Chapter 3

Green Composite Manufacturing via

Compression Molding and Thermoforming

K.C. Birat, Muhammad Pervaiz, Omar Faruk, Jimi Tjong, and Mohini Sain

Abstract Increasing concern over material usage and its impact on the environmental
have escalated the growth of green composite materials. There are tremendous oppor-
tunities where conventional mineral and synthetic-based materials can be replaced
with green composite materials. Before green composites can be used to manufacture
various products, it is important to understand their processing steps and optimize
process parameters. Past researches on green composites were focused mostly on
characterization, and less research can be found in manufacturing of green compos-
ites. Common technologies include but are not limited to injection molding, extrusion,
thermoforming, and compression molding. In this chapter, manufacturing process of
green composites via compression molding and thermoforming is developed based on
patents and literature review. Main emphasis is given toward key processing steps,
such as material selection, preprocessing, semifinished product manufacturing, and
green composite fabrication. Moreover, processing data of some commercially avail-
able green composites and biopolymers is summarized.

Keywords Green composites • Compression molding • Thermoforming • Material

selection • Semifinished product • Prepregs • Composite fabrication

3.1 Green Composites

There is a growing trend in plastic part manufacturers for processing new class of
composite materials, called green composites for reducing the environmental impact
and reducing the cost of raw materials (Reddy and Yang 2011). These composites
offer practical solution to conventional glass-fibre-reinforced or mineral-filled plastic
composites where renewability and sustainability of materials were compromised

K.C. Birat (*) • M. Pervaiz • O. Faruk • M. Sain

Faculty of Forestry, Centre for Biocomposites and Biomaterials Processing (CBBP),
University of Toronto, 33 Willcocks Street, Toronto, ON, Canada, M5S 3B3
e-mail: b.kc@mail.utoronto.ca
J. Tjong
Faculty of Forestry, Centre for Biocomposites and Biomaterials Processing (CBBP),
33 Willcocks St, Toronto, ON, Canada, M5S 5B3

© Springer International Publishing Switzerland 2015 45

M.S. Salit et al. (eds.), Manufacturing of Natural Fibre Reinforced
Polymer Composites, DOI 10.1007/978-3-319-07944-8_3
46 K.C. Birat et al.

(Thakur et al. 2013). Green composites can be defined as the combination of two or
more materials completely from renewable sources. For example, composites con-
taining natural fibre and biopolymers or the combination of two biopolymers (Ben
and Kihara 2007; Gejo et al. 2010) Natural fibre are carbohydrates derived from
various plant sources, while biopolymers are usually derived from plant-based sug-
ars, starch, proteins, or vegetable oils (Ben and Kihara 2007). Most of the research
and development work in the past focused on composites from natural fibre rein-
forced with polyolefins and thermosets (Ben and Kihara 2007; Reddy and Yang
2011). With these composites, there are concerns regarding their end-of-life recy-
cling and disposal (Gejo et al. 2010). Hence, the research focus has shifted toward
green composites that come from 100 % renewable source and are completely bio-
degradable after the product life (Takemura 2010). In recent years, few applications
of green composites are found in food and packaging, agricultural, automotive, and
medical industry. Most commonly used natural fibres are wood, hemp, flax, wheat,
jute, sisal, coconut, banana, and bagasse. Recently, micro- and nanocellulose from
plants, algae, and bacteria are also being studied as a new source of natural fibre
reinforcements (Reddy and Yang 2011). Commonly studied biopolymers are soy-
based epoxy, starch, proteins polycaprolactone (PCL), polyhydroxybutyrate (PHB),
polylactic acid (PLA), polyester amide 11 (PA11), and polyvinyl alcohol (PVA)
(Reddy and Yang 2011; Takemura 2010). Among these, PLA has seen much
commercial success while PHB and PA11 are also slowly emerging (U.S. Patent
No. US20100170649 A1 2010a).
Most common processing technologies for green composites are injection mold-
ing, compression molding, extrusion, thermoforming, pultrusion, and resin transfer
molding (RTM) (Faruk et al. 2012). Study by Altun et al. (2013) used injection
molding to manufacture wood flour and PLA composites, while Hu et al. (2012)
used compression molding to manufacture jute and PLA composites. Other study
reported use of thermoforming (Chang et al. 2009) and RTM (Faruk et al. 2012).
Higher demand for plastic composites as a substitute for metal parts has led to series
of novel methods that combine these technologies such as direct long-fibre thermo-
plastics (DLFTs) (Faruk et al. 2012). Broadly, selection of these manufacturing
technologies depends on the type and the form of material to be processed, volume
of production, capital cost requirement, complexity of the part design, and quality
of the part (Sain and Pervaiz 2008). In this chapter, we explore the fabrication pro-
cess for green composites via compression molding (CM) and thermoforming (TF).
Basic processing steps and their features are briefly summarized with the emphasis
on green composite materials.

3.1.1 Compression Molding and Thermoforming

In compression molding, thermoplastic or thermoset material (in the form of gran-

ules, sheet, or prepregs) is melted in the mold cavity under heat and pressure, followed
by cooling and part removal after it is cured (solidified) (Faruk et al. 2012; Onal and
Adanur 2005). In thermoforming, a thermoplastic sheet is heated to its softening
3 Green Composite Manufacturing via Compression Molding and Thermoforming 47

point and stretched over into a single-sided mold and holding in place while it cools
and solidifies to form a desired part (Erchiqui et al. 2009; Klein 2009). Schematic
of CM and TM process is shown in Fig. 3.1. From the production point of view, CM
is usually used for complex part designs and TM for simpler part designs. However
more and more complex parts are being thermoformed due its increasing use
(Erchiqui et al. 2009). Part quality requirement is also another consideration for the
selection of CM and TF. CM is also used in relatively higher-quality parts as com-
pared to TF because of fewer knit lines and less fibre-length degradation (Faruk
et al. 2012). However inconsistencies as a result of incomplete mixing of fibre with
resin may persist in CM if fibre yarns or fibre mats are used (Cheng 2009). Likewise,
stretching process in TF creates nonuniform wall thickness which is undesirable for
higher-quality parts with tight geometric tolerances (Klein 2009). Some other fea-
tures of CM and TF are summarized in Table 3.1.

a
Top Mold v
v, F

Guide
Pins Molded
Sheets/prepregs/granules
part

Bottom Ejector
Mold Pins v

b Heater
Clamps
Clamps open
closed Finished part
Green-composite sheet

v v

Mold
Vacuum
holes

Vacuum

Fig. 3.1 Schematic diagram of (a) compression molding and (b) thermoforming (via vacuum)
process
48 K.C. Birat et al.

Table 3.1 Features of compression molding and thermoforming technologies

Compression molding
SN Features (CM) Thermoforming (TF)
1 Type of process Usually discontinuous Continuous
2 Application type Low-volume production High-volume production and
and high-tolerance parts low-tolerance parts
3 Acceptable raw Sheets, composite Sheets only
material form granules, prepregs
4 Material waste Low High
5 Application Automotive hood, fender, Food and packaging containers,
door panels, gears, etc. aircraft windscreens, interior
panels, boat hulls, etc.

3.2 Fabrication Process

During fabrication of green composites, processing parameters determine the extent

of morphological changes, surface interaction, and chemical cross-linking between
constituents of green composite (Gällstedt et al. 2004). Understanding of these phe-
nomena is significant for gaining fundamental knowledge of processing window.
Processing of green composite is different to traditional polymer composite due to
changes in rheological behavior, thermal instability, tendency to water absorption,
and morphological differences within natural fibre types and species (Sain and
Pervaiz 2008). Natural fibres and biopolymers exhibit viscoelastic behavior causing
a change in its flow characteristics (Sain and Pervaiz 2008). Fewer studies on the
flow behavior of natural fibre-filled systems showed increase in viscosity of the
composites with fibre content and reduced processability (La Mantia and Morreale
2011). On the other hand, biopolymers like PLA are crystalline and exhibit poor
flow properties (Lim et al. 2008). Their degradation starts at temperature above
190 °C and narrows at the processing window (Zampaloni et al. 2007). Moreover,
hydrophilic nature of natural fibre reduces fibre-matrix adhesion and fibre disper-
sion which are keys for processing within preferred output rates (Thakur et al.
2011b). Other challenge is that natural fibres from different plant sources are differ-
ent in chemical composition and morphology making them even more difficult to
process (Faruk et al. 2012).
Compression molding and thermoforming are secondary processes because they
both involve preprocessing of selected materials to manufacture semifinished prod-
ucts such as sheets, granules, or prepregs (Du et al. 2010; Klein 2009). Fabrication
of green composites via compression molding and thermoforming can be divided
into following four basic steps (Fig. 3.2):
1. Material selection
2. Material preprocessing
3. Semifinished product manufacturing
4. Green composite fabrication
3 Green Composite Manufacturing via Compression Molding and Thermoforming 49

1. Material Additives Natural fibres Biopolymers

Selection

Fibre
2. Material Modification/
Preparation
preprocessing Copolymerization

Pretreatment
Drying Fibre mats/ Fibre bundles/
yarns Elementary

3. Semi-Finished
Fibre mat Compounding
Product
technology technology
Manufacturing

Sheets/ Prepregs Granules

Drying Laminates

Compression
Thermoforming Molding
4. Green Composite
fabrication

Finished Part

Fig. 3.2 Flowchart of green composite fabrication process using compression molding and
thermoforming

3.2.1 Material Selection

3.2.1.1 Material Selection Criteria

Raw material selection starts early in the product development process. Selection is
based on considerations such as cost, functional properties, and processability of
green composites (Erchiqui et al. 2009). Lower raw-material costs and lower pro-
cessing temperature for green composites have resulted in overall cost benefit to the
manufactures (Nilsson et al. 2012). Next criterion for material selection is to achieve
mechanical, physical, and thermal properties as per part specification (Gejo et al. 2010).
50 K.C. Birat et al.

Moreover, properties such as melt viscosity, specific heat capacity, thermal conductivity,
and crystallinity affect their processing (Lim et al. 2008; Menzel et al. 2013). Higher
melt viscosity can lead to problems such as unwanted molecular orientation and
internal stress in the downstream processing (Menzel et al. 2013). This property is
also critical for maintaining good flow of the melt and reducing the processing time.
Besides, specific heat and thermal conductivity of the polymer dictate how much
energy is required to heat and cool the mold during compression molding and ther-
moforming. Another material property specific to thermoforming process is the
areal draw ratio (ADR). It is defined as the ratio of area on formed part to area prior
to forming. Typical ADR value for commonly thermoformed materials ranges from
3.4 to 8.0 (Klein 2009).

3.2.1.2 Overview of Raw Materials for Green Composites

Natural fibres, polymers, and additives are common raw materials in green compos-
ites. Among natural fibre and polymers, cellulose-PLA (Frone et al. 2011; Wang and
Drzal 2012), kenaf-PLA (Ben and Kihara 2007), jute fibre-wheat gluten (Reddy and
Yang 2011), wheat gluten-cellulose, and PHA with hemp, jute, or flax (U.S. Patent
No. US20080160567 2011) were previously used. The composition of natural fibres
usually ranged from 40 to 75 % in compression molding and 15 to 50 % in thermo-
forming (Ayrilmis and Jarusombuti 2010; Takagi 2011). In case of micro- and nano-
cellulose fibres and PLA, fibre content greatly varied between 2 and 32 % (Cherian
et al. 2011; Wang and Drzal 2012). In addition to fibre and matrix, various additives
are used to enhance processing by better wetting and dispersing fibres in the poly-
mer matrix (Wang 2011). Types of additives include lubricants, dispersants, plasti-
cizers, release agents, stabilizers, and various processing aids. Based on several
studies, recommended compositions of additives were 1–5 % (by weight) for green
composites (La Mantia and Morreale 2011; Zampaloni et al. 2007).

3.2.2 Preprocessing

3.2.2.1 Fibre Preparation

Commonly, natural fibres in bales, silos, or wood chips are predigested using
mechanical, chemical, thermal, enzymatic, or combination of these methods to
separate fibre bundles (Du et al. 2010; Faruk et al. 2012; Sain and Pervaiz 2008).
Depending on the source of natural fibre, they can be categorized as core fibre,
wood fibre, seed fibre, leaf fibre, bast fibre, etc. (Faruk et al. 2012). Despite their
source, basic chemical components are cellulose, hemicellulose, and lignin (Sain
and Pervaiz 2008). Among these, cellulose fibres are more commonly used as a
reinforcement in composites (Faruk et al. 2012). Most studies use cellulose fibres
in fibre bundle form, while some refine further into elementary fibres such as
3 Green Composite Manufacturing via Compression Molding and Thermoforming 51

Fig. 3.3 Wood-based

micro-cellulose fibres after
acid hydrolysis (courtesy of
CBBP, University of Toronto)

microcrystalline cellulose (MCC) and nanocellulose (NC) for higher mechanical

properties. An example of acid-hydrolyzed micro-cellulose fibre is shown in Fig. 3.3.
In a study by Frone et al. (2011), microfibrils of cellulose were prepared by mechan-
ical grinding and solution-casting technique, while MCC were prepared by acid
hydrolysis. In another study, combination of acid hydrolysis and steam explosion
was used to isolate cellulose nanofibres from pineapple leaf (Cherian et al. 2011).
Combination of two or more pretreatment methods is recommended for higher
micro- or nanofibre yields (Immonen et al. 2013).

3.2.2.2 Drying

Drying of natural fibre and biopolymers is a crucial step in green composite pro-
cessing. Depending on the industrial setup (in-line vs. batch downstream process),
drying may be required prior to pretreatment, compounding, and/or composite fab-
rication process. Various studies suggested drying of natural fibres to 1–3 % and
biopolymers below 1 % humidity prior to processing (Ayrilmis and Jarusombuti
2010; La Mantia and Morreale 2011). La Mantia and Morreale (2011) recom-
mended that small amount of humidity may help to soften the cellulose fibre during
processing. Drying time and temperature varied greatly for natural fibre and bio-
polymers among various studies. Frone et al. (2011) dried PLA pellets and MCC
fibres in an oven for 9 h at 80 °C and 24 h at 30 °C, respectively. Other studies dried
fibres at 80 °C prior to compounding; however, the time varied between 4 and 48 h
(Sawpan et al. 2011; Zampaloni et al. 2007). For drying most natural fibres, recom-
mended drying practice is 80 °C for 4 h.
52 K.C. Birat et al.

Si-CH2

900 850 800 750

AMF

MF

4,000 3,500 3,000 2,500 2,000 1,500 1,000 500

Wavenumbers (cm–2)

Fig. 3.4 FTIR spectra of untreated (MF) and silane-treated (AMF) cellulose microfibril. Adapted
from Frone et al. (2011). Copyright 2014. By permission from John Wiley and Sons

3.2.2.3 Fibre Pretreatment

The basic principle behind pretreatment is to chemically modify the fibre surface by
binding the sizing agents or by changing the thermodynamics between fibre and
matrix (U.S. Patent No. US20080160567 2011). Various physical and chemical fibre
pretreatment methods are used to enhance interfacial bonding (U.S. Patent No.
US7208221 B2 2007). Among physical methods, homogenization and vacuum treat-
ment are used; however chemical methods are more common (Takagi and Asano
2008; Zampaloni et al. 2007). Among chemical methods, fibre treatment with surfac-
tants, alkali, acid hydrolysis, silanes, and isocyanates are more common. In a study by
Thakur et al. (2011b), cellulosic fibres were mercerized for better surface adhesion
with methyl acrylate and reduced water absorption properties. Frone et al. (2011) used
10 % APS (3-aminopropyltriethoxysilane) and acid hydrolysis to remove amorphous
regions in cellulose fibres. In Fig. 3.4, FTIR (Fourier Transform Infrared Spectroscopy)
spectra of APS-treated cellulose microfibril show the formation of Si-CH3 bond. In
another study, 7.5 % of epoxy and anhydride-based compatibilizers were used to
improve adhesion between cellulose fibre and PLA (Immonen et al. 2013).

3.2.2.4 Modification of Biopolymers

Depending on the types of biopolymers used and their application, modification is

necessary to achieve the desired processability and performance properties (Frenz
et al. 2008). Biopolymers have poor processability due to lower melt strength,
3 Green Composite Manufacturing via Compression Molding and Thermoforming 53

sensitivity to water, and lower impact strength (Imre and Pukánszky 2013; Thakur
et al. 2011a). For example, PLA and PHA have relatively lower molecular weight
and are brittle limiting their rheological properties during CM and TF (Thakur et al.
2011a). Conventional methods of polymer modification such as plasticization and
physical blending are low-cost alternatives but may not achieve desired miscibility
with biopolymers (Imre and Pukánszky 2013). In order to overcome this issue,
chemical methods such as copolymerization, grafting, and transesterification are
most widely used. Study by Okamoto et al. (2009) used various plasticizers (polyes-
ter diols) to enhance the ductility and elongation at break of PLA. Another study
used combination of chain extension and interfacial modification in PLA/TPS
blends to enhance its melt strength and the rheological properties (Li and Huneault
2011). For thermoforming of pea starch, grafting with PCL was used to enhance the
elongation to break mechanical properties and reduce the water absorption (Fig. 3.5)
(Chang et al. 2009). Some studies also used copolymers to enhance fibre dispersion
and improve mechanical properties of biopolymers. Drzal et al. (2009) used polysty-
rene (PS) to copolymerize soy protein, while Frenz et al. (2008) used chain extend-
ers (Joncryl® from BASF) for PLA, PHA, and PHB. These studies showed that
copolymerization enhanced fibre-matrix entanglement leading higher melt strength
and larger processing window during compounding and thermoforming process.

3.2.3 Semifinished Product Manufacturing

Semifinished products in CM and TF can be in the form of granules, sheets,

prepregs, or laminates (Table 3.1). Technologies involved in manufacturing semi-
finished products can be categorized into compounding and fibre mat technology.

Pea Starch
Transmittance I %

St-g-PCL(III)

1,730
C=0 in PCL

4,000 3,200 2,400 1,600 800

wavenumber / cm–1

Fig. 3.5 FTIR spectra of pea starch and grafted pea starch with polycaprolactone (St-g-PCL).
Adapted from Chang et al. (2009). Copyright 2014. By permission from John Wiley and Sons
54 K.C. Birat et al.

Typically, fibre mat technology is used with longer fibres (bast fibres of length
10–30 mm) and compounding technology for shorter fibres (wood fibre, seed fibre,
core fibre of length < 10 mm) (Faruk et al. 2012; Reddy and Yang 2011). However,
some extrusion technologies such as pull drill and pultrusion are capable of com-
pounding longer and continuous fibres (Faruk et al. 2012).

3.2.3.1 Compounding Technology

Compounding of green composites can be done via extrusion or mixing. Extrusion

is a continuous process while mixing is a batch process. Among extrusion tech-
niques, corotating twin screw extruders are commonly used for better compound-
ing of green composites (La Mantia and Morreale 2011). Drzal et al. (2009) used
this technology for producing composite sheet from soy flour and starch-based
biopolymers. Temperature range was 95–130 °C and screw speed was 100 rpm
(U.S. Patent No. US20060043629 A1 2009). Author also recommended maintain-
ing processing conditions during extrusion if biopolymers are copolymerized
with other biodegradable polymers due to their high susceptibility to denaturing. In
another study, melt extrusion was used to make composite sheets from laminated
PHA with woven natural fibre (U.S. Patent No. US20080160567 2011). Among
mixing technologies, dry blending is the most common method for mixing poly-
mer, additives, and natural fibre (Ayrilmis and Jarusombuti 2010; Benthien and
Thoemen 2012). This technique is simple and cost-effective but lacks even distribu-
tion of raw materials. Frone et al. (2011) used two-roll mill Brabender mixer to
produce composite granules at 165 °C and rotor speed of 27 and 22.5 rpm. Another
study used low-intensity mixture such as ribbon blender to compound cellulose and
PVC (U.S. Patent No. US6971211 B1 2005). Some study also used pre-blended
granules of natural fibre and polymer (Benthien and Thoemen 2012).

3.2.3.2 Fibre Mat Technology

In this process, fibre mat or yarns are impregnated with thermoplastic or thermoset
resins to form sheets or prepregs (Du et al. 2010). Unlike conventional glass fibres,
natural fibres are not usually supplied in rovings or yarns. For manufacturing
micro- or nanocellulose and PLA composite sheets, studies suggested using
homogenization technique followed by membrane filtration and drying (Takagi
2011; Wang and Drzal 2012). Study by Kim et al. (2010a) reported use of a carding
method to form natural fibre mat for making composite sheets. In the process, PLA
and PP fibre (30 mm long) and natural fibre (50–70 mm long) were carded together
to form webs, needle punched and pre-pressed at 120 °C to form a prepreg mat. In
another method, alternate layers of polypropylene (PP) powder (400 μm) and short
kenaf fibre were used to form a composite sheet (Zampaloni et al. 2007). PP pow-
der was sprayed evenly over kenaf fibre and pressed using Carver Laboratory Press.
For nonwoven mats with longer fibre (10–50 mm), Nechwatal et al. (2005) reported
3 Green Composite Manufacturing via Compression Molding and Thermoforming 55

Fig. 3.6 Composite sheet fabrication from nonwoven mats using spraying method. Reprinted from
Nechwatal et al. (2005). Copyright 2014. By permission from Wiley-VCH Verlag GMBH & CO

three methods for fabricating composite sheets. Polymers could be sprayed,

powdered, or added in fibre spinning process. Method for fabricating composite via
spraying polymer into nonwoven natural fibre mat is shown in Fig. 3.6. Khondker
et al. (2006) developed a micro-braiding method for continuous yarns of jute and
PLA. In this method, composite yarns were wounded in metallic frame to form a
mat for compression molding. In a study by Takemura (2010), woven jute fibre
sheets were used to make preforms and impregnated with PVA resin to form com-
posite laminate.
In conventional compression molding, SMC (sheet molding compound) and
BMC (bulk molding compound) prepregs are formed using thermosetting resin such
as unsaturated polyester (UPE), additive and glass-fibre reinforcement, or filler (Du
et al. 2010). Recently, SMC technology has been developed for manufacturing green
composite sheets with thermoplastic resin. In a patented method developed by Drzal
et al. (2009), chopped natural fibres were fed (via vibratory feeder) into the carrier
film where thermoplastic resin was sprayed and pressed with compression roller to
make continuous sheets. Author also developed another method for making prepregs
from natural fibres and UPE (U.S. Patent No. US7208221 B2 2007). In the process,
dried layer of natural fibres of moisture content less than 10 % was carried in a first
film and mixed with the second film carrying catalyzed polyester resin. Inventor
recommended that prepregs must be stored in refrigerated temperatures before com-
pression molding into a final part. In another study, prepregs were made from jute
fibre mat that was evenly sprayed with wheat gluten (Reddy and Yang 2011).

3.2.4 Green Composite Fabrication

3.2.4.1 Compression Molding

In compression molding (CM), semifinished products such as sheets or prepregs are

used to manufacture finished parts. For sheets and prepregs, most studies used alter-
nate stacking method to compression molding of green composites (Du et al. 2010;
56 K.C. Birat et al.

Fig. 3.7 Compression molding of kenaf and PLA via alternate stacking. Reprinted from Ben and
Kihara (2007). Copyright 2014. By permission from Trans Tech Publications

Ma and Joo 2010; Reddy and Yang 2011). Study by Ben and Kihara (2007) used
alternate stacking of kenaf fibres and PLA sheets for fabricating composite lami-
nates (Fig. 3.7). Similar processing was used by Ma and Joo (2010) for fabricating
jute and PLA composites. Processing steps varied on the type of materials and the
number of alternate stacking. For kenaf and PLA sheets, processing steps involved
melting at 10 MPa pressure for 10 s, holding at 1 MPa for 20 min, and impregnation
at 10 MPa for 10 s. Platen temperature throughout the process was maintained at
185 °C (Ben and Kihara 2007). In contrast, fabrication of CM cellulose and PLA
sheets involved two steps: pre-pressing and pressing. During pre-pressing, 5 MPa
of pressure was applied for 3 min followed by 15 MPa of pressure for 2 min, and
the platen temperature was maintained at 165 °C (Frone et al. 2011). Number of
alternate sheets or prepregs depends on the thickness of individual sheets or pre-
pregs and the thickness of the finished part. Five mats with alternating UPE resin
were stacked prior to molding to achieve 3 mm thickness of the composite lami-
nates (Du et al. 2010). Some study also used prepregs for fabricating green com-
posites. In a study by Du et al. (2010), prepregs of kenaf and polyester resin were
compression molded to form composite laminates (dimension = 102 × 178 × 3 mm)
at 175 °C. Processing steps involved pressing at 5 MPa for 10 s and turning of heat.
It was followed by constant pressure of 5 MPa for 1 h until the temperature of the
mold was cooled to 100 °C (Du et al. 2010). Reddy and Yang (2011) also used
prepreg of jute fibre and wheat gluten to form composite laminate. A composite
press was used at temperature range of 150–180 °C for 5–20 min at 140 MPa of
pressure followed by cold-water cooling and laminate removal (Reddy and Yang
2011). In these studies, release agents (silicon) and wax papers were used to avoid
contacts between the material and mold platen (Ayrilmis and Jarusombuti 2010; Du
et al. 2010).
In CM, curing time, curing temperature, and clamp pressure are the important
process parameters that need to be optimized for the desired part (Onal and Adanur
2005). Few studies were found in optimizing processing parameters for green or
3 Green Composite Manufacturing via Compression Molding and Thermoforming 57

bio-based composites. Ben and Kihara (2007) investigated in optimizing melt

temperature, holding time, and impregnation time of kenaf and PLA composites.
Based on the mechanical properties of fabricated composites, combination of melt
temperature of 185 °C and holding time of 15 min were optimal for kenaf and
PLA composites. For impregnation time, 30 s was recommended time for quasi-
isotropic lamination. However, volume fraction of both fibre and PLA was not
reported in the study which is an important consideration for optimizing processing.
In another study, influence of press temperature on panel properties was investi-
gated (Benthien and Thoemen 2012). Based on physical and mechanical properties
of wood flour and polypropylene panels, optimal press temperature was 210 °C.
This temperature is high for natural fibres and may result in fibre degradation.
Reddy and Yang (2011) also studied effects of molding (holding and impregnation)
time and temperature on wheat gluten-jute fibre composites. Results showed that
molding time and temperature of 170 °C and 15 min produced the maximum flex-
ural properties. Overall, curing temperature green composites should be in range of
150–180 °C while pressure and time varies with the type of material used and the
thickness of the sheets or prepregs.

3.2.4.2 Thermoforming

Prior to thermoforming, drying of semifinished green composites is required to avoid

blemish defects on the finished parts (U.S. Patent No. US20130331518 A1 2013). In
thermoforming process, composite sheets are roll fed or precut depending on their
thickness (Klein 2009). For precut sheets, clamping frame is used to avoid twisting
and warping. Next, sheets are heated to its softening temperature (Tg) via convection
or radiant heaters located on one or both sides of the sheets (Zampaloni et al. 2007).
Prior to forming process, preheating is recommended to eliminate risk of material
shear and premature fracture as a result of rapid cooling from ambient temperature
(Lim et al. 2008; Zampaloni et al. 2007). Hence, the recommended steps in thermo-
forming green composites are load/unload, preheat, heat, and forming (Klein 2009).
A thermoforming machine with thermoformed part is shown in Fig. 3.8.
Studies in thermoforming green composites used prepregs of cellulose fibre
(40–70 % w/w) and thermoplastic (U.S. Patent No. US8012389 B2 2009), sheet
laminates of cellulose (17 % w/w), sheets of PLA (Lim et al. 2008), and composite
sheets of kenaf and polypropylene (Zampaloni et al. 2007). Forming method and
processing parameters of these composites were slightly different. In a patented
method developed by Immonen et al. (2013), cellulose and PLA composite sheets
(width 10 cm) were dried and pressed at 185 °C for 3 min (U.S. Patent No.
US20130331518 A1 2012). Study by Lim et al. (2008) recommended the thermo-
forming temperature in the range of 80–110 °C and use of aluminum (Al) molds for
lower faster thermoforming cycles. Another study on processing parameters opti-
mization of kenaf and polypropylene showed optimal forming temperature, die
temperature, heating time, and the draw depth as 190 °C, 165 °C, 15 min, and
50.8 mm, respectively (Zampaloni et al. 2007). Authors also suggested that these
composite sheets have better formability due to less wrinkling and distortions.
58 K.C. Birat et al.

Fig. 3.8 Thermoforming machine with a thermoformed coffee cup lid (courtesy of CBBP,
University of Toronto)

3.3 Commercial Green Composite Semifinished Products

Over the past few years, there has been significant growth in compression-molded
and thermoformed products using green composites. FuturaMat has developed
thermoformable green composites BioCeres® and BioFibra® (FuturaMat© Website:
Our Plastics n.d). BioCeres® is made from corn-based thermoplastic starch (TPS)
and wheat flour, while BioFibra® is made from TPS and spruce wood flour.
Similarly, ©Polyfea has developed Caprowax P™ from cellulose and TPS for ther-
moforming applications (POLYFEA Polymer 2009). It claims that these com-
pounds do not require pre-drying and recommends processing at lower shear rates
and pressures. Some examples of commercial green composites and their process-
ing parameters are summarized in Table 3.2.
Other commercial examples include natural fibres with polyolefins. FlexForm
Technologies has developed nonwoven mats and panels for CM and TF based on
natural fibres reinforced with polypropylene matrix, while Composites Evolution
has developed prepregs using flax fabric and polyolefins for CM (Fig. 3.9).
Composites Evolution has recently developed a prepreg from flax fabric and
PLA. Their current automotive application includes package trays, door panels,
headliners, seat backs, trailer side walls, pillars, etc. These panels are thermo-
formed at 200 °C and 0.379 MPa pressure using matched metal cooling (Gardiner
2006). Solvay industries also produced Gonaf® and Technogor® sheets using
sisal fibres and PP matrix for use in CM and TF application (Gardiner 2006).
Recommended processing methods for these sheets were heating at 180–190 °C
for 50 s and applying pressure of 0.786–0.979 MPa pressure for 40 s. Example
of compression-molded door panel and thermoformed seat back is shown in
Fig. 3.10.
3 Green Composite Manufacturing via Compression Molding and Thermoforming 59

Table 3.2 Processing method for some commercial green composites and biopolymersa
Trade name/ Form/
material processing Processing
SN composition method Properties parameters
1 Cereplast®6000 Pellets/sheet MFR: 3.0 g/10 min Drying: 2–4 h @
PLA extrusion and Ten. str @ yield: 49.6 MPa 71–82 °C
thermoforming Flex. mod: 3.79 GPa Cyl. temp:
Elong. @ brk: 9.0 % 154–174 °C
HDT @ 0.45 MPa: 51.1 °C Melt temp: 194 °C
2 Mirel™ P3001/ Pellet/sheet Ten. str @ yield: 19.0 MPa Drying: 4 h @
F3002 extrusion and Flex. mod: 1.48 GPa 80 °C
PHA thermoforming Elong. @ brk: 13 % Cyl. temp:
HDT @ 0.45 MPa: 116 °C 165–175 °C
Melt temp:
165–170 °C
3 Biocycle®189C-1/ Powder/sheet MFR: 15 g/1omin Drying: 4 h @
PHB extrusion and Ten. str @ yield: 30 MPa 50 °C
thermoforming Flex. mod: 2.6 GPa Cyl. temp:
Elong. @ brk: 2.2 % 140–170 °C
HDT @ 0.45 MPa: 120 °C Melt temp: 170 °C
4 Caprowax Granules/ MFR: 2–6 cm3/10 min No drying required
P™6006-11-000 thermoforming Vicat softening temp: 56 °C Cyl. temp:
granulat/cellulose 80–150 °C
fibre and TPS Melt temp:
90–120 °C
Thermoforming
temp: 75–85 °C
5 BioCeres® Pellets/ MFR: 8.1 g/10 min N/A
BC-LBE01/ thermoforming Ten. str @ yield: 32.6 MPa
TPS and wheat Flex. mod: 3.3 GPa
Elong. @ brk: 2.9 %
HDT @ 1.8 MPa: 41 °C
6 Plantic® R1/ Film/ Ten. str: 42–46 MPa Glass transition
TPS thermoforming Elong. @ brk: 20–36 % temperature:
Elmendorf tear str: 40–50 °C
3,500–5,500 g Vicat softening
Film thickness: 300–550 μm temperature:
130–135 °C
a
All data are available at UL IDES Prospector http://www.ides.com/

3.4 Summary

Green composites are made from 100 % renewable and low-cost materials
compared to conventional materials. They offer practical solutions to growing envi-
ronmental and economic concerns in the development of new products. However,
fabrication of green composites via compression molding and thermoforming is
different to traditional polymer composites mainly due to changes in rheological
behavior, thermal instability, and chemical and morphological differences in natural
60 K.C. Birat et al.

Fig. 3.9 Examples of commercial green composite semifinished products: (a) nonwoven bast
fibres and polyolefin mat from FlexForm Technologies and (b) flax-fibre prepregs. Reprinted with
permission from Composite Evolution (Composite Evolution: www.compositesevolution.com)

Fig. 3.10 Commercial examples of green composites: (a) thermoformed automotive seat back
with FlexForm® (FlexForm Technologies, website: www.flexformtech.com) and (b) compression-
molded automotive door panel from Fibrowood® (Johnson Controls, website: www.johnsoncon-
trols.com)

fibres and biopolymers. Hence, specific processing guidelines must be followed for
manufacturing green composites. Processing steps involves four main steps: mate-
rial selection, preprocessing of fibre and/or biopolymers, manufacturing of semifin-
ished products, and part manufacturing. In material selection, raw materials are
selected based on functional properties and processability of materials. For process-
ability, properties such as melt viscosity, specific heat capacity, thermal conductiv-
ity, and crystallinity of materials. Once the materials are selected, fibre and polymers
need to be preprocessed. Preprocessing involved fibre pretreatment, modification of
biopolymer, and drying. Next step is to manufacture semifinished products such as
granules, prepregs, sheets, or laminates via compounding or fibre mat technology.
3 Green Composite Manufacturing via Compression Molding and Thermoforming 61

In the final step, composite parts are manufactured using semifinished products. In
each of these steps, careful attention in regard to moisture and thermal degradation
of green composite must be given.
In recent years, there has been increasing number of green composite products in
the market. It is expected that green composite market will continue to progress as
long as tighter government environmental regulation around the world continues to
influence corporate goals toward the use of more sustainable and environmentally
friendly materials in their new product designs.

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