve improvements, as well as to compare
alternative products. For comprehensive infor- The impact assessment assesses the environ-
mation, the reader is referred to the works of mental impact and is composed of three parts:
the Society of Environmental Toxicology and (i) The classification step determines the pol-
Chemistry (SETAC, 1993) and the Center of lutant emissions contributing to each impact
Environmental Science in the Netherlands category or problem type (greenhouse effect,
(CML, 1994; Heijungs, 1992). Two cases stu- human toxicity, ecotoxicity, etc.).
dies are presented to illustrate the application (ii) The characterization step weighs and
of LCA where glass reinforced composites are quantifies the impact of the emissions within
compared to steel and aluminum on the one each category.
hand, and to natural fiber reinforced compo- (iii) The valuation step assesses the relative
sites on the other. importance of each impact category by deter-
mining the damages on safeguard subjects and
the respective societal values of these damages
and subjects.
2.33.5.1.1 Goal definition, scope, and
functional unit
The goal definition defines the aim and the 2.33.5.1.4 Improvement analysis
scope of the study as well as the function and
functional unit of the studied product. The The aims of the improvement analysis are to
scope defines the functional boundaries, that determine environmental weak points in the
is, the life cycle steps to be considered in the production system as well as available technol-
analysis, and the type of impacts that will be ogies for improvements and organizational
accounted for. It further involves geographical measures to accomplish such changes. In this
boundaries and temporal boundaries. The lat- phase, sensitivity studies and uncertainty ana-
ter obviously depends on the lifetime of the lyses are performed together with improvement
product; it also depends on the lifetime of the assessment.
selected emissions. The functional unit relates
to the service provided by the use of the product
and, as such, is a key feature of any LCA. In 2.33.5.1.5 Key issues in life cycle assessment
most cases, the functional unit should be dis-
tinguished from the production unit. As an It is generally recognized that a screening
example of a functional unit, let us consider a approach, where one ignores all effects contri-
composite panel used in sandwich structures for buting to less than a given fraction of the total
thermal and acoustic insulation, for instance in impact, for example, 5%, should be performed
buildings. The production unit would typically prior to carrying out a more detailed LCA.
be one square meter of the composite, whose Explicit definitions of the system function and
primary function would be to give structural boundaries, including functional unit, are essen-
stiffness to the sandwich. Additionally, second- tial elements in the analysis. Further key issues
ary functions of the panel would be to integrate include allocation procedures and sensitivity
fixtures for assembly and to offer decorative analyses to determine the reliability of the data
alternatives. The production unit is expressed in (see, for instance, the related publication of the
this example in m2. The functional unit, how- Center of Environmental Science, CML, of the
ever, considers the service provided by such Leiden University, 1994). Finally, the LCA tool
composite panel, that is, to provide thermal finds its usefulness when the interpretation
and noise insulation for a given lifetime, phase enables the selection of more environmen-
which would typically be of the order of several tally friendly materials and technologies.
tens of years. It will therefore be expressed in
terms of m2 year.
2.33.5.1.6 Active and passive applications
2.33.5.1.2 Inventory analysis By definition, an environmentally active pro-

duct mainly impacts the environment during
The inventory lists pollutant emissions and service, contrary to an environmentally passive
resources consumption attributed to the pro- product, for which the main impacts are during
duct system defined in the preceding step. The manufacture and end-of-life treatment. The cu-
inventory process is often time-consuming, and mulated life cycle impacts of these two types of
finds help from databases implemented for in- products would be such as sketched in
stance in ecodesign tools. Figure 10.
Figure 10 Normalized cumulative impact of environmentally active (e.g., automotive) and passive (e.g.,
furniture) applications.
2.33.5.2 Life Cycle Assessment of Recycling ment, the environmental impact of which is
essentially determined by transportation (Ishi-
Use of the life cycle assessment method as a kawa, 1997). Higher recycling rates are ob-
decision-making tool is in constant progress. viously associated with a rapid increase in
We would like to point out here important transportation distance that is proportional to
factors to be accounted for when planning a the environmental impact. Efforts in integrated
recycling operation for composite materials. waste management were found to lower this
Dominant direct contributions to the environ- contribution to the total impact (e.g., Schmidt
mental impact of recycling are likely to arise and Fleischer, 1997). Several approaches for an
during collection of end-of-life parts, with its optimum recycling network can be found in the
corresponding transportation burden, then dur- studies of Eyerer and co-workers (Bohnacker
ing the reprocessing operation, and eventually et al., 1995; Saur et al., 1997), Schwarz and
during further transportation. As will be de- Steininger (1997), Everett et al. (1998), and
tailed in the following case studies, and if one Newell and Field (1998), who stress the impor-
excludes the environmental effects of transpor- tance of how to allocate inputs and outputs
tation, the impact of producing secondary (i.e., between primary and secondary materials.
recycled) materials is generally lower than that
of primary materials, due to savings in feedstock
extraction and refining processes. This fact is
determinant in the case of aluminum, as seen in 2.33.5.3 Case Study of Components for
the corresponding material intensities reported Transportation Applications
in Table 1. As a consequence, there is a wide-
spread belief that increasing recycling levels, This case study considers a hypothetical
that is, the fraction of secondary material in a structural component developed for transpor-
given application, will systematically lead to an tation applications. An example of such a com-
overall reduction in environmental load, in spite ponent would be the front end of a car,
of the fact that such linear interpolation only although some of the materials selected for
provides a lower bound for the impact. Indeed, comparative purposes might not be relevant
it does not account for nonlinear effects, result- to the state-of-the-art technology for front-
ing for instance from the increasing environ- ends. Nonetheless, this case study is intended
mental impacts of revitalization (in order to to illustrate the trade-offs which arise when
maintain the quality of the recycled material) optimizing both technology and environmental
at higher recycling rates. An example of such impacts in the case of an active product, as was
nonlinearity has been reported for paper recy- defined in the preceding section. Few of such
cling (Schmidt and Fleischer, 1997). In the case analyses have been published, and in-depth
of composites, these effects would typically cor- comparative analyses can be found in the
respond to the use of stabilizers and compatibi- work of Eyerer et al. (1994) and Bohnacker
lizers to overcome degradation of the polymer et al. (1995). Most of the data used in the
matrix and its probable contamination with inventory analysis was found in studies of Re-
foreign inclusions. Other nonlinearities arise nard et al. (1994) and Young and Vanderburg
when considering the logistics of waste manage- (1994).
Table 5 Material selection for the life cycle assessment of a structural component.
Material Weight Production yield Recycling potential Price

(kg) (%) (%) (SFr/kg)
Steel sheet 10 65 90 0.5

Polyester composite (SMC) 7.0 100 20 3
Thermoplastic composite (GMT) 4.5 100 40 4
Aluminum 3.8 65 90 2
Sources: Renard et al., 1994; Young and Vanderburg, 1994.
Table 6 Energy consumption (MJ, boldface) and CO2 emissions (kg, italics) of selected materials related to
the life-cycle of a structural component.
Steel sheet SMC GMT Al
Extraction of raw materials 388 29 378 6 422 9 1315 224

Recycling of materials 110 8 49 3 50 4 292 23
Manufacture of part 171 12 41 3 42 3 133 8
Service 100 000 km 1423 85 995 60 640 39 541 34
Total, 0% recycling 1982 126 1414 69 1104 51 1989 266
Total, 100% recycling 1704 105 1085 66 732 46 966 65
2.33.5.3.1 Materials selection and functional 2.33.5.3.2 Energy and CO2

unit
For the sake of simplicity, the LCA considers
The four materials selected are steel, only energy requirements and CO2 emissions.
aluminum, a thermoplastic composite (poly- The environmental impact, expressed in envir-
propylene-based GMT (see Chapter 2.27, this onmental load units (ELU, Ryding, 1994), is
volume), for glass mat thermoplastic), and a calculated according to the EPS method using
thermoset composite (polyester-based SMC the equivalence of 0.014 ELU/MJ for the gross
(see Chapter 2.22, this volume), for sheet mold- energy requirements (GER) and 0.088873
ing compound), as specified in Table 5. The ELU/kg equivalent CO2 for the global warming
steel component is considered to be the refer- potential (GWP). A marginal weight gain, that
ence material, and is attributed an arbitrary is, the savings in fuel consumption during the
weight of 10 kg. The corresponding weight of use phase due to reduced weight, was assumed
the component was calculated for the two com- to be equal to 0.04 ml/kg.km (Maggee, 1982).
posite materials, with the criteria of constant The results of the LCA inventory for both 0 and
equivalent bending stiffness per weight of ma- 100% recycling scenarios are reported in
terial, E1/3/r, where E is the Young's modulus Table 6, where a service of 100 000 km was
and r is the density (Ashby, 1992). The weight considered. Figure 11 represents graphically
of the aluminum part was set to be equal to the linear evolution of the overall impact,
3.8 kg (Renard et al., 1994). In addition, Table 5 expressed in ELU units, with kilometrage. The
specifies the production yield and the recycling initial intercept corresponds to the production
potential for each material type, as well as its impact, and the slope of the line corresponds to
typical market cost. The recycling potential the impact during service, which is simply pro-
represents the fraction of regrind that is incor- portional to the weight of the component.
porated in the virgin material to produce a new Despite the simplifications used in the inventory
part, according to the technical state-of-the-art and impact assessment, the calculated environ-
(Furrer, 1995; Kelderman, 1995). mental profiles provide useful information to
The production unit is one component, and is compare composites with steel and aluminum.
expressed in terms of its weight. The functional First and foremost, the driving force to lower
unit is the component for a given service, say weight in transportation applications is strik-
200 000 km, which would correspond to ing. Similarly, the environmental benefit of
7 kg 6 200 000 km for the SMC part. Two func- recycling aluminum is considerable, whereas it
tional boundaries are considered as alternative is less obvious for steel as well as for the com-
scenarios to compare a nonrecycling option posite materials. This remark is highlighted in
with a hypothetical 100% recycling option. Figure 12, where the effect of recycling rate on
Figure 11 Environmental impact of selected materials for a structural automotive component vs.
kilometrage during service, for 0% and hypothetical 100% recycling scenarios. See text for details.
Figure 12 Environmental impact of selected materials for a structural automotive component vs. recycling
rate, for a service of 100 000 km. See text for details.
environmental impact is calculated for a service materials. The calculation is based on simulated
of 100 000 km from a linear interpolation of annealing principles found to be equivalent to
the data obtained for 0 and 100% recycling optimizing travel distances, and treated as the
scenarios. famous traveling salesman problem (see, for
As was previously pointed out, high recycling instance, the compilation of Lawler, 1990). It
rates are associated with nonlinear effects, with uses as a reference the average transportation
corresponding rapid increase in environmental distances for waste management documented
impact. Figure 13 reproduces a simulation car- in the study of Schmidt and Fleischer (1997).
ried out for the aluminum and SMC composite The worst case calculation corresponds to a
Figure 13 Environmental impact of selected materials for a structural automotive component vs. recycling
rate, for a total service of 200 000 km, and under two scenarios of collection logistics. See text for details.
nonoptimized route between cities of different environmental assessment, to define in particu-

sizes and arbitrary locations. The best case lar optimal product composition. This case
calculation performs in a first step a local route study is based on recent work where the envir-
optimization between a number of small cities onmental impact of transport pallets made of
and one large city, and then calculates the glass-fiber-reinforced polypropylene was com-
remaining route between the large cities. pared to natural-fiber reinforced polypropylene
Although the exact values reported in the figure during a cycle of manufacture, use, and recy-
should be taken with caution, their magnitude cling (Gfeller-Laban and Nicollier, 1999; Lund-
is qualitatively comparable to data published quist et al., 1999). Particular attention is paid to
elsewhere (Schmidt and Fleischer, 1997), and the effect of fiber content on energy consump-
thus provide useful information. In the case of tion, which reflects to a good extent the overall
aluminum, it is almost always beneficial to use impact. Over one million pallets are made per
secondary material, as its environmental impact year and 150 million tons of wood pallets are
is by far smaller that that of primary aluminum. sent to landfill each year in the US alone
By contrast, the optimal recycling rate for the (Marsh, 1998). Thermoplastic pallets are a vi-
composite material clearly depends on the able alternative since they have higher longevity
logistics scenario. It is approximately 30% for and require less maintenance, thus representing
nonoptimized collection, and of the order of high potential for cost savings by product life
70% if the collection logistics are optimized, extension.
that is higher than the current practices. To
summarize, the main conclusions drawn from
this case study are twofold: 2.33.5.4.1 Materials selection and functional
(i) Very high recycling rates are not necessa- unit
rily environmentally friendly.
(ii) The environmentally optimal recycling Traditional E-glass fibers (GF; density 2.6,
rate is often higher than the actual recycling rate. Young's modulus 72 GPa) and a standard grade
of polypropylene (PP; density 0.905, Young's
modulus 1.15 GPa) were selected as the refer-
2.33.5.4 Case Study of Glass-fiber and ence materials. The natural fibers were obtained
Natural-fiber Reinforced from China reed, a perennial grass, character-
Thermoplastics ized by a fast growth due to a particularly
effective photosynthesis (Werner and Kohler,
As was introduced in Section 2.33.1, increas- 1994), and whose production reaches ca. 20
ing the use of renewable resources is one of the tons/ha/y of biomass. The China reed fibers
three routes towards sustainable resource man- (CR; density 1.05, Young's modulus 30 GPa)
agement, providing this increase is based on were obtained through grinding and sieving,
Table 7 Composition and properties of the glass-fiber reinforced PP (GF) and the China reed fiber
reinforced PP (CR) composite pallets, according to the three stiffness scenarios.
Scenario 1: Scenario 2: Scenario 3:

low stiffness medium stiffness high stiffness
GF CR GF CR GF CR
Composite stiffness (MPa) 8.2 8.2 15.3 15.3 20.3 20.3

Fiber volume fraction (%) 10 24.6 20 49.1 27 66.3
Fiber weight fraction (%) 24.2 27.4 41.8 52.8 51.5 69.5
Pallet weight (kg) 15 13.1 15 11.8 15 11.0
Pallet volume (m3) 0.0140 0.0140 0.0121 0.0121 0.0110 0.0110
with a yield of 70%. The remaining 30% resi- mitted to J. Risk. Anal.), for the entire life
dues are presently landfilled. cycle of the pallets: from agricultural produc-
The functional unit is one composite pallet, tion of China reed and production of glass
defined by its shape, i.e., its volume, and its fibers, grinding of China reed fibers, transport,
stiffness, further satisfying service requirements production of polypropylene, pallet fabrica-
during 5 years. To compare the two types of tion, pallet use, and pallet elimination by
reinforcements, it is crucial that the correspond- means of incineration with heat recovery. The
ing pallet have the same volume and mechanical energy consumption and emissions of over 50
properties. The glass-fiber reinforced pallet was pollutants in air, soil, and water determined in
selected as the reference product, with a weight the inventory were reported to the functional
of 15 kg. Three scenarios were envisaged: unit. In the impact assessment, the pollutants
(i) low-stiffness composite pallet (E = were weighted with characterization factors en-
8.2 MPa), where the reference pallet has a abling their summation into total impacts on
glass-fiber volume fraction of 10%. resource consumption, human health, and ter-
(ii) medium-stiffness composite pallet (E = restrial and aquatic ecosystems. Figure 14
15.3 MPa), where the reference pallet has a shows the consumption of primary nonrenew-
glass-fiber volume fraction of 20%. able energy for the three scenarios.
(iii) high-stiffness composite pallet (E = Several remarkable conclusions can be drawn
20.3 MPa), where the reference pallet has a from these results. First, it is evident that the
glass-fiber volume fraction of 27%. manufacturing stage of polypropylene is sys-
The composition of the China-reed fiber rein- tematically the greatest contribution to the
forced pallets was simply calculated using the overall energy consumption. The implication
rule of mixtures as a first approximation, so that of this is that higher fiber fractions, whether
all pallets with a given fiber fraction have the glass fibers or natural fibers, are beneficial from
same stiffness and same volume, with the con- the energy consumption point of view. Previous
dition that all glass-fiber reinforced pallets work has shown that the same was true for all
weigh 15 kg. The composition and weight of classes of impact indicators, at the exception of
all types of pallets are reported in Table 7. In the human toxicity factor which slightly in-
all instances, due to the lower density of the creases with increasing fiber fraction, and the
natural fibers, the weight of the corresponding eutrophication factor, in the case of the China
pallet is less than that of the glass-fiber rein- reed fiber reinforced pallet (Gfeller-Laban and
forced alternative. Surprisingly, the weight of Nicollier, 1999). These results were confirmed
the natural fiber reinforced pallet decreases with by the CML impact assessment method (Hei-
increasing fiber fraction, while the density of the jungs, 1992).
fibers is slightly higher than that of the polymer Second, the contribution of China reed agri-
matrix. This decrease is contrary to the glass- cultural production to the overall energy con-
fiber case, and results from the decrease in sumption is negligible, and is by far smaller
volume of the China reed pallet. than that of the glass fibers. In spite of a higher
contribution to eutrophication effects, all im-
pact categories related to the China reed pro-
2.33.5.4.2 Impact assessment and sensitivity duction have a lower contribution compared to
analysis the production of glass fibers.
It should finally be mentioned that the dur-
The environmental impact of the composite ability of the natural fiber composite could be a
alternatives was assessed using the CST95 limitation when selecting this class of reinforce-
method (Jolliet and Crettaz, 1997 and sub- ments. In this case study, a lifetime of 5 years
Closure and Perspectives 25
Figure 14 Primary nonrenewable energy consumption for glass fiber/PP vs. China reed/PP composite
transport pallets (after Gfeller-Laban and Nicollier, 1999; Lundquist et al., 1999).
was considered for both types of composites. A as the Polluter Pays Principle (PPP) instituted
sensitivity analysis revealed that the China reed by the OECD, also in the year 1972. The 1980s
fiber reinforced pallets have a lower environ- have subsequently seen increasing development
mental impact than the glass fiber reinforced of design for environment and life cycle assess-
pallets providing that their lifetime is at least ment tools, as described in this chapter.
2.23 years. During the 1990s, a novel concept emerged
under the name industrial ecology, already en-
visioned in the 1950s, as recently reviewed by
Erkman (1997). According to Ehrenfeld (1997),
2.33.6 CLOSURE AND PERSPECTIVES industrial ecology is a new system for describ-
ing and designing sustainable economies. It
Until mid-twentieth century, there was no offers guidelines to designers of products and
serious consideration of the interaction between the institutional structures in which production
increasing industrialization and the ecosystem. and consumption occur, as well as frameworks
The year 1952, with the introduction of the Safe for the analysis of complex material and energy
Minimum Standard of Conservation Principle flows across economies. In short, industrial
(SMS), marks a clear change in awareness on ecology promotes systems where internal
the vulnerability of the ecosystem. In the next flows are greater than external flows, and, as
two decades, the number of international events such, integrates the three mains topics discussed
related to global environmental issues, whether in this chapter, namely (i) durability analysis of
conferences or government regulations, in- composites, (ii) their sustainable design includ-
creased a considerable extent. In 1968, the In- ing recycling issues, and (iii) life cycle assess-
tergovernmental Program on the Man and the ment. Recent studies in the field of industrial
Biosphere (MAB) was launched after the Bio- ecology with emphasis on material-related is-
sphere Conference of UNESCO, followed in sues (e.g., Szekely and Trapaga, 1995; Frosch
1970 by the US Clean Air Act, and the United et al., 1997) suggest that large environmental
Nations Conferences on the Law of Sea (UN- benefits can be achieved by closing material
CLOS). The United Nations Environment Pro- loops, which, as a reminder, is reached by ex-
gram (UNEP) was created in 1972 during the tending product lifetime, by recycling materials,
Stockholm Conference on Human Environ- or by using renewable resources.
ment. During the same year, the report Limits The wide spectra of applications using poly-
to growth of the Club of Rome and MIT and mer composites nevertheless imply that an op-
its Standard World Model were published. This timal loop-closing strategy has to be defined for
rapid increase in environmental awareness had each particular case. As reported in the preced-
direct implications on the industry, which ing sections, considerable efforts are devoted to
mainly reacted following end of pipe ap- improve durability analyses, as also to develop
proaches. These were essentially dealing with reliable recycled and renewable composites. In
depollution strategies, rather than cleaner pro- the latter two fields, these efforts have been
duction and pollution prevention actions, such accompanied by the development of numerous
ecodesign tools, and there is no doubt that such C. A. Bernardo, A. M. Cunha and M. J. Oliveira, Polym.
activities will continue to expand. Finally, we Eng. Sci., 1996, 36, 511519.
V. Bhasin, D. Conroy and J. Reid, Naval Eng. J., 1998,
would like to stress that more work is still 110, 5165.
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A. K. Bledzki, S. Reihmane and J. Gassan, Polym.-Plast.
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ACKNOWLEDGMENTS pp. 715.
W. L. Bradley and T. S. Grant, J. Mater. Sci., 1995, 30,
The author would like to express his grati- 55375542.
R. D. Bradshaw and L. C. Brinson, J. Eng. Mater.
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2.

2.33.1 INTRODUCTION TO LIFE CYCLE ENGINEERING 2

2.33.5.1.5 Key issues in life cycle assessment 19

2.33.1 INTRODUCTION TO LIFE CYCLE resources turnover, from cradle to cradle, as

Material MI abiotic resources MI water

Fiber-reinforced composite 2.91 49.1

2.33.1.3 The Criteria and Analyses of

Figure 3 Priorities in life cycle engineering.

According to this hierarchy, incineration towards equilibrium of amorphous glassy poly-

2.33.2 THE LIFE CYCLE OF POLYMER

Table 3 Factors contributing to aging and degradation of polymer matrices.

Nature of polymers Aging and degradation factors Phenomenology

(i) Organic matter . Temperature (pyrolysis) . Molecular scission

particularly moisture- and temperature-sensi- 2.33.2.2 Brief Review of Aging and

unidirectional composites, and of Curtin and characterized by a distribution of relaxation

2.33.3.3 Reduction of Material Intensity

Figure 8 Recycling technologies (adapted from Lundquist et al., 2000).

2.33.4.1 Chemical Routes to Recycling 2.33.4.2 Mechanical Recycling and Quality

Table 4 Mechanical properties of composites containing recycled SMC fractions.

Composite Modulus Strength Elongation at break

Reference SMC (25% glass fibers)a 14 86 0.9

2.33.4.2.3 Fiber reinforcements reinforced concrete, and compression molded

mainly applied to internal analyses of products, 2.33.5.1.3 Impact assessment

2.33.5.1.2 Inventory analysis By definition, an environmentally active pro-

Material Weight Production yield Recycling potential Price

Steel sheet 10 65 90 0.5

Sources: Renard et al., 1994; Young and Vanderburg, 1994.

Steel sheet SMC GMT Al

Extraction of raw materials 388 29 378 6 422 9 1315 224

2.33.5.3.1 Materials selection and functional 2.33.5.3.2 Energy and CO2

nonoptimized route between cities of different environmental assessment, to define in particu-

Scenario 1: Scenario 2: Scenario 3:

Composite stiffness (MPa) 8.2 8.2 15.3 15.3 20.3 20.3

J. G. Poulakis, C. D. Arvanitopoulos and C. D. Papas- R. A. Schapery, in `Progress in Durability Analysis of

Copyright # 2000 Elsevier Science Ltd. Comprehensive Composite Materials

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