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A review on new bio-based constituents for natural fiber-polymer composites

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 Journal of Cleaner Production 149 (2017) 582e596

Contents lists available at ScienceDirect

Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Review

A review on new bio-based constituents for natural fiber-polymer

composites
€nen a, *, Oisik Das b, Laura Tomppo a
€isa
Taneli Va
a
Department of Applied Physics, University of Eastern Finland, 70211, Kuopio, Finland
b
Department of Civil and Environmental Engineering, Centre for Advanced Composite Materials (CACM), University of Auckland, Auckland, 1142, New
Zealand

a r t i c l e i n f o a b s t r a c t

Article history: Composite materials based on renewable agricultural and biomass feedstocks are increasingly utilized as
Received 17 November 2016 these products significantly offset the use of fossil fuels and reduce greenhouse gas emissions in com-
Accepted 18 February 2017 parison with conventional petroleum-based materials. However, the inclusion of natural fibers in poly-
mers introduces several challenges, such as excess water absorption and poor thermal properties, which
need to be overcome to produce materials with comparable properties to the conventional composite
Keywords:
materials. Instead of using rather expensive chemical and physical modification methods to eliminate
Biochar
these aforementioned challenges, a new trend of utilizing waste, residues, and process by-products in
Biocomposite
Natural fibers
natural fiber-polymer composites (NFPCs) as additives or reinforcements may bring considerable en-
Polymer-matrix composites (PMCs) hancements in the properties of NFPCs in a sustainable and resilient manner. In this paper, the effects of
Mechanical properties waste materials, residues or process by-products of multiple types on NFPCs are critically reviewed and
Waste their potential as NFPC constituents is evaluated.
© 2017 Elsevier Ltd. All rights reserved.

Contents

1. Introduction and background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 582

2. Challenges associated with NFPCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 584
2.1. Limited mechanical properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 585
2.2. Excess water absorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 585
2.3. Poor thermal properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 587
2.4. Processing and homogeneity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 587
3. Approaching the challenges with bio-based alternatives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 588
3.1. Biochar . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 588
3.2. Lignin . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 590
3.3. Sewage sludge . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 591
3.4. Animal fibers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 591
3.5. Hybridization with multiple fiber types . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 592
4. Future trends . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 593
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 594

1. Introduction and background

In response to the consumers’ demands for lighter-weight, en-

ergy-efficient, carbon sequestering and more sustainable materials,
* Corresponding author. industries are focusing more and more on materials based on
€isa
E-mail address: taneli.vaisanen@uef.fi (T. Va €nen). renewable resources (Fiksel, 2003; Stokke et al., 2014). Ecological

http://dx.doi.org/10.1016/j.jclepro.2017.02.132
0959-6526/© 2017 Elsevier Ltd. All rights reserved.
 €isa
T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596 583

concerns such as environmental safety and recyclability have also

resulted in an increasing interest in green materials (Sain and
Panthapulakkal, 2004). Furthermore, the need to find new alter-
natives for materials derived from non-renewable resources is
strongly present at the level of policy generation. The governmental
considerations seem to be aligning to create an environment for
producing more advanced products from various types of bio-
masses (Winandy et al., 2008).
Natural fiber-polymer composites (NFPCs) have a status of
renewable and sustainable materials since they are composed of
natural fibers embedded in a polymer matrix, which may be also of
biological origin (e.g. polylactic acid, PLA) (Va€isa
€nen et al., 2016).
Natural fibers are derived either directly from agricultural sources
or as a processing or production residues when crops are processed
for their primary uses, such as nutrition (Bassyouni and Waheed Ul
Hasan, 2015). Examples of natural fibers used in NFPCs include
wood, jute, hemp, kenaf, sisal, coir, flax, bamboo and fruit fibers.
Matrix materials of NFPCs can be classified into thermosets and
thermoplastics, and further into non-degradable and biodegrad-
able polymers (Puglia et al., 2005). NFPCs with non-degradable
thermoplastics cannot undergo biodegradation but they can be
easily recycled compared to thermoset composites. In contrast,
NFPCs consisting of a biodegradable polymer matrix can be broken
down into natural degradation products after their intended use
(Sain and Panthapulakkal, 2004).
Thermoplastics are the most commonly used matrix materials
for NFPCs as they are, in contrast to thermosets, re-moldable, thus
permitting more efficient use of raw materials through recycling
(Clemons, 2008). Polypropylene (PP), polyethylene (PE), poly-
styrene (PS) and polyvinyl chloride (PVC) are examples of ther-
moplastics used in NFPCs. Examples of thermosets include epoxy,
polyesters and polyurethane (PU). Commonly used biodegradable
polymer matrices are PLAs, polyglycolic acid (PGA), poly-b-
hydroxyalkanoates (PHA), which are thermoplastics, and poly-
caprolactone (PCL), which is a thermoset (Sain and Panthapulakkal,
2004).
The partial substitution of the polymer with natural fibers
provides multiple advantages as natural fibers are inexpensive,
typically biodegradable and have a low density. In addition, some
properties, such as tensile strength and elastic modulus, of the
resulting composite materials are better compared with the neat
polymers (El-Shekeil et al., 2012; Mohanty et al., 2006; Mutje et al.,
2007; Premalal et al., 2002; Rashed et al., 2006). More importantly,
NFPCs have shown better performance in life cycle assessments
(LCAs) when compared with conventionally reinforced composites
(Joshi et al., 2004). Overall, NFPCs have an advantage in relation to
toxicity, emission of effluent, energy consumption and abundance
of disposal options (Patel et al., 2005).
There are also other factors contributing towards improved
market development and opportunities for NFPCs (Pandey et al.,
2015). The development of production and manufacturing pro-
cesses with intentions to mitigate environmental damages are
being supported by legislative provisions. Moreover, the dedication
of research institutions and centers to find new ways to elevate the
status on natural fibers to a new level while considering the balance
between sustainability, economics and performance is also an
important factor influencing the future prospects of NFPCs. The
most important factors determining the commercial success of
NFPCs are presented in Fig. 1.
To expand the use of NFPCs in a variety of applications, the
properties of these composites should be somewhat comparable to
the conventional materials like metals and petrochemical de-
rivatives. If the density of the fiber is not taken into account, syn-
thetic fibers have superior mechanical properties compared to
natural fibers. However, the specific strength and modulus (Table 1)
Fig. 1. The triangle of commercial success for NFPCs.
of natural fibers are similar to synthetic fibers. Furthermore, the
price of natural fibers is considerably lower than that of synthetic
fibers (Table 2).
However, in many cases, NFPCs do not possess a similar level of
performance as, e.g., glass fiber reinforced composites (Zini and
Scandola, 2011), which is mainly due to the incompatibility be-
tween hydrophilic natural fiber and hydrophobic polymer matrix.
Traditionally, this issue has been at least partially solved by
adequate physical and chemical modifications. Physical modifica-
tions include sputtering, corona discharge, low temperature
plasma, calandering, stretching, thermal treatment and the pro-
duction of hybrid yarns (Adekunle, 2015; Da nyadi et al., 2010;
Moghadamzadeh et al., 2011; Mukhopadhyay and Fangueiro,
2009; Oporto et al., 2007). The aim of the physical methods is to
alter the structural properties of the fibers and consequently
improve the mechanical bonding between the matrix and fibers.
Some methods also induce changes on the surfaces of the com-
posite components, thereby affecting processability and the me-
chanical properties of the composites. Chemical modification
methods, such as silane treatments, graft copolymerization,
cyanate treatment, impregnation of fibers, and alkali swelling and
substitution reactions, aim to improve the adhesion between fibers
and the polymer matrix through generation of reactive functional
groups on fiber surfaces (George et al., 2001).
Despite their positive effects on NFPCs, the physical and
chemical modification methods increase the risk for chain degra-
dation as well as lead to increment in the production cost (Pandey
et al., 2015). Additionally, it is difficult to address all the problems
associated with NFPCs with one single method (Das et al., 2015c).
Another issue with some of these methods, such as using maleic
anhydride grafted polypropylene (MAPP) as a coupling agent to
introduce a covalent bond between fibers and the matrix, is that
they are based on non-renewable sources and thus do not represent
the modern aspects of developing future generation biocomposites
based solely on renewable materials.
To simultaneously combat the challenges associated with NFPCs
and the application of petroleum-based products and traditional
waste treatment methods (e.g., landfilling), the utilization of bio-
584 €isa
T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596

Table 1
Mechanical properties of natural and synthetic fibers.

Fiber Density (g/cm3) Tensile strength Specific strength Elastic modulus Specific modulus Reference
(MPa) (MPa cm3/g) (GPa) (GPa cm3/g)

Wood 1.4 90e180 64e130 10e70 7e50 Lilholt and Lawther, 2000; Stokke et al., 2014
Flax 1.4e1.5 350e1040 250e650 28e70 18 Lilholt and Lawther, 2000; Stokke et al., 2014; Bledzki
and Gassan, 1999; Faruk et al., 2012; George et al., 2001;
Holbery and Houston, 2006; Ku et al., 2011; Saheb and
Jog, 1999
Hemp 1.4e1.6 690 630 30e70 25 Lilholt and Lawther, 2000; Stokke et al., 2014; Bledzki
and Gassan, 1999; Faruk et al., 2012; Holbery and
Houston, 2006; Ku et al., 2011;Zampaloni et al., 2007
Jute 1.3e1.5 200e770 310e625 20e55 2e37 Lilholt and Lawther, 2000; Stokke et al., 2014; Bledzki
and Gassan, 1999; Faruk et al., 2012; Holbery and
Houston, 2006; Ku et al., 2011; Saheb and Jog, 1999;
Zampaloni et al., 2007
Coir 1.2e1.5 180 146 4e6 3e5 Stokke et al., 2014; Bledzki and Gassan, 1999; Faruk
et al., 2012; Holbery and Houston, 2006; Ku et al., 2011;
Zampaloni et al., 2007
Cotton 1.5e1.6 290e490 191e310 5e12 3e8 Akil et al., 2011; Wambua et al., 2003
Sisal 1.5 100e800 335e430 9e22 6e15 Lilholt and Lawther, 2000; Stokke et al., 2014; Bledzki
and Gassan, 1999; Faruk et al., 2012; George et al., 2001;
Holbery and Houston, 2006; Saheb and Jog, 1999;
Zampaloni et al., 2007
Kenaf 1.4e1.5 930 641 53 36 Stokke et al., 2014; Faruk et al., 2012; Holbery and
Houston, 2006; Ku et al., 2011; Zampaloni et al., 2007
Bamboo 0.6e1.1 140e230 600 11e17 48e89 Stokke et al., 2014; Faruk et al., 2012; Yu et al., 2014
Wool 1.3 50e315 38e242 2.3e5 1.8e3.8 Cheung et al., 2009; Kim et al., 2014; Pickering et al.,
2016
Feather 0.9 100e203 112e226 3e10 3.3e11 Pickering et al., 2016; Zhan and Wool, 2011; Zini and
Scandola, 2011
Silk 1.3e1.4 100e1500 100e1500 5e25 4e20 Pickering et al., 2016; Reddy et al., 2012; Shah et al.,
2014
Glass 2.6 2200e3600 850e1300 65 27 Akil et al., 2011; Dai and Fan, 2014; Kocak and Mistik,
2015; Okubo and Fujii, 2002; Westman et al., 2010
Carbon 1.4e1.8 3000e4000 1710 250e500 164e171 Akil et al., 2011; Westman et al., 2010

based by-products, waste or residues derived from industrial pro- 2000), concurrently resulting in less expensive composite products.
cesses in NFPCs seems to be the next step towards the development This paper aims to review the most current developments in the
of affordable, sustainable and resilient composite systems that have area of NFPCs. The specific objective of this review is to identify and
adequate properties for diverse applications. The utilization of address the most common challenges encountered in NFPC in-
waste or residues as additives or reinforcements in NFPCs confers dustry, based on the recently reported work in this field. The un-
multiple benefits; first, the amount of materials based on non- derlying rationale of this study is to assess and rationalize the
renewable resources may be reduced in the composites. Second, necessity for the development of both ecologically and economi-
the use of waste or residues in NFPCs provides an efficient way to cally more sustainable practices for waste utilization and NFPCs.
re-use these materials instead of dumping them on landfills or This is the first paper to diversely evaluate the potential of waste
using as an energy source. Third, recent studies have given evi- materials and processing by-products as NFPC constituents in order
dence that many drawbacks encountered in adapting natural fibers to overcome the challenges associated with these composites.
for composites can be overcome through addition of inexpensive
waste or residue materials (Das et al., 2015a, 2015b, 2016d, 2016e; 2. Challenges associated with NFPCs
DeVallance et al., 2015; Madhoushi et al., 2014; Rozman et al.,
The incorporation of natural fibers into the polymers induces
several challenges that need to be addressed to improve the per-
Table 2
formance of NFPCs. One of the most prominent problems of using
Average prices of natural and synthetic fibers (Morris,
2009; Muthuraj et al., 2015; Shah et al., 2014).
natural fibers as a reinforcement for polymers is that natural fibers
are inherently hydrophilic and polar (Clemons and Caulfield, 2006;
Fiber Price (US$/kg)
Rowell et al., 2000) whereas most of the polymers used in NFPCs
Wood 0.3e0.6 have non-polar characteristics. This creates difficulties in com-
Flax 2.1e4.2 pounding, which in turn results in poor performance of the com-
Hemp 1.0e2.1
Jute 0.4e1.5
posite. The hydrophilic nature of natural fibers also adversely
Coir 0.3e0.5 affects the water absorption behavior of the composites as the polar
Cotton 2.1e4.2 hydroxyl groups present in the fibers increase the amount of water
Sisal 0.6e0.7 absorbed into the composite (Mohammed et al., 2015).
Kenaf 0.3e0.5
Another challenge of using natural fibers as reinforcement for
Bamboo 0.5
Wool 1.6e2.4 composites is their limited thermal stability. The processing tem-
Feather 1.1e2.0 perature of natural fibers is limited to around 200
C, reducing the
Silk 2.6e40.0 choice of the matrix material to plastics with a low melting tem-
Glass 2.0 perature, e.g., PP, PE, PVC and PS (Lilholt and Lawther, 2000). This,
Carbon 22.0e27.0
in turn, introduces another challenge, as most of these plastics are
 €isa
T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596
Table 3
Mechanical properties of commodity and engineering thermoplastics (Bogoeva-Gaceva et al., 2007; Holbery and Houston, 2006; Ku et al., 2011; Leong et al., 2014).
Polymer Commodity thermoplastics
PP PE
Tensile strength (MPa) 26e41 15e78
Tensile modulus (GPa) 1.3 0.2
Flexural strength (MPa) 40 17
Flexural modulus (GPa) 1.0e1.8 0.055e1.5
weaker in terms of mechanical performance (Table 3) when
compared with engineering thermoplastics, such as polycarbonate
(PC), acrylonitrile butadiene styrene (ABS) and polyethylene tere-
phthalate (PET).
To minimize the use of petroleum-derived materials, the rela-
tive amount of natural fibers in NFPCs should be as high as possible
without compromising on the performance properties of the
composites. However, many studies have shown that the process-
ability of NFPCs becomes challenging when the fiber content ex-
ceeds a certain limit, which varies among different formulations
(typically ~50 wt%) (Mueller and Krobjilowski, 2004; Pickering
et al., 2016; Thakur and Thakur, 2014). This is due to the agglom-
eration of fibers, which eventually deteriorates the mechanical
performance of composites as well as leads to other problems, such
as higher water absorption (Mueller and Krobjilowski, 2004; Saheb
and Jog, 1999). The agglomeration is caused by the inter-fiber
hydrogen bonding resulting from the inability of the polymer ma-
trix to efficiently wet the fibers.
The properties of the fiber reinforcement have a major influence
on the properties of the final NFPC product. The properties of the
natural fibers are governed by their main chemical constituents;
cellulose, hemicelluloses and lignin (Sain and Panthapulakkal,
2004). Fig. 2 illustrates the dependency of the properties of natu-
ral fibers on their main chemical constituents.
2.1. Limited mechanical properties
NFPCs have been successfully used in many applications,
including automotive industry, construction, decoration and pack-
aging. However, the use of NFPCs is currently limited to semi-
structural applications that require the material to at least sup-
port its own weight in addition to bearing light external loads, such
as soft knocks or impacts. Structural applications are defined as
those that play a significant role in supporting the structure of the
final designed component (Staiger and Tucker, 2008). The use of
NFPCs in these applications has been scarce primarily due to the
lack of superior mechanical strength.
It is not only the fibers that determine the mechanical properties
of NFPCs; both the polymer matrix and the fiber reinforcement
constitute the mechanical performance of the NFPC (Saheb and Jog,
Fig. 2. The dependency of the properties of natural fibers on their chemical
constituents.
585
Engineering thermoplastics
PVC PS PC ABS PET
41e52 25e69 72 65 82
2.5e4.1 2.8 2.4 2.1 3.0
69e114 70 90 75 130
2.8 4.0e5.0 2.3 2.5 5.8
1999). The production of NFPCs with homogeneous mechanical
properties could be challenging as the structure and thus proper-
ties of natural fibers vary considerably depending on the source,
growth conditions, and chemical and mechanical treatments (Dai
and Fan, 2014). The use of recycled polymers in NFPCs may
impose additional problems since recycled plastics may exhibit
different performances and contain many grades, colors and con-
taminants (Najafi, 2013).
The main reason for the insufficient mechanical properties of
NFPCs is the poor fiber-matrix interaction, which is caused by the
different chemical nature of the matrix and the fiber reinforcement
(Lu et al., 2000). The chemical incompatibility of these constituents
results in inefficient stress transfer from the matrix to fibers. The
stress transfer phenomenon is further complicated by character-
istic components of natural fibers, including orientation, impu-
rities, moisture absorption, volume fraction (Vf) and physical
properties (Dhakal, 2015). Consequently, the strength and stiffness
of the composite are impaired but in contrast, toughness is
increased. A strong interface enables the composite to bear load
even if multiple fibers are broken because the load can be trans-
ferred to the intact portion of the fibers. It is therefore crucial to
have a good interfacial adhesion between the matrix and fibers to
improve the mechanical strength of NFPCs.
Critical fiber length (lc) is another important concept that helps
to comprehend the mechanical properties of fiber-reinforced
composites (Bourmaud and Baley, 2007; Stark and Rowlands,
2003). Critical fiber length depends on the tensile strength and
diameter of the fiber as well as the shear strength of the fiber-
matrix interface. This means that fibers with an optimal aspect
ratio (the ratio of fiber length to diameter) in relation to the matrix
shear strength should be used to maximize the mechanical prop-
erties of NFPCs. Fig. 3 shows the tensile stress profile in natural
fibers of different lengths during NFPC straining.
The effect of fiber length on the mechanical properties of NFPCs
is ambiguous (Peltola, 2004). According to the fiber reinforcement
theory, the longer the fibers the better is the strength of the com-
posite. On the other hand, the dispersion of shorter fibers is easier
during processing, and some researchers have suggested that good
dispersion improves the properties of NFPCs more than adhesion.
The processing of NFPCs significantly affects the fiber morphology,
as shown by Bourmaud and Baley (2010). Compounding and in-
jection molding decreased fiber diameter, length and consequently
the aspect ratio; up to over an 85% decrease was observed in length
after compounding and injection molding.
2.2. Excess water absorption
The tendency of natural fibers to attract water is another sig-
nificant drawback of using natural fibers as reinforcement for
polymers. The water absorption of natural fibers causes thickness
swelling and dimensional instability of the composite, which may
result in a severe composite damage even in a short term.
Furthermore, as water is absorbed into the composite, the com-
posite becomes more susceptible to fungi, insects and other
586 €isa
T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596

Fig. 3. The tensile stress profile in natural fibers of different lengths during NFPC straining. Fibers shorter than lc (a) cannot reach the ultimate tensile strength of the fiber whereas
fibers with length equal (b) or longer (c) to lc reach the ultimate tensile strength and can fracture. The consequent effects of fiber lengths on the composite properties are listed
below the graphs.

harmful organisms (Hosseinaei et al., 2012; Kim et al., 2008).
Therefore, considerable water uptake of NFPCs can be a prominent
limiting parameter as far as the final application of the composite is
concerned.
To effectively diminish the water absorption of NFPCs, it is
important to understand the mechanisms of moisture absorption in
these materials. In general, the process is complex owing to the
involvement of two distinct systems, hydrophobic polymer matrix,
and hydrophilic natural fibers (Mishra, 2008). Vlaev et al., 2009,
have identified three mechanisms, through which composite ma-
terials absorb moisture; (1) diffusion of water molecules inside the
micro-gaps between the polymer chains, (2) capillary transport of
water molecules into the gaps and flaws at the fiber-matrix inter-
face, and (3) transportation of water through matrix micro-cracks
formed during the compounding. According to various studies
(Espert et al., 2004; Marcovich et al., 1999; Sreekala et al., 2002;
Wang et al., 2006), it seems that this process is governed by two
distinct mechanisms depending on the fiber content in the com-
posite: diffusion and percolation.
In diffusion process, water molecules are transported from one
part of an NFPC system to another as a result of random molecular
motions. For NFPCs, Fickian diffusion has been assumed to be the
dominant mechanism for moisture absorption but the adaption of
the Fick’s laws of diffusion to the NFPCs is somewhat problematic
since it is based on two assumptions that are not always met with
NFPCs; first, the composite structure should be homogeneous.
Second, the water molecules transfer from higher to lower con-
centration only because of random motion of the molecules. The
structure of NFPCs is not always homogeneous, especially at low
(<30%) fiber contents. Hence, the diffusion theory fails to explain
the moisture absorption mechanism in NFPCs. A more encom-
passing model is required to comprehensively explain the moisture
absorption mechanisms in NFPCs.
Percolation theory was applied to NFPCs by Wang et al., 2006.
Percolation theory is an applicable model for NFPCs with low fiber
content as it takes into account the randomness of the composite
structure. The authors suggested that the diffusion theory is the
dominant mechanism of NFPCs with high fiber loadings when the
fibers are highly connected. When the fiber content is close to or
below the percolation threshold, percolation is the dominant
mechanism for moisture absorption of NFPCs. The difference be-
tween percolation and diffusion is clarified in Fig. 4.
The moisture absorption and the resulting thickness swelling
are proportional to the fiber content in the NFPCs (Das and Biswas,
2016; George et al., 1998; Gupta, 2016). The water absorption is also
highly dependent on the fiber size as demonstrated by Migneault
et al., 2008, and Das and Biswas, 2016. Mechanical properties of
NFPCs are considerably affected by the water absorption. Espert
et al., 2004, showed that the water absorption in NFPCs leads to
decreased Young’s modulus and stress at maximum load because
the water molecules change the structure and properties of the
fibers, matrix and the interface between them. Dhakal et al., 2007,

Fig. 4. An NFPC with a structure that enables water absorption through (a) percolation and (b) diffusion (C ¼ A fiber capsulated by the polymer matrix).
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T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596
made similar observations for hemp/polyester composites; expo-
sure to moisture significantly deteriorated tensile and flexural
properties of the composite due to the degradation of the fiber-
matrix interface. For natural fibers, there exists an optimum
moisture content, in which the mechanical performance of the fi-
bers is maximized (Celino et al., 2014). However, there are some
inconsistencies in the results, which is probably due to the different
test conditions and variability factors of the fibers.
The complexity of the water absorption mechanisms in NFPCs is
also evident when the moisture equilibrium is concerned. For
example, Tajvidi et al., 2006, showed that it may take several
months for different NFPCs to reach moisture equilibrium. How-
ever, if the individual components of these composites were con-
cerned, it would be expected that the time to reach the equilibrium
was shorter. For example, commodity polymers reach the moisture
equilibrium in a few days, whereas wood fibers reach the equilib-
rium in weeks.
2.3. Poor thermal properties
The poor fire resistance and smoke generation properties of
NFPCs are significant disadvantages of these materials since,
depending on the application, NFPCs must pass regulatory fire
tests. The thermal degradation of the fibers begins at approximately
200
C (Yao et al., 2008), which substantially limits the number of
suitable polymers for NFPCs. The thermal properties of an NFPC are
mainly governed by the characteristics of the natural fibers but they
are also dependent on the matrix polymer and the interactions
between these main constituents. Fig. 5 shows the stages of a
typical combustion in NFPCs. In addition, some fire properties at
various stages are presented.
Rather surprisingly, the bonding between the matrix and the
fiber reinforcement is critical not only for the mechanical proper-
ties but also for the stability of the composite when exposed to fire
and heat. As the compatibility between the polymer and fibers is
improved, the thermal stability of the composite is also enhanced
(Horrocks and Kandola, 2005), because more energy is required to
separate the constituents. In contrast to this, Das et al., 2016b,
suggested that the thermal properties of the composites are
worsened with good interfacial bonding as the better bonding
means that heat is conducted more as opposed to a gap between
Fig. 5. Stages of combustion in NFPCs.
587
the fiber and the matrix.
Materials are subject to thermal decomposition and combustion
depending on conditions when exposed to fire or any other high-
intensity heat source. The combustibility of an NFPC depends on
many factors, including the type of raw materials used for its
manufacture (fibers, polymer and additives), composite density,
structure, thermal conductivity and humidity (Horrocks and
Kandola, 2005; Kozłowski and Władyka-Przybylak, 2008).
Thermal properties of a material can be analyzed by several
methods. Thermogravimetric analysis (TGA) measures the mass
change, thermal degradation temperature and thermal stability of
composite materials. Thermomechanical analysis (TMA) can mea-
sure the thermal expansion of the material as a function of tem-
perature. In addition, derivative thermogravimetry (DTG) and
differential scanning calorimetry (DSC) can be used.
Several strategies have been employed to overcome the poor
thermal properties of NFPCs. The most common approach is to
apply different types of fire retardants during the manufacturing
process or at the stage of finishing (e.g., coatings) (Kozłowski and
Władyka-Przybylak, 2008). Other methods include the utilization
of non-flammable binders, resins or polymers and the addition of
nanoparticles to the composites. However, it has been documented
that addition of fire retardants severely compromises the strengths
of the composites (Subasinghe and Bhattacharyya, 2014).
2.4. Processing and homogeneity
The low thermal stability and the challenges associated with the
processing of NFPCs are somewhat interconnected; the main
challenge of using natural fibers as a reinforcement for various
polymers is their low thermal degradation temperature (~200
C),
which limits the number of available polymers considerably.
However, the processing of NFPCs includes other difficulties, such
as fiber agglomeration, high viscosity of composite melts with an
increased fiber content and inhomogeneous fiber dispersion during
the processing. The tendency of natural fibers for high water ab-
sorption is also problematic when the processing of the composite
is concerned (Bettini et al., 2008).
However, compared with the conventional reinforcements, such
as nylon, rayon, glass and Kevlar®, natural fibers provide significant
advantages with respect to the processing of composites; the
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T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596

substitution of conventional reinforcements with natural fibers

results in considerable energy savings as well as improved safety
during the processing. Furthermore, NFPCs are less abrasive to
machine and tool surfaces, causing less wear than composites
containing synthetic fibers (Huda et al., 2008).
The application of lignocellulosic fillers and reducing the
thickness of the products to less than 1 mm are extremely difficult
in terms of filling and the residual stress distribution generated in
cavity molds (Azaman et al., 2013). Residual stresses can be divided
into residual flow stresses and residual thermal stresses. According
to Wang and Young, 2005, flow-induced stresses caused by poly-
mer chains depend on the orientation and freeze-off packaging
pressure whereas thermally induced residual stresses are caused by
the inhomogeneous cooling of the molded parts. According to Rudd
et al., 1997, the shrinkage upon solidification can be up to 8%.
Fiber agglomeration during the processing is mainly induced by
the excess fiber loading. It is more likely that chemically similar
fibers contact and bind to each other to form agglomerates than
that the polymers are able to sufficiently wet the fibers during the
processing. Not only does the fiber agglomeration deteriorate the
mechanical properties of the composite but it also affects the
density and water absorption behavior of the composite (Pickering
et al., 2016). High viscosity decelerates the processing speed and
makes it difficult to produce uniform products (Leong et al., 2014).
The uneven fiber distribution may result from excess fiber content Fig. 6. The most important aspects in order to optimize the processability and prop-
but fiber morphology, e.g., the length of the fibers, also affects the erties of NFPCs.
homogeneity of the final product.
The moisture content of the fibers has a critical effect on the
quality of the final product (Leong et al., 2014). This is due to the additives or reinforcements in polymeric composites has been
high temperatures used during the processing, which causes water steadily growing during the past decades. However, the exploita-
to evaporate from the composite melt. The evaporation of water tion of waste materials in composites may evoke problems if not
leads to the formation of bubbles that increases the porosity of the further processed, as their homogeneity is not guaranteed (Holbery
composite and consequently deteriorates its properties. Many and Houston, 2006). The need for additional steps in the production
apparatus are equipped with degassing units that allow the water line should be avoided in order to minimize the costs of the final
vapor to exit the machine during the processing but the problem composite product. Thus, to produce NFPCs with attractive prop-
may still remain (Bledzki et al., 2008). erties, the waste or residue materials, or processing by-products
The traditional ways to overcome the challenges associated with used as an additive of filler in these composites should fulfill the
the processing of NFPCs include the use of additives, such as plas- following criteria:
ticizers, lubricants, shrinkage control additives, fillers and colorants
(Tucker, 2004). However, the problem is that, typically multiple / Homogeneity
types of additives are simultaneously required to optimize the / Sufficient availability
processability of NFPCs. Furthermore, additives are not always / Reasonable price
compatible with each other, and thus the addition of one may / Minimal need for excessive processing
nullify the positive effects of the other (Sherman, 2004). One / Recyclable or biodegradable
example of additives is plant oils, which have shown better lubri- / Compatibility with the main constituents of NFPCs
cation ability, viscosity indices, and superior anticorrosion proper- / Does not negatively affect the processability of NFPCs.
ties when compared with the traditional mineral oil based
alternatives. They have also been classified as non-flammable liq- As shown and discussed by multiple authors (Bogoeva-Gaceva
uids due to their high flashpoints of greater than 300
C (Salimon et al., 2007; Holbery and Houston, 2006; Koronis et al., 2013;
€isa
Va €nen et al., 2016), it is likely that the reinforcement of poly-
et al., 2010). However, the addition of additives further increases
the production costs associated with composite manufacturing. mers with natural fibers, waste or residue materials or processing
Fig. 6 presents the key processing aspects in order to manufacture by-products cannot provide similar strength when compared with
NFPCs with optimized properties. their synthetic counterparts. However, the utilization of waste
materials in NFPCs provides vast opportunities because of the
3. Approaching the challenges with bio-based alternatives diverse raw material base, which may also be seen as an advantage
as the properties of the resulting biocomposites can be tailored
The limitations in the mechanical strength, moisture behavior, according to the demands of the application. The rationale for the
thermal properties and processability highlight the need for the development of novel bio-based NFPCs is presented in Fig. 7.
development of new bio-based additives or fillers for NFPCs that
could simultaneously act as, e.g., coupling agents, lubricants and 3.1. Biochar
fire retardants. The combination of increased environmental
awareness, political incentives and dwindling crude oil resources There are different definitions for biochar but in this review it
drives towards the more efficient utilization of plant or waste based refers to products from thermo-chemical conversion or pyrolysis of
materials (Teuber et al., 2015). As a consequence, the research any bio-based materials. Virtually any plant based biomass
aiming to find new ways to use waste, residues and by-products as (including wastes) can be converted into biochar. Biochar is
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T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596
Fig. 7. The rationale for the development of new bio-based NFPCs.
characterized by a carbon based structure having several different
kinds of pores on its surface (Das et al., 2016a). The pores are mainly
formed by the evolution of volatiles from the solid during thermal
degradation of the biomass. However, biochar is reported to have
three different pore structures: external pores, residual macro-
pores, and pyrogenic nano-pores (Gray et al., 2014). The pores be-
tween the biochar particles constitute the external pores whose
size depends on the particle size and morphology. The internal
pores in the feedstock make up the residual macro-pores whose
size ranges between 1 and 100 mm. The residual macro-pores make
up most of the pore volume of a biochar. The pyrogenic nano-pores
are formed due to the voids formed on the carbon structure as a
consequence of chemical changes at higher pyrolysis temperature
(>500
C). The sizes of pyrogenic nano-pores are ~50 nm, however
they can also be of sub-nanometer range. The nano-pores are
responsible for the resulting surface area of the biochar. Due to the
presence of these pores, biochar has a honeycomb structure (Das
et al., 2016b) (Fig. 8).
The porous structure of biochar has been extremely utilized in
the area of filtration and contaminant removal. On the other hand,
the carbon backbone of biochar has been applied in the field of soil
amendment (Srinivasan and Sarmah, 2015). In spite of the sus-
tainable uses of biochar, its application in composites was limited
until recently. Researchers envisaged that the porous and carbo-
naceous structure of biochar could be applied to manufacture
Fig. 8. SEM of poultry litter biochar (taken by Oisik Das at University of Auckland).
589
sustainable composites with enhanced performance properties.
One of the first studies to report biochar addition in polymeric
composites was by Ahmetli et al., 2013. The authors conducted a
comparative study to observe the reinforcement potential of chars
from different sources in epoxy composites: plastic waste, wood
shavings, and pine cone biochar. Later Das et al., 2015a, attempted
to find out the most suitable loading amount of pine wood derived
biochar in wood/PP composites. The authors observed that a
loading amount of 24 wt% was the most appropriate for enhancing
the mechanical properties of the composites. Sometime later
DeVallance et al., 2015, applied hardwood biochar to manufacture
wood/PP composites and they observed that a loading amount of
25 wt% exhibited best mechanical properties which was similar to
the findings of Das et al., 2015a. Several loading amounts of bamboo
biochar were used by Ho et al., 2015, as reinforcements in PLA
composites. Bamboo biochar was observed to enhance the tensile,
flexural and ductile properties of the resulting composites owing to
their relatively high surface area. Das et al., 2015a, postulated that
the molten polymer flows into the pores of the biochar thus
creating a mechanical interlocking, which causes the improvement
in mechanical properties. All the above-mentioned studies
demonstrated the reinforcement potential of residue biomass
derived biochar, which opened doors for sustainable application of
these renewable materials. However, these investigations were
developmental in nature and the researchers used biochar with low
surface area. In addition, mostly the effects of biochar addition on
mechanical properties were observed. Therefore, the further in-
vestigations involving biochar in polymer composites delved into
other functional properties (e.g. flammability) and used high sur-
face biochar.
Das et al., 2016c, used six different chars obtained from diverse
sources (waste pine wood, poultry litter, and sewage sludge) to
manufacture wood/PP composites using the technique of
compression molding. The authors investigated the changes in
mechanical, chemical, thermal, morphological, and flammability
properties as a result of the biochar addition. The poultry litter
biochar imparted the best tensile and flexural properties due to the
presence of Ca-based ash in it. Composite added with poultry litter
biochar also had lowest values of heat release rates (HRR) under
radiative heat in cone calorimeter. All the biochars were found to
increase the thermal stability of the composites in thermogravi-
metric study. Elsewhere Nan et al., 2015, created composites of
biochar/polyvinyl alcohol and tested their electrical, thermal, and
mechanical properties. The authors reported a similar electrical
conductivity of 2 and 10 wt% biochar composites compared to
carbon nanotubes/graphene added composites. These two afore-
mentioned studies investigated the effect of biochar on the other
important properties of composites (flammability and electrical
conductivity) in addition to the changes in mechanical properties
brought about by biochar inclusion.
More recently, Ikram et al., 2016, applied Taguchi’s design of
experiments to identify the most suitable material factors, which
would be determining the mechanical and flammability properties
of the resulting composites. The authors employed the following
material factors: particle size of high surface area biochar (pine
wood); presence and absence of coupling agent and wood in the
composites; and melt flow index of the PP matrix. The composite
samples were manufactured by melt blending and injection
molding. The authors reported that the presence of coupling agent
(maleic anhydride grafted polypropylene/MAPP) and wood
(together with biochar) was critical for the enhancements in tensile
and flexural properties of the composites. However, upon con-
ducting cone calorimeter tests, the authors observed that there was
no statistical difference between the peak heat release rates
(PHRRs) and HRR of the composite samples formed using different
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material factors. Therefore, it was concluded that the formulation
best suited for mechanical properties could be applied without
affecting the flammability properties. In another study by Das et al.,
2016a, high surface area biochar (~335 m2/g) was added to PP
without any other natural fiber reinforcement at five different
loading amounts of 0, 15, 25, 30, 35 wt%. The composites were
manufactured in a process similar to the one done by Ikram et al.,
2016. The PHRRs and smoke production of the composites (upon
combustion) were drastically reduced as a result of biochar addi-
tion. At higher biochar loading levels, tensile/flexural modulus and
flexural strength were increased. In addition, the thermal stability
of the composites gradually enhanced with increasing loading
amounts of biochar. A further study by Das et al., 2016b, reported
that biochar addition saves production costs by ~18% as the amount
of MAPP could be gradually reduced from 3 wt% to 1 wt% without
any significant changes in mechanical properties.
Biochar has been identified as potential addition in composites
through the researches described above and in a recent review by
V€ais€
anen et al., 2016. The enhancements of mechanical properties
of the composites are brought about by the pore infiltration by
polymer and better dispersion of biochar particles in the matrix. On
the other hand, thermally stable carbon in biochar provides a rigid
and compact char structure during combustion, which inhibits the
transfer of heat and mass between ambient O2 and the polymer.
Consequently, the combustion is decelerated and the smoke pro-
ductions are reduced. This betterment of performance properties of
composites is particularly attractive as biochar application also
promotes waste utilization and sustainability. Finally, addition of
biochar also proved to be beneficial for saving composite produc-
tion costs. Therefore, it is clear that biochar could constitute as next
generation renewable reinforcements in polymeric composites.
However, most of the studies done did not report an increase in
tensile strengths unless used in conjunction with another natural
fibre (e.g. wood). The porous biochar lacks surface functional
groups as the volatiles exit during its production through pyrolysis.
Therefore, future studies should attempt to impart surface func-
tional groups on to biochar surface (through physical and chemical
treatments) so that it can take part in MAPP/coupling agent assisted
adhesion with the polymer matrix. The resulting interfacial adhe-
sion between biochar and polymer could potentially increase the
tensile strengths.
3.2. Lignin
Lignin is a common by-product from the pulp and paper in-
dustry (Liu et al., 2014). It is the second most abundant biopolymer
after cellulose and it accounts for 1e45 wt% of natural fibers (Dias
et al., 2016; V€ ais€
anen et al., 2016). The structure of lignin is com-
plex and non-uniform with aliphatic and aromatic constituents
(Morandim-Giannetti et al., 2012). The main precursors are three
aromatic alcohols, sinapyl alcohols, p-coumaryl and coniferyl. At
the moment, lignin is mainly utilized as fuel for energy balance for
the pulping process but recent findings have shown that lignin
derivatives have significant potential for value-added products (Liu
et al., 2014).
Lignin has been investigated as a compatibilizer and as antiox-
idant in NFPCs. The presence of both non-polar aliphatic and polar
groups justifies the use of lignin as a compatibilizer since these may
provide compatibility between the polymer matrix and the fibers
(Rozman et al., 2000). The use of lignin as an antioxidant is due to
its similar structure to hindered phenols that are used as primary
antioxidants in polymers (Pouteau et al., 2003).
Acha et al., 2009, used lignin as a compatibilizer in jute fabric-PP
composites. The composites consisted of 25 wt% jute fabric rein-
forcement with 5 wt% of lignin and 70 wt% of PP. Even though their
scanning electron micrographic (SEM) observations indicated that
the addition of lignin improved the adhesion between jute fibers
and the PP matrix, the mechanical properties of the composites
were not improved; only minor benefits were obtained in impact
behavior. However, the authors showed that lignin could act as a
fire retardant when added to neat PP.
Rozman et al., 2000, produced coir-PP composites with lignin as
a compatibilizer. The fiber content in the composites varied be-
tween 20 and 50 wt%. With each fiber content value, the lignin
content ranged from 0 to 20 wt%. Furthermore, the authors pro-
duced similar composites using Epolene E43 (a tradename for
MAPP produced by Eastman Chemical Company) as an additive
instead of lignin to compare the compatibilizers. The addition of
lignin decreased the water absorption and thickness swelling of the
composites, which was due to the non-polar hydrocarbon chains
and aromatic rings in the lignin. The authors hypothesized that
lignin could decrease the water absorption of the composites either
by bulking the cell wall or by plugging the lumen of the cell wall.
Similar to the findings by Acha et al., 2009, Rozman et al., 2000,
found that the addition of lignin enhanced the interfacial adhesion
between the polymer matrix and the fibers. Despite this, no
improvement in the mechanical properties were observed because
lignin induced fiber agglomeration. The results of this study,
however, show that lignin has potential as an additive for NFPCs
that need to have low water absorption instead of improved me-
chanical properties.
Morandim-Giannetti et al., 2012, used lignin as an additive in
PP/coir composite. The composites were produced by maintaining
the PP level at 70% while varying the coir fiber content between 20
and 30%. Lignin contents were varied from 0 to 10%. PP grafted with
maleic anhydride (PP-g-MA) was used as a compatibilizer in some
formulation with a 4% content. The results showed that the incor-
poration of lignin did not enhance the tensile strength of the
composite but improved the elongation at break, although a large
variability in elongation was observed. In contrast to the findings by
Acha et al., 2009, and Rozman et al., 2000, the SEM micrographs
showed that the addition of lignin reduced composite compatibility
because of the formation of a separated lignin phase at the inter-
phase. The thermal resistance of the composites was improved
with lignin; the initial decomposition temperature and oxidation
induction times increased for both the compatibilized and non-
compatibilized composites. The authors explained this finding by
proposing two probable protection mechanisms: the role of lignin
as a primary antioxidant and its action as a barrier against the
thermal degradation by coating the fiber reinforcement. Overall,
the authors could have tested composites with decreasing PP
contents while increasing the lignocellulosic content to observe if
there were any improvements with these formulations.
Wood et al., 2011, prepared hemp-epoxy composites with lignin
as a compatibilizer. The composites were prepared with a range of
lignin contents (0, 1, 2.5 & 5 wt%). The fiber content in the com-
posites was 20.68e22.46 wt%. The 2.5 wt% addition of lignin
significantly increased the tensile modulus and ultimate tensile
strength of the composites. Enhancements were also observed in
the flexural properties of the composites after the lignin addition,
the optimum lignin level being 2.5 wt%. The highest impact
strength was observed for the composite containing 5 wt% of lignin.
The optical microscopy and SEM analyses indicated that the addi-
tion of lignin the bonding between the composite constituents,
which is in agreement with Acha et al., 2009, and Rozman et al.,
2000. However, in contrast with the other studies, the results ob-
tained by Wood et al., 2011, showed that the inclusion of lignin in an
NFPC improves the mechanical properties of the composite. This
rather contradictory finding can be explained by the differences
between the polymer matrices as well as by the different
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manufacturing methods. In addition, the type of the fiber may also
have an effect; lignin content in hemp fiber is typically 3e10%,
where as in coir it is 40e45% (Bogoeva-Gaceva et al., 2007; Espert
et al., 2004; Faruk et al., 2012; Lilholt and Lawther, 2000; Liu
et al., 2012; Narendar and Priya Dasan, 2012; Reddy and Yang,
2005; Rowell et al., 2000). Therefore, the interfacial bonding
mechanisms between the fiber and lignin may differ. The relative
compositions (matrix/reinforcement/lignin) of the composites
were also somewhat different.
Overall, the authors could have tested composites with
decreasing PP contents while increasing the lignocellulosic content
to observe if there were any improvements with these formula-
tions. In addition, substituting a higher share of the polymers with
lignin could have provided different results. In order to avoid
compromises in the mechanical properties of NFPCs having lignin
as an additive, new ways to prevent the fiber agglomeration in the
composites should be developed.
3.3. Sewage sludge
Sewage sludge is a waste residue generated in great quantities
from, e.g., the pulp and paper processing or wastewater treatment
processes. Typically, most of the sludge is either landfilled or
incinerated but some of the sludge is also utilized in farming
(Hamzeh et al., 2012). The sludge typically consists of fine cellulosic
fibers (fibers are too short to be retained on fiber screens and paper
machines) and inorganic materials, such as kaolin, clay and calcium
carbonate (Hamzeh et al., 2011). The fine fibers have a high aspect
ratio, causing minimal abrasion to the processing equipment and
providing high strength to the composite (Son et al., 2001).
Son et al., 2001, prepared paper sludge-thermoplastic (PP, high
impact polypropylene (HIPP), high-density PE (HDPE) and low-
density PE (LDPE)) composites with different sludge particle sizes
and extrusion temperatures. The thickness swelling and water
absorption of the composites increased when the size of the paper
sludge particles decreased. Even though the larger particles had
higher cellulose contents, which would hypothetically increase the
water absorption of the composites with larger particles, the au-
thors suggested that the porosity of the particles affected the water
absorption more. Thus, the composites with smaller particles were
less dense and thus their water absorption values were higher.
Increasing the particle size increased the tensile and flexural
strengths of the composites despite some outlying data. This was
due to the higher cellulosic fiber content in the larger particles. In
addition, the authors hypothesized that the reduction in the
amount of inorganic materials in the paper sludge with a larger
particle size positively affected the interfacial adhesion between
the fiber reinforcement and the polymer matrix. The higher cellu-
losic fiber content in the larger particles also positively influenced
the composite notched impact strengths when the thermoplastic
polymer was either HIPP or HDPE. No trends were observed in un-
notched impact strength with respect to the thermoplastic polymer
types, which was due to the fact that the un-notched impact
behavior is controlled by fracture initiation processes that are
dominated by stress concentrations in the composite system. The
authors also observed that the increase in the extrusion tempera-
tures positively affected the dimensional stabilities and tensile
properties of the composites. The effect of the extrusion tempera-
ture on the impact properties varied depending on the formulation.
Ink-eliminated sludge flour (IESF) has been tested as a filler for
PP (Qiao et al., 2003). The addition of IESF in PP decreased the Izod
impact properties of the composites substantially (up to over a 92%
decrease). Furthermore, a decrease in the tensile strength was
observed. However, hardness and the flexural properties were
enhanced after the IESF addition. The compatibilization with MAPP
591
had positive effects on the tensile and flexural properties but not in
the Izod impact properties or hardness. The structural and thermal
analyses showed that the addition of IESF induced the crystalliza-
tion orientation of PP along the b-axis as well as had a restraining
effect on the crystallization on the b-phase. Because IESF acted as
nucleating agent, the composites possessed quicker crystallization
rate and lower crystallization supercooling degree during the
crystallization process. The addition of IESF increased the crystal-
lization and melting temperature of the material. Among the
composites, the IESF-PP composites coupled with MAPP had the
greatest values of enthalpy during the crystallization process. Paper
sludge-PP composites have poor fire resistance but the incorpora-
tion of flame retardants can enhance the flame retardancy of the
composite system (Jang and Lee, 2000). However, this could
counter the positive effects of IESF on the mechanical properties of
the composites as the addition of fire retardants severely com-
promises the strengths of the composites (Subasinghe and
Bhattacharyya, 2014).
Hamzeh et al., 2011, 2012, tested paper sludge and ink-
eliminated sludge (IES) as an additive or filler in HDPE/wood
flour-composites. The rationale of these studies was to find addi-
tional use for these waste materials along with using them as an
energy source. The compositions of the composites were varied as
follows: the paper sludge, IES and wood flour content ranged from
0 to 60 wt% and the polymer content was either 37 wt% or 58 wt%.
Enhanced flexural properties were achieved after the addition of
paper sludge even in the absence of coupling agent. This is an
important finding as the incorporation of coupling agents is typi-
cally a prerequisite in order to produce NFPCs with an adequate
mechanical strength. The comparison of paper sludge and IES as
fillers show that the composites made with IES had better physico-
mechanical properties compared to paper sludge filled composites.
The water absorption and thickness swelling values of the com-
posites decreased with increasing sludge content, showing con-
trasting behavior when compared with wood flour content. The
presence of either wood flour or sludge expectedly resulted in the
higher weight loss of composites when exposed to white-rot fungi,
which is due to the higher content of organic materials available for
the fungus to feed on (Hamzeh et al., 2011). The studies by Hamzeh
et al. clearly demonstrate the high potential of waste sludge as
reinforcement for thermoplastics composites, either individually or
as filler in other NFPCs systems.
3.4. Animal fibers
Animal fibers are the second most important source of natural
fibers after plant fibers. Although these fibers are not as abundantly
available as plant fibers and their prices are usually higher
compared with plant-derived fibers (Table 2), they have shown to
be effective reinforcements for polymers (Shubhra et al., 2010).
Examples of animal fibers include silk, wool, hair and feather. Silk
fiber is synthesized by silk gland cells and stored in the lumen of
the silk glands, after which it is converted into silk fibers. Overall,
silk fibers exert high strength, extensibility and compressibility,
and thus they are attractive raw materials alternatives for com-
posites. Wool is another alternative to be used as a composite
reinforcement. Wool fibers are obtained from mammals, and fibers
find their primary use in textile industry. However, the utilization
of wool in NFCPs has drawn attention because wool exert, in
contrast to many other animal fibers, fairly good thermal proper-
ties; the rates of flame spread and heat release are low, and also the
heat of combustion is low (Ramamoorthy et al., 2015). Furthermore,
significant amounts of chicken feather are annually generated as a
by-product from the poultry industry (Amieva et al., 2015). Their
reinforcement ability has been evaluated by a number of
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researchers.
Shubhra et al., 2010, prepared NFPCs from plant and animal fi-
bers to compare their mechanical and degradation properties. The
composites consisted of silk fibers þ PP and jute fibers þ PP. The
results showed that composites having jute fibers as reinforcement
(20 wt%) absorbed more water than the ones reinforced with silk
fibers (20 wt%). This was due to the hydrophilic nature of jute fibers.
However, silk fibers are hygroscopic, meaning that instead of
bonding to the water molecules in the material, these fibers attract
and absorb water without actively bonding to the molecules. The
comparative studies on mechanical properties of the composites
showed that the composites reinforced with silk fibers exhibit
better mechanical properties than jute fiber reinforced composites,
which was due to the better adhesion between the silk fibers and
the PP matrix. Similarly, the silk fiber reinforced composites
retained greater mechanical strength than jute-based composites
because of the less degradative character of silk fibers. In practice,
the costly nature of silk fibers outweighs its advantage of better
reinforcing ability when compared to jute fibers (Table 2). In
contrast to the results by Shubhra et al., 2010, Taşdemır et al., 2008,
found that PC reinforced with cotton fibers exerted better me-
chanical properties compared with the silk fiber reinforced com-
posites. The authors suggested that the adhesion between the
cotton fibers and the PC matrix was better than between the silk
fibers and PC. The SEM investigations confirmed these findings. The
differences between these findings could be explained by the
different fiber contents; Taşdemır et al., 2008, fabricated the com-
posites with 3% fiber loading whereas the composites prepared by
Shubhra et al., 2010, contained 20 wt% of fibers.
Wool fibers have been used in several NFPC formulations. The
addition of wool fibers in PP improves the fire retardancy of the
material by increasing thermal stability and char residue, and
decreasing HRR (Bertini et al., 2013; Kim et al., 2014; Kim and
Bhattacharyya, 2016). The addition of ammonium polyphosphate
(APP) can further improve the fire retardant properties of the
composites (Kim and Bhattacharyya, 2016) but the high price
(13e14 US$/kg) and the ecological concerns related to the use of
APP limits the use of this constituent in NFPCs. The addition of wool
fibers also improves the tensile properties of the composites, and
the improvement can be further enhanced by the addition of MAPP
because of the improved interfacial adhesion between wool and PP
(Kim et al., 2014; Kim and Bhattacharyya, 2016). Improvements in
elastic modulus have also been observed (Bertini et al., 2013;
Conzatti et al., 2013).
Barone and Schmidt, 2005, prepared NFPCs consisting of keratin
fibers obtained from chicken feathers and LDPE. The Vf of keratin
feather fiber varied between 0 and 0.5. The results from the me-
chanical test showed that the inclusion of keratin feather fibers in
LDPE improved the elastic and specific modulus of the composites
as well as lead to an enhancement in the yield stress. However, the
yield strain of the composites decreased along with the increasing
fiber content. In addition to the improved mechanical properties,
the incorporation of the fibers decreased the density of the com-
posites by 2%. The microscopic evaluations indicated that there was
some interaction between the fibers and the polymer even in the
absence of the coupling agent. Huda and Yang, 2008, prepared
NFPCs with two different fiber reinforcements, jute and ground
chicken quill, to compare their reinforcement ability. Quill is one of
the three basic parts of the feathers. In terms of weight, half of the
feather is quill, and it consists mainly of keratin protein with pri-
marily b-sheet (Amieva et al., 2015). The quill content in quill-PP
composites ranged from 20 to 50% whereas in jute-PP composites
the jute fiber content varied between 40 and 70%. In terms of
mechanical performance, the comparison of these composites
clearly shows that the jute fiber reinforced composites exhibited
better mechanical properties than the ones reinforced with quill
fibers. For example, if the composites with the same fiber contents
(40e50%) are compared, the impact resistance of the jute fiber
reinforced composites was 82% higher when compared with quill-
PP composites. In addition, the tensile properties of the jute-PP
composites were over three times higher than those of quill-PP
composites. The inferior properties of quill-PP composites were
due to the considerably lower aspect ratio of the fibers despite the
better compatibility between quill fibers and the PP matrix. The
different dispersion of the fibers could also explain the findings.
Interestingly, the optimized flexural properties for these compos-
ites were achieved with rather different fiber contents; for quill-PP
composites, the optimal fiber content was 35% whereas 60% con-
tent was optimal for jute-PP composites. With these contents, the
flexural strength of quill-PP composites was higher (10.2 MPa)
compared with jute-PP composites (9.0 MPa). In addition, quill-PP
composites had superior acoustical properties compared to jute-PP
composites, indicating that these composites could be ideal mate-
rials for acoustic panels and headliner substrates. Jime nez-Cer-
vantes Amieva et al., 2015, also prepared quill-PP composites.
However, the quill loadings in their composites were 5, 10 and
15 wt%. The hydrophobic nature of quill fibers resulted in a good
distribution and impregnation into the PP matrix, which was
confirmed in SEM and dynamic mechanical analyses (DMA). The
results suggest that small amounts of quill (5e10 wt%) was optimal
in terms of density and mechanical properties of the composites.
This could also explain the results obtained by Huda and Yang,
2008; the 20e50% loading of quill in PP leads to matrix over-
loading, which reduces the efficient load transfer. The TGA analyses
showed that the thermal behavior of the composites was enhanced
only for the composites with 10 wt% quill content. Cheng et al.,
2009, assessed mechanical and thermal properties of chicken
feather fiber (CFF)-PLA composites. The addition of CFFs in PLA
resulted in a deterioration of tensile strength but the 2 wt% content
of CFFs improved the elongation at break significantly. The 5 wt%
CFF content was ideal in terms of the elongation at break. The DMA
analyses showed that the incorporation of CFFs considerably
increased the stiffness of the composites and decreased the me-
chanical loss factor, indicating the reinforcing effect of CFFs on the
PLA matrix. The thermal stability of the composites was also
enhanced as compared to pure PLA.
The utilization of animal fibers seems to be a viable choice for
the development of new NFPCs. However, the high cost (Table 2)
and the low availability as compared to plant fibers are major issues
when considering the more widespread use of these fibers
(Ramamoorthy et al., 2015). As is the case with plant fibers, the
heterogeneity of animal fibers may become a concern when pro-
ducing composites for more demanding applications. The produc-
tion of NFPCs with multiple fiber types, i.e., hybridization with
animal and plant fibers, could be a logical step in the development
novel NFPCs. Namely, if the good thermal resistance and low water
absorption of wool were combined with the excellent reinforcing
ability of, e.g., jute fibers, it could be possible to overcome the
aforementioned problems associated with NFPCs.
3.5. Hybridization with multiple fiber types
Hybrid composites are developed by using more than one type,
shape or size of reinforcement (Ashori and Sheshmani, 2010). The
popularity of these materials is constantly increasing due to their
capability of providing freedom of tailoring composites and
achieving properties that cannot be attained in composite systems
containing only one type of reinforcement (Kumar et al., 2015). The
typical aim of producing hybrid NFPCs is to maintain the advan-
tages of the fibers and alleviate some disadvantages (Swolfs et al.,
 €isa
T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596
2014). Another aim of the composite hybridization is also to reduce
the price of the final composite product. Although the use of natural
fibers in composites is less expensive compared with the conven-
tional reinforcements, there are considerable differences in the
prices of natural fibers, as shown in Table 2. For example, the price
of wood fibers may be as much as 14 times lower than the price of
cotton fibers. A partial substitution of cotton fibers with wood fi-
bers could provide significant advantages in terms of the perfor-
mance of the composite as well as in the production costs.
Several types of hybrid NFPCs have been studied. The hybridi-
zation of wood flour-PP composites with waste cone flour
(20e40 wt%) negatively affected the flexural properties and water
resistance of the composite (Ayrilmis et al., 2010). However, a 10 wt
% addition of pine cone flour into the composite did not have sig-
nificant effect on the flexural or water absorption properties. Thus,
adding low amounts of pine cone flour into wood flour-PP com-
posites seems to be a noteworthy choice in order to produce hybrid
composites with adequate properties. The production of hybrid
composites consisting of polyester, short banana fibers and sisal
fibers also results in a positive hybrid effect for tensile and flexural
properties (Idicula et al., 2005). The tensile strength of the com-
posite is increased as the Vf of the banana fiber is higher. Similar
trend cannot be observed with respect to the flexural strength; the
optimum level for the flexural strength can be obtained when the Vf
of banana fibers is approximately 50% of the total fiber content (40
Vf). The impact strength of the composites reduced as the banana
fiber content increased but increasing the total fiber content in the
composites positively affected the impact strength of the com-
posite. The reduction in the impact strength after the inclusion of
banana fibers was due to the lower microfibrillar angle of banana
fibers (11
) compared to sisal fibers (20
), and also due to the better
compatibility between banana fibers and the polymer matrix. This
can be attributed to the fact that the better compatibility decrease
the possibility for fiber pullout that would positively affect the
impact properties due to the, e.g., frictional forces. This also ex-
plains the increase in impact strength when the Vf of the fibers was
higher. Venkateshwaran et al., 2012, also prepared hybrid NFPCs
using banana and sisal fibers as reinforcements in an epoxy resin. In
contrast to the results by Idicula et al., 2005, the optimum amount
of banana fibers with respect to the tensile properties of the com-
posites was 50% of the total fiber content, which was also fixed to
40% Vf.
Ashori, 2010, showed that the use of fibers with substantially
different morphologies can be advantageous with respect to the
performance of NFPCs. NFPCs containing 66e70% of PP and 30 wt%
of lignocellulosic materials were prepared. The lignocellulosic
material consisted of newspaper fiber (NF) and/or wood flour (WF).
The results of the study showed that the addition of lignocellulosic
fibers clearly enhanced the tensile and flexural modulus of the
composites. The addition of WF (aspect ratio 5.6) deteriorated the
properties of the composite whereas the inclusion of NF (aspect
ratio 47.7) had a less dramatic effect due to the different mor-
phologies. However, the thermal stability of the composites was
enhanced as the WF content in the composites was higher, which
was probably caused by the high thermal stability of lignin present
in the WF. Ashori and Sheshmani, 2010, prepared hybrid NFPCs
from recycled PP, recycled newspaper fibers (RNF) and poplar wood
flour (PWF). PP content in the composites ranged from 66% to 70%
whereas RNF and PWF contents varied between 0% and 30% while
maintaining the total fiber content at 30%. The aim of the study was
to assess the moisture absorption and thickness swelling behavior.
The lowest values for the water absorption and thickness swelling
were obtained for the composites with the highest quantities of
PWF whereas the opposite results were obtained for the compos-
ites with high amounts of RNF. This finding is due to the lower
593
holocellulose and higher lignin content in PWF.
Composites consisting of cork, coir fibers and HDPE also
demonstrate positive hybrid effect (Fernandes et al., 2013); the
10 wt% addition of coir fiber into the composite in the presence of
coupling agent resulted in an increase of 30% on the tensile
maximum strength and 39% on tensile modulus when compared
with the composites consisting of cork, HDPE and coupling agent.
Overall, the reinforcing effect of coir fibers in these composites was
evident.
In summary, the hybridization of NFPCs represents an efficient,
sustainable and economical way of waste utilization. In many cases,
the presence of a compatibilizer is still a necessity in order to obtain
adequate enhancements in the characteristics of the composites.
The choice of the compatibilizer needs to be addressed more in the
future studies. In addition, more studies are needed to test the
suitability of other fibers types for NFPC hybridization. For example,
the hybridization of NFPCs with animal and plant fibers needs to be
explored more in the future. The preliminary results from Ganesh
and Rekha, 2013, show the positive hybridization effect at high fi-
ber contents (over 30%) when polyester resin is reinforced with
chicken feather and rice husk fibers.
4. Future trends
Due to the interest in renewability and sustainability, research
and development on NFPCs is constantly increasing and their use is
expanding into new areas of applications. The low price, biode-
gradability, wide availability and low density of natural fibers act as
catalysts in the substitution of conventional reinforcements of
composites, such as glass and carbon, into these greener alterna-
tives. Despite the above-mentioned favorable properties of NFPCs,
there exist some drawbacks that may limit their expansion into
wider use. In this review, the limited mechanical durability, excess
water absorption, poor thermal properties and challenges in the
processing and production of homogeneous NFPCs were identified
as the four major drawbacks associated with NFPCs.
In light of the recent advancements on this field, it is evident
that the challenges associated with NFPCs are increasingly being
approached with bio-based solutions because the use of substances
produced by environmentally harmful and energy intensive tech-
niques does not represent the values that the consumers, industries
and governmental bodies have adapted during the past decades. An
expanding approach in this field is the utilization of waste and
residue materials, and by-products from industrial processes as the
composite constituents. Not only could this approach address the
challenges associated with NFPCs, but it would also represent a
novel way for waste utilization and solve the challenges concerning
traditional waste treatment methods, such as landfilling. However,
there are still potential renewable materials to be utilized in NFPCs
and it is therefore crucial to continue the research on finding new
sustainable alternatives for petroleum-derived and ecologically
unfriendly NFPCs substituents, such as polymers and additives.
Certain bio-based alternatives have shown immense potential:
addition of wool was found to be beneficial for the lowering of
composite’s flammability due to its char forming ability. On the
other hand, biochar was reported to enhance the mechanical
properties while also simultaneously reducing the combustibility
and production costs of the resulting composites. Hybridization
with multiple bio-based reinforcements has been identified as a
promising technique to produce cheaper composites with certain
mechanical properties enhanced.
More comprehensive practices are needed in order to solve the
challenges associated with NFPCs. It is both economically and
ecologically reasonable to seek for new materials and processing
methods that are able to simultaneously solve several challenges
594 €isa
T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596
encountered in the use of NFPCs instead of focusing only on a single
problem. On the other hand, the consideration of environmental
aspects has become an essential part in the research and devel-
opment of new materials, i.e., the raw materials used in NFPCs
should be obtained from renewable sources and the processing of
the composites should be based on sustainable practices. The
concept ‘Think global, act local’ should be adapted as an essential
mindset in NFPC industry.
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