Advances in Building Technology, Volume 1 225
M. Anson, J.M. Ko and E.S.S. Lam (Eds.)
© 2002 Elsevier Science Ltd. All rights reserved
LOW-COST, BIO-BASED COMPOSITE MATERIALS FOR
HOUSING APPLICATIONS
L.T. Drzal, A. K. Mohanty, G. Mehta, M. Misra
Composite Materials and Structures Center
Dept of Chemical Engineering and Materials Science
Michigan State University, East Lansing, Michigan, USA, 48824
ABSTRACT
In an on-going project, sponsored by the National Science Foundation, to develop bio-based
composite materials for the next generation of American housing panel applications, a group of
researchers at Michigan State University are striving to generate eco-friendly greener composite
materials for structural applications. The objective of this research is to determine if bio-composites
designed and engineered from natural/bio-flbers and blends of polyester resin and derivitized soybean
oil can replace existing glassfiber-polyestercomposites for use in housing structures. Bio-composites
provide environmental gains, reduced energy consumption, lighter weight, insulation and sound
absorption properties, elimination of health hazards and reduce dependence on petroleum based and
forest product based materials. A three cornered approach including the use of engineered natural
fibers, polymer resin modification and development of a new high volume continuous manufacturing
processes(Bio-Composite Sheet Molding Compound Panel-BCSMCP) is required to achieve the
objective of producing an affordable alternative construction material for the housing industry of the
21st century.
KEYWORDS
Housing Panels, Biocomposites, Unsaturated Polyester Resins, Derivitized soybean oil
INTRODUCTION
1000/T
Contemporary housing needs are challenging designers
and builders to utilize more inventive materials in order %
to provide housing that are environmentally benign and at |
the same time provides for the requisite occupant **
environment and operating efficiency. Increasing
attention is turning to bio-based materials from renewable
resources. The future for bio-based building materials is
•ill ill
Industrial/
Consumer
bright (Figure 1, refl) and several new agricultural
natural fiber-based building materials are already making Figure 1: Growth Outlook For Bio-
based Composites by Application
in United States, 2000-2005
226
their mark in the building industry. Natural fiber composites (bio-based composite materials) are
economical commodity composites that have useable structural properties at relatively low cost. The
manufacture, use and replacement of conventional building materials (e.g. petroleum-based plastics,
glass fibers, etc.) are becoming priorities because of the growing environmental consciousness . There
is a growing interest in the use of natural/bio-fibers as reinforcing components for thermoplastics and
thermosets. Advantages of natural fibers over traditional reinforcing fibers such as glass and carbon
are: low cost, low density, acceptable specific properties, ease of separation, enhanced energy
recovery, CO2 sequesterization and biodegradability. Although thermoplastics have the added
advantage of recyclability, thermosets have the necessary mechanical properties for use as structural
bio-composites. Bio-composites derived from natural fibers and traditional thermoplastics or
thermosets are not fully environmentally friendly because matrix resins are non-biodegradable.
However these bio-composites do now maintain a balance between economics and environment
allowing them to be considered for applications in the automotive, building, furniture and packaging
industries.
The use of reinforced thermoset composites by automakers has nearly doubled in the last decade, and
is expected to increase 47 percent during the next five years3 through 2004. The majority of resins
REINFORCING NATURAL FIBERS/FILLERS
WOOD
NON-WOOD NATURAL/BIO-FIBERS FIBERS
STRAW
FIBERS
rn
I BAST 11 LEAF || SEED/FRUIT | FIBERS
GRASS
1
Examples:
I Examples:
Kenaf, Flax, Examples: Soft and
JuteJIemp Cotton, Coir Hard Woods
Examples: Examples: Examples:
Corn/Wheat Sisal, Henequen, Bamboofiber^Switchgrass,
/Rice Straws Pineapple Leaf Fiber Elephant grass etc.
Figure 2: Broad classification of Natural/Bio-fibers: Strong potential reinforcing fibers
in designing bio-composites for Building Products Industry
used in the composite industry are thermosets4. About 65% of all composites produced currently for
various applications; use glass fiber and polyester or vinyl ester resins. Unsaturated polyester (USP)
resins are widely used, thanks to a relatively low price, ease of handling and a good balance of
mechanical, electrical and chemical properties. Natural fibers have recently made a comeback in FRP
(fiber reinforced plastics) to replace glass fiber in many applications such as automotive and building
products. The engine and transmission covers of Mercedes-Benz transit buses now contain polyester
resin reinforced with natural fiber5. Natural fiber reinforced polyester composites have received much
commercial success in the infrastructure area primarily for low cost housing applications.
There is, however, a major drawback associated with the application of bio-fibers for reinforcements
of organic matrix resins. Due to the presence of hydroxyl and other polar groups on the surface and
227
throughout bio-fibers, moisture absorption can be high which leads to poor wettability by the matrix
resin and weak interfacial bonding between fibers and hydrophobic matrices. In order to develop
composites with better mechanical properties, it is necessary to impart hydrophobicity to biofibers by
suitable chemical treatments6.
The mechanical behavior of fiber, the types of fiber (non-woven, woven, short/long fibers), the nature
of matrix, and fiber-matrix adhesion play vital role in controlling the properties of composites. This
paper gives an overview of natural fiber reinforced polyester composites highlighting the future
aspects of such bio-based composite materials in building applications.
REINFORCING NATURAL/BIO-FIBERS
Plastics, by themselves are not fit for
load bearing application due to their
lack of strength, stiffness and
dimensional stability. However
fibers possess high strength and
sufficiently stiffness but cannot be
used for load bearing applications
because of their fibrous structure. In
fiber-reinforced composites, the
fibers serve as reinforcement by
giving the strength and stiffness to
the structure. Bio-fibers may be
classified in two broad categories:
Non-wood fibers and Wood fibers
(Fig. 2). Interest in the use of non-
wood cellulose fibers in plastic
composite structures has increased
Figure 3. Various Sources for BioFibers. rather dramatically in recent years.
The non-wood bast (from the stem
part of the plant) fibers are poised to be utilized to a greater extent than wood fibers in bio-composite
housing structures. The best-known
examples are: (i) bast fibers: flax, ramie, 9"*°".
kenaf7mesta, hemp and jute (ii) Leaf fibers:
sisal, pineapple leaf fiber (PALF), and
henequen (iii) seed fibers: cotton; fruit
fibers: coconut fiber i.e. coir. (Fig.3) All
natural fibers (wood and non-wood) are
lingo-cellulosic in nature with the basic
components being cellulose and lignin
(Fig. 4). The density (g/cm3) of
natural fibers (varies from -1.2-1.5) is much
less than that of E-glass (2.55); the specific
strength of natural fibers is quite
comparable to glass fibers. The elastic
modulus and specific modulus7 of natural
fibers are comparable or even superior to
E-glass fibers (Table 1 and Fig. 5).
Figure 4: Structure of Cellulose (shown top) and lignin
(shown bottom): basic constituents of natural fibers
228
POLYESTER RESIN MATRIX POLYMERS FOR BIO-COMPOSITES
The polyester resins, because of their versatility and low cost, are widely used in polymer composites.
_ „ . _ , , . -_ . , ^ + Polyester resins are classified
Table 1: Modulus comparison of E-glass and some important ( S c h e m e i) 33- (i) o r t h 0 resins
Natural Fibers (after ref 6 and partially modified; (ij) ^ ^ ^ bisphenol.A:
fumarates, (iv) chlorendics,
Fiber Density Elastic Specific and (v) vinyl ester. Ortho-
Type (g/cm3) Modulus modulus resins, known as general-
(GPa) purpose polyester resin, are
E-glass 2.55 73 29 based on phthalic anhydride,
Hemp 1.48 70 47 maleic anhydride and glycols
Flax 1.4 60-80 43-57 (Scheme 2). Ortho-resin is the
Jute 1.46 10-30 7-21 least expensive among all the
Sisal 1.33 38 29 polyester resins. The solutions
Coir 1.25 6 5 of unsaturated polyesters and
Cotton 1.51 12 8 styrene vinyl monomers
Unsaturated Polyester Resins 1
1
4 I I i A
|Bisphenol-Al
Ortho 1 Vinyl ester
1 Isoresins 11 fumarates 1 IChlorendicsl
resins 1 1 resins
E-gass Hemp
5- General purpose polyester resins
Figure 5: Modulus and Specific modulus:
E-glass vs. some Natural Fibers Scheme 1: Unsaturated Polyester resins—Classifications
(reactive diluents) are known as unsaturated polyester (UP) resins. Considerable work has been
reported on the synthesis, characterization, and curing behavior of UP resins8. The curing reaction of
UP is a free-radical chain growth polymerization between reactive diluents styrene and UP resin. A
wide range of peroxides, azo and azine
o CH3 - C H - C H i
I I
compounds can be used as initiators,
depending on the curing temperature. For
room temperature curing as in the case of
Phthalic Anhydride Maleic Anhydride Propylene glycol hand-lay-up structures, methyl ethyl ketone
peroxide (MEKP) is used; for moderate
O
II
temperature curing benzyl peroxide is used.
C - O - C H -CH - O - C - C H = C H - C - O - C H -
2
I
For high temperature processing, di-t-butyl
2 CH —'n peroxide or t-butyl perbenzoate is used. A
mixture of initiators is used when a large
Preparation of Polyester Resin temperature increase is expected. To
e ^ „ accelerate the decomposition of peroxides,
Scheme 2 *
some metal compounds, tertiary amines, and
mercaptans can be used. Cobalt naphthenate (CoNp) and cobalt octanoate (CoOc) are the most widely
used accelerators.
229
OUR APPROACHES TO STRUCTURAL BIO-BASED COMPOSITE MATERIALS FOR
HOUSING APPLICATIONS
Natural fiber composites are emerging as a realistic alternative to glass-reinforced composites. While
they can deliver the same performance for lower weight, they can also be 25-30 percent stronger for
the same weight Research
success from our lab.-scale
BIO-COMPOSITE experiments of our group9"11
PROCESSINGS has shown that it is possible
to produce bio-composites
with properties that can
compete with glass fiber
EFFICIENT reinforced composites.
MATRIX
BIO-FIBER Natural fiber (NF)
POLYMER
SURFACE unsaturated polyester (UP)
MODIFICATION
TREATMENTS composites show lower
density, equal flexural
modulus, comparable
flexural strength but
HIGH PERFORMANCE relatively poor impact
BIO-COMPOSITE strength as compared to a
FORMULATION glass fiber (GF)
composites12. Our three-
pronged approach to
Figure 6: Design of superior strength Bio-Composite-Approaches designing superior strength
(Fig. 6) bio-composites for
housing structures includes:
• An efficient (low cost but effective) bio-fiber surface treatment
• Matrix modification (Blending withfiinctionalizedvegetable oil)
• New, property-enhancing bio-composite process - - Sheet Molding Manufacturing.
Bio-fiber treatments and Design of "Engineered Natural/Bio-fibers"
Design of "Engineered Natural/Bio-
fiber" is schematically represented in
I Kenaf I Fig. 7. Engineered bio-fibers" are
rl IHempH
Surface II
treated: 1
KENAF/ 1 1 blends of kenaf ,
"Engineered
Bio-fibers"
defined as a blend of surface treated bast
(e.g. Kenaf, Hemp) and a leaf fiber (e.g.
HEMP/
i
Li 1 Hemp, & PALF: ready for Pineapple leaf fiber, PALF). Selection
•r
1
PALFM
PALF 1
1 composite
fabrications
of blends of bio-fibers is also based on
the fact that the correct blend achieves
an optimum balance in mechanical
properties. The Kenaf and/or Hemp
Figure 7: Design of Engineered Natural/Bio-fiber based composites exhibit excellent
tensile and flexural properties, while
leaf fiber (PALF) composites give the
best impact properties of the composites. A blended composition of two bast and one leaf fiber is
selected to achieve a balance of flexural and impact properties of the targeted bio-composites. Alkali
treatment (AT) of natural fibers appears to be a very promising treatment, having the right
combination of surface chemical and structural benefits along with low cost. The alkali treatment
enhances the biofiber surface roughness, causes surface fibrillation and thus drastically improves
230
fiber-matrix adhesion. An increase in strength for bio-composites can also be achieved through the use
of silane treatment. However, the choice of the correct silane coupling agent and treatment conditions
all play a vital role in achieving superior strength composites. A general compatibilization mechanism
for silane treated natural cellulose fiber and polymer resin composites is represented in Scheme 3.
Matrix modification (Blend of polyester resin and derivitized vegetable oil)
Unsaturated polyester resin is petroleum-based and is not eco-friendly. Attempts are in progress in our
group to replace polyester resin with vegetable oil based resins. Through successful blending of
petroleum-based polyester resin and derivitized soybean oil we are developing a number of bio-based
R— S i ( 0 C H 3)3+ 3 H 2 0 R - S i (O H ) 3 + 3 C H 3 O H
3R - S i (OH)3
—2 H 2 0 Condensation
R
*
H O - S i —O -S, i — O - S j i - 0 H
6H OH OH
H
H ydrogen
bond
9 HO HO
l_
C e llulose
form a t i o n
( N a t u r a l fiber)
C ellu l o s e
X
H* > H; H H; NH
V
HO—Si—O —
V S i — O —Si
V OH
R k R
Heat 1- H20
C ellulose
1
0
6 0 Scheme 3
1 1
H O 1 - O — S i — 0 — S i -— O H
—Si -
1 k
P O L Y M E R R E S IN
k
R
1 J
resins for producing bio-composites. Combining a suitable reinforcement with a properly modified
resin blend of polyester and vegetable oil will result in a novel bio-composite material. The
incorporation of derivitized vegetable oil into polyester resins can improve the toughness of the resin
and the resulting bio-composites. The content of derivitized vegetable oil and varying curing agent
composition will affect the overall performance of the materials. Optimally maximizing the
concentration of derivitized soybean oil under accurate curing conditions and incorporating suitably
surface treated natural fibers will launch a new generation of eco-friendly bio-composites for housing
applications.
Bio-Composite Processing
Bio-composites can now compete with glass-polyester composites both on a cost and performance
basis. Most of the existing results on bio-composites are based on hand-lay-up labscale fabrication
techniques. However the success of a high volume processing technique will be necessary to produce
bio-composites in composite panels for housing applications economically. We have created a
unique new process for fabrication of bio-composites. This process is similar to the Sheet Molding
Compound (SMC) process but is a new and necessary approach for bio-composites.
231
SMC type of materials are often used in semi-structural components. The short production cycle times
and the excellent surface appearance of some grades make it attractive as a panel material. Stronger
SMC type material can be developed, mainly by incorporating high fiber contents. A schematic
representation of a high volume bio-composite processing in making bio-composites from chopped
Polyester
Polyester
Resin/filler paste Resin/filler paste
Carrier Film
m
[J « — Chain Link
Compaction Belt
& on line Curing
.^ processl
Carrier Film PANEL
Belt Drive
Figure 8: Schematic of Continuous Bio-Composite Sheet Molding Compound Panel
(BCSMCP) Manufacturing Process being developed at Michigan State University
natural/bio-fiber and polyester resin or resin/filler paste is shown in Fig. 8. Polyester resin in
combination of CaC(>3 filler is required to be blended with biofibers to produce structural quality low
cost housing panels.
CONCLUSIONS
New environmental regulations and societal concerns have triggered the search for new products and
processes that are compatible with the environment. The incorporation of bio-resources into
composite materials can reduce dependency on petroleum reserves. American market studies clearly
identify the potential impact and opportunities for natural fiber composites. Natural fiber composites
have the potential for major applications in building products. The majority of such applications
include natural fiber-thermoplastic composites for applications like decking, window/siding/railing,
flooring, furniture and automotive interiors. The vast majority of this market volume deals with wood
fiber and remainder is comprised of non-wood agricultural natural fibers like kenaf, hemp and flax.
Wood-fibers cannot impart the required strength for paneling applications, so our efforts target to use
non-wood bast and leaf-based natural fibers. Natural fiber - thermoset composites show improved
mechanical properties over thermoplastic-based bio-composites and such properties are required for
paneling applications. In the U.S., current housing panels made from glass fiber - polyester composite
contains -10-20% glass fiber. Since natural fibers are less expensive (~ 25-30 cents/lb. in North
America) than both glass fiber and PE resin, incorporation of the maximum permissible amount of
inexpensive natural fibers into the composite structure would not only provide immense economical
benefit, but also would result in housing structures with maximum permissible content of renewable
resource based natural fibers. The impact/stiffness balance of bio-composites needs to be solved
through the combination of bio-fibers (hybrid of bast and leaf fibers) and matrix modification through
blending with derivitized vegetable oil. The future for bio-composites ("GREENER" than exiting
232
glass composites) is bright because of the shortage of landfill availability, difficulty in recyclability of
fiber glass composites, and the uncertainty of petroleum price/availability. Achieving this unique
balance of mechanical properties and environmental benefits will create new markets for bio-
composites for 21st century building product applications.
ACKNOWLEDGEMENTS
Financial support was [provided from the National Science Foundation (NSF) under Partnership for
Advancing Technologies in Housing (PATH), 2001 Award # 0122108.
REFERENCES
1. Harris, T. (2001). Trends In New Filler And Reinforcement Technologies For Plastic Composites,
Conference on Functional Fillers, San Antonio, TX.
2. Mohanty, A. K., Misra, M.. and Hinrichsen, G. (2000)Macromol Mater. Sci. 276/277,1.
3. Composite Week Newsletter, (2000) 10(2).
4. Composites Technology, (2000).
5. DaimlerChrysler HighTech Report (1999), 88.
6. Mohanty, A K., Misra, M. and Drzal, L. T, (2001) Polym. Interf. 8(5), 313.
7. Brouwer, W. D., (2000). Natural Fiber Composites: Where Can Flax Compete with Glass ?,
SAMPE Journal, 36(6), 18.
8. M. Malik, V. Choudhary, I. K. Varma, J. Macromol. Sci. - Rev. Macromol. Chem Phys; C40
(2&3), 139 (2000).
9. Mohanty, A. K. , Misra, M. and Drzal, L. T, (2001). Surface Modification of Natural Fibers to
Improve Adhesion As Reinforcements for Thermoset Composites, Proceedings of the 24th Annual
Meeting of the Adhesion Society - Adhesion Science for the 21st Century" 418-420.
10. Mohanty, A. K. , Misra, M. and Drzal, L. T., (2001). Environmentally Benign Powder
Impregnation Processing And Role Of Novel Water-Based Coupling Agents In Natural Fiber-
Reinforced Thermoplastic Composites, Polymer Preprint - Polymer Chemistry Division, ACS,
42(2), 31
ll.Belchler, L., Drzal, L. T, Misra, M. and Mohanty, A. K. (2001) Natural Fiber Reinforced
Thermoset Composites: Studies on Fiber-Matrix Adhesion of Aligned Henequen Fiber - Epoxy
Composites Polymer Preprint - Polymer Chemistry Division, ACS, 42(2), 73.
12. Schloesser, T., (2000). Natural Fiber Composites in Automotive Applications, 3rd International
Symposium- Bioresource Hemp & other fiber crops, Wolfsburg, Germany.