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

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DOI: 10.1016/j.jclepro.2017.02.132

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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.
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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). Fig. 1. The triangle of commercial success for NFPCs.
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 of natural fibers are similar to synthetic fibers. Furthermore, the
(Clemons, 2008). Polypropylene (PP), polyethylene (PE), poly- price of natural fibers is considerably lower than that of synthetic
styrene (PS) and polyvinyl chloride (PVC) are examples of ther- fibers (Table 2).
moplastics used in NFPCs. Examples of thermosets include epoxy, However, in many cases, NFPCs do not possess a similar level of
polyesters and polyurethane (PU). Commonly used biodegradable performance as, e.g., glass fiber reinforced composites (Zini and
polymer matrices are PLAs, polyglycolic acid (PGA), poly-b- Scandola, 2011), which is mainly due to the incompatibility be-
hydroxyalkanoates (PHA), which are thermoplastics, and poly- tween hydrophilic natural fiber and hydrophobic polymer matrix.
caprolactone (PCL), which is a thermoset (Sain and Panthapulakkal, Traditionally, this issue has been at least partially solved by
2004). adequate physical and chemical modifications. Physical modifica-
The partial substitution of the polymer with natural fibers tions include sputtering, corona discharge, low temperature
provides multiple advantages as natural fibers are inexpensive, plasma, calandering, stretching, thermal treatment and the pro-
typically biodegradable and have a low density. In addition, some duction of hybrid yarns (Adekunle, 2015; Da nyadi et al., 2010;
properties, such as tensile strength and elastic modulus, of the Moghadamzadeh et al., 2011; Mukhopadhyay and Fangueiro,
resulting composite materials are better compared with the neat 2009; Oporto et al., 2007). The aim of the physical methods is to
polymers (El-Shekeil et al., 2012; Mohanty et al., 2006; Mutje et al., alter the structural properties of the fibers and consequently
2007; Premalal et al., 2002; Rashed et al., 2006). More importantly, improve the mechanical bonding between the matrix and fibers.
NFPCs have shown better performance in life cycle assessments Some methods also induce changes on the surfaces of the com-
(LCAs) when compared with conventionally reinforced composites posite components, thereby affecting processability and the me-
(Joshi et al., 2004). Overall, NFPCs have an advantage in relation to chanical properties of the composites. Chemical modification
toxicity, emission of effluent, energy consumption and abundance methods, such as silane treatments, graft copolymerization,
of disposal options (Patel et al., 2005). cyanate treatment, impregnation of fibers, and alkali swelling and
There are also other factors contributing towards improved substitution reactions, aim to improve the adhesion between fibers
market development and opportunities for NFPCs (Pandey et al., and the polymer matrix through generation of reactive functional
2015). The development of production and manufacturing pro- groups on fiber surfaces (George et al., 2001).
cesses with intentions to mitigate environmental damages are Despite their positive effects on NFPCs, the physical and
being supported by legislative provisions. Moreover, the dedication chemical modification methods increase the risk for chain degra-
of research institutions and centers to find new ways to elevate the dation as well as lead to increment in the production cost (Pandey
status on natural fibers to a new level while considering the balance et al., 2015). Additionally, it is difficult to address all the problems
between sustainability, economics and performance is also an associated with NFPCs with one single method (Das et al., 2015c).
important factor influencing the future prospects of NFPCs. The Another issue with some of these methods, such as using maleic
most important factors determining the commercial success of anhydride grafted polypropylene (MAPP) as a coupling agent to
NFPCs are presented in Fig. 1. introduce a covalent bond between fibers and the matrix, is that
To expand the use of NFPCs in a variety of applications, the they are based on non-renewable sources and thus do not represent
properties of these composites should be somewhat comparable to the modern aspects of developing future generation biocomposites
the conventional materials like metals and petrochemical de- based solely on renewable materials.
rivatives. If the density of the fiber is not taken into account, syn- To simultaneously combat the challenges associated with NFPCs
thetic fibers have superior mechanical properties compared to and the application of petroleum-based products and traditional
natural fibers. However, the specific strength and modulus (Table 1) 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
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T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596 585

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 Engineering thermoplastics

PP PE PVC PS PC ABS PET

Tensile strength (MPa) 26e41 15e78 41e52 25e69 72 65 82


Tensile modulus (GPa) 1.3 0.2 2.5e4.1 2.8 2.4 2.1 3.0
Flexural strength (MPa) 40 17 69e114 70 90 75 130
Flexural modulus (GPa) 1.0e1.8 0.055e1.5 2.8 4.0e5.0 2.3 2.5 5.8

weaker in terms of mechanical performance (Table 3) when 1999). The production of NFPCs with homogeneous mechanical
compared with engineering thermoplastics, such as polycarbonate properties could be challenging as the structure and thus proper-
(PC), acrylonitrile butadiene styrene (ABS) and polyethylene tere- ties of natural fibers vary considerably depending on the source,
phthalate (PET). growth conditions, and chemical and mechanical treatments (Dai
To minimize the use of petroleum-derived materials, the rela- and Fan, 2014). The use of recycled polymers in NFPCs may
tive amount of natural fibers in NFPCs should be as high as possible impose additional problems since recycled plastics may exhibit
without compromising on the performance properties of the different performances and contain many grades, colors and con-
composites. However, many studies have shown that the process- taminants (Najafi, 2013).
ability of NFPCs becomes challenging when the fiber content ex- The main reason for the insufficient mechanical properties of
ceeds a certain limit, which varies among different formulations NFPCs is the poor fiber-matrix interaction, which is caused by the
(typically ~50 wt%) (Mueller and Krobjilowski, 2004; Pickering different chemical nature of the matrix and the fiber reinforcement
et al., 2016; Thakur and Thakur, 2014). This is due to the agglom- (Lu et al., 2000). The chemical incompatibility of these constituents
eration of fibers, which eventually deteriorates the mechanical results in inefficient stress transfer from the matrix to fibers. The
performance of composites as well as leads to other problems, such stress transfer phenomenon is further complicated by character-
as higher water absorption (Mueller and Krobjilowski, 2004; Saheb istic components of natural fibers, including orientation, impu-
and Jog, 1999). The agglomeration is caused by the inter-fiber rities, moisture absorption, volume fraction (Vf) and physical
hydrogen bonding resulting from the inability of the polymer ma- properties (Dhakal, 2015). Consequently, the strength and stiffness
trix to efficiently wet the fibers. of the composite are impaired but in contrast, toughness is
The properties of the fiber reinforcement have a major influence increased. A strong interface enables the composite to bear load
on the properties of the final NFPC product. The properties of the even if multiple fibers are broken because the load can be trans-
natural fibers are governed by their main chemical constituents; ferred to the intact portion of the fibers. It is therefore crucial to
cellulose, hemicelluloses and lignin (Sain and Panthapulakkal, have a good interfacial adhesion between the matrix and fibers to
2004). Fig. 2 illustrates the dependency of the properties of natu- improve the mechanical strength of NFPCs.
ral fibers on their main chemical constituents. 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,
2.1. Limited mechanical properties 2003). Critical fiber length depends on the tensile strength and
diameter of the fiber as well as the shear strength of the fiber-
NFPCs have been successfully used in many applications, matrix interface. This means that fibers with an optimal aspect
including automotive industry, construction, decoration and pack- ratio (the ratio of fiber length to diameter) in relation to the matrix
aging. However, the use of NFPCs is currently limited to semi- shear strength should be used to maximize the mechanical prop-
structural applications that require the material to at least sup- erties of NFPCs. Fig. 3 shows the tensile stress profile in natural
port its own weight in addition to bearing light external loads, such fibers of different lengths during NFPC straining.
as soft knocks or impacts. Structural applications are defined as The effect of fiber length on the mechanical properties of NFPCs
those that play a significant role in supporting the structure of the is ambiguous (Peltola, 2004). According to the fiber reinforcement
final designed component (Staiger and Tucker, 2008). The use of theory, the longer the fibers the better is the strength of the com-
NFPCs in these applications has been scarce primarily due to the posite. On the other hand, the dispersion of shorter fibers is easier
lack of superior mechanical strength. during processing, and some researchers have suggested that good
It is not only the fibers that determine the mechanical properties dispersion improves the properties of NFPCs more than adhesion.
of NFPCs; both the polymer matrix and the fiber reinforcement The processing of NFPCs significantly affects the fiber morphology,
constitute the mechanical performance of the NFPC (Saheb and Jog, 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.
Fig. 2. The dependency of the properties of natural fibers on their chemical Furthermore, as water is absorbed into the composite, the com-
constituents. posite becomes more susceptible to fungi, insects and other
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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). Second, the water molecules transfer from higher to lower con-
Therefore, considerable water uptake of NFPCs can be a prominent centration only because of random motion of the molecules. The
limiting parameter as far as the final application of the composite is structure of NFPCs is not always homogeneous, especially at low
concerned. (<30%) fiber contents. Hence, the diffusion theory fails to explain
To effectively diminish the water absorption of NFPCs, it is the moisture absorption mechanism in NFPCs. A more encom-
important to understand the mechanisms of moisture absorption in passing model is required to comprehensively explain the moisture
these materials. In general, the process is complex owing to the absorption mechanisms in NFPCs.
involvement of two distinct systems, hydrophobic polymer matrix, Percolation theory was applied to NFPCs by Wang et al., 2006.
and hydrophilic natural fibers (Mishra, 2008). Vlaev et al., 2009, Percolation theory is an applicable model for NFPCs with low fiber
have identified three mechanisms, through which composite ma- content as it takes into account the randomness of the composite
terials absorb moisture; (1) diffusion of water molecules inside the structure. The authors suggested that the diffusion theory is the
micro-gaps between the polymer chains, (2) capillary transport of dominant mechanism of NFPCs with high fiber loadings when the
water molecules into the gaps and flaws at the fiber-matrix inter- fibers are highly connected. When the fiber content is close to or
face, and (3) transportation of water through matrix micro-cracks below the percolation threshold, percolation is the dominant
formed during the compounding. According to various studies mechanism for moisture absorption of NFPCs. The difference be-
(Espert et al., 2004; Marcovich et al., 1999; Sreekala et al., 2002; tween percolation and diffusion is clarified in Fig. 4.
Wang et al., 2006), it seems that this process is governed by two The moisture absorption and the resulting thickness swelling
distinct mechanisms depending on the fiber content in the com- are proportional to the fiber content in the NFPCs (Das and Biswas,
posite: diffusion and percolation. 2016; George et al., 1998; Gupta, 2016). The water absorption is also
In diffusion process, water molecules are transported from one highly dependent on the fiber size as demonstrated by Migneault
part of an NFPC system to another as a result of random molecular et al., 2008, and Das and Biswas, 2016. Mechanical properties of
motions. For NFPCs, Fickian diffusion has been assumed to be the NFPCs are considerably affected by the water absorption. Espert
dominant mechanism for moisture absorption but the adaption of et al., 2004, showed that the water absorption in NFPCs leads to
the Fick’s laws of diffusion to the NFPCs is somewhat problematic decreased Young’s modulus and stress at maximum load because
since it is based on two assumptions that are not always met with the water molecules change the structure and properties of the
NFPCs; first, the composite structure should be homogeneous. 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 587

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

Fig. 5. Stages of combustion in NFPCs.


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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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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
Fig. 7. The rationale for the development of new bio-based NFPCs. 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
characterized by a carbon based structure having several different the molten polymer flows into the pores of the biochar thus
kinds of pores on its surface (Das et al., 2016a). The pores are mainly creating a mechanical interlocking, which causes the improvement
formed by the evolution of volatiles from the solid during thermal in mechanical properties. All the above-mentioned studies
degradation of the biomass. However, biochar is reported to have demonstrated the reinforcement potential of residue biomass
three different pore structures: external pores, residual macro- derived biochar, which opened doors for sustainable application of
pores, and pyrogenic nano-pores (Gray et al., 2014). The pores be- these renewable materials. However, these investigations were
tween the biochar particles constitute the external pores whose developmental in nature and the researchers used biochar with low
size depends on the particle size and morphology. The internal surface area. In addition, mostly the effects of biochar addition on
pores in the feedstock make up the residual macro-pores whose mechanical properties were observed. Therefore, the further in-
size ranges between 1 and 100 mm. The residual macro-pores make vestigations involving biochar in polymer composites delved into
up most of the pore volume of a biochar. The pyrogenic nano-pores other functional properties (e.g. flammability) and used high sur-
are formed due to the voids formed on the carbon structure as a face biochar.
consequence of chemical changes at higher pyrolysis temperature Das et al., 2016c, used six different chars obtained from diverse
(>500  C). The sizes of pyrogenic nano-pores are ~50 nm, however sources (waste pine wood, poultry litter, and sewage sludge) to
they can also be of sub-nanometer range. The nano-pores are manufacture wood/PP composites using the technique of
responsible for the resulting surface area of the biochar. Due to the compression molding. The authors investigated the changes in
presence of these pores, biochar has a honeycomb structure (Das mechanical, chemical, thermal, morphological, and flammability
et al., 2016b) (Fig. 8). properties as a result of the biochar addition. The poultry litter
The porous structure of biochar has been extremely utilized in biochar imparted the best tensile and flexural properties due to the
the area of filtration and contaminant removal. On the other hand, presence of Ca-based ash in it. Composite added with poultry litter
the carbon backbone of biochar has been applied in the field of soil biochar also had lowest values of heat release rates (HRR) under
amendment (Srinivasan and Sarmah, 2015). In spite of the sus- radiative heat in cone calorimeter. All the biochars were found to
tainable uses of biochar, its application in composites was limited increase the thermal stability of the composites in thermogravi-
until recently. Researchers envisaged that the porous and carbo- metric study. Elsewhere Nan et al., 2015, created composites of
naceous structure of biochar could be applied to manufacture 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
Fig. 8. SEM of poultry litter biochar (taken by Oisik Das at University of Auckland). (PHRRs) and HRR of the composite samples formed using different
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material factors. Therefore, it was concluded that the formulation scanning electron micrographic (SEM) observations indicated that
best suited for mechanical properties could be applied without the addition of lignin improved the adhesion between jute fibers
affecting the flammability properties. In another study by Das et al., and the PP matrix, the mechanical properties of the composites
2016a, high surface area biochar (~335 m2/g) was added to PP were not improved; only minor benefits were obtained in impact
without any other natural fiber reinforcement at five different behavior. However, the authors showed that lignin could act as a
loading amounts of 0, 15, 25, 30, 35 wt%. The composites were fire retardant when added to neat PP.
manufactured in a process similar to the one done by Ikram et al., Rozman et al., 2000, produced coir-PP composites with lignin as
2016. The PHRRs and smoke production of the composites (upon a compatibilizer. The fiber content in the composites varied be-
combustion) were drastically reduced as a result of biochar addi- tween 20 and 50 wt%. With each fiber content value, the lignin
tion. At higher biochar loading levels, tensile/flexural modulus and content ranged from 0 to 20 wt%. Furthermore, the authors pro-
flexural strength were increased. In addition, the thermal stability duced similar composites using Epolene E43 (a tradename for
of the composites gradually enhanced with increasing loading MAPP produced by Eastman Chemical Company) as an additive
amounts of biochar. A further study by Das et al., 2016b, reported instead of lignin to compare the compatibilizers. The addition of
that biochar addition saves production costs by ~18% as the amount lignin decreased the water absorption and thickness swelling of the
of MAPP could be gradually reduced from 3 wt% to 1 wt% without composites, which was due to the non-polar hydrocarbon chains
any significant changes in mechanical properties. and aromatic rings in the lignin. The authors hypothesized that
Biochar has been identified as potential addition in composites lignin could decrease the water absorption of the composites either
through the researches described above and in a recent review by by bulking the cell wall or by plugging the lumen of the cell wall.
V€ais€
anen et al., 2016. The enhancements of mechanical properties Similar to the findings by Acha et al., 2009, Rozman et al., 2000,
of the composites are brought about by the pore infiltration by found that the addition of lignin enhanced the interfacial adhesion
polymer and better dispersion of biochar particles in the matrix. On between the polymer matrix and the fibers. Despite this, no
the other hand, thermally stable carbon in biochar provides a rigid improvement in the mechanical properties were observed because
and compact char structure during combustion, which inhibits the lignin induced fiber agglomeration. The results of this study,
transfer of heat and mass between ambient O2 and the polymer. however, show that lignin has potential as an additive for NFPCs
Consequently, the combustion is decelerated and the smoke pro- that need to have low water absorption instead of improved me-
ductions are reduced. This betterment of performance properties of chanical properties.
composites is particularly attractive as biochar application also Morandim-Giannetti et al., 2012, used lignin as an additive in
promotes waste utilization and sustainability. Finally, addition of PP/coir composite. The composites were produced by maintaining
biochar also proved to be beneficial for saving composite produc- the PP level at 70% while varying the coir fiber content between 20
tion costs. Therefore, it is clear that biochar could constitute as next and 30%. Lignin contents were varied from 0 to 10%. PP grafted with
generation renewable reinforcements in polymeric composites. maleic anhydride (PP-g-MA) was used as a compatibilizer in some
However, most of the studies done did not report an increase in formulation with a 4% content. The results showed that the incor-
tensile strengths unless used in conjunction with another natural poration of lignin did not enhance the tensile strength of the
fibre (e.g. wood). The porous biochar lacks surface functional composite but improved the elongation at break, although a large
groups as the volatiles exit during its production through pyrolysis. variability in elongation was observed. In contrast to the findings by
Therefore, future studies should attempt to impart surface func- Acha et al., 2009, and Rozman et al., 2000, the SEM micrographs
tional groups on to biochar surface (through physical and chemical showed that the addition of lignin reduced composite compatibility
treatments) so that it can take part in MAPP/coupling agent assisted because of the formation of a separated lignin phase at the inter-
adhesion with the polymer matrix. The resulting interfacial adhe- phase. The thermal resistance of the composites was improved
sion between biochar and polymer could potentially increase the with lignin; the initial decomposition temperature and oxidation
tensile strengths. induction times increased for both the compatibilized and non-
compatibilized composites. The authors explained this finding by
3.2. Lignin proposing two probable protection mechanisms: the role of lignin
as a primary antioxidant and its action as a barrier against the
Lignin is a common by-product from the pulp and paper in- thermal degradation by coating the fiber reinforcement. Overall,
dustry (Liu et al., 2014). It is the second most abundant biopolymer the authors could have tested composites with decreasing PP
after cellulose and it accounts for 1e45 wt% of natural fibers (Dias contents while increasing the lignocellulosic content to observe if
et al., 2016; V€ ais€
anen et al., 2016). The structure of lignin is com- there were any improvements with these formulations.
plex and non-uniform with aliphatic and aromatic constituents Wood et al., 2011, prepared hemp-epoxy composites with lignin
(Morandim-Giannetti et al., 2012). The main precursors are three as a compatibilizer. The composites were prepared with a range of
aromatic alcohols, sinapyl alcohols, p-coumaryl and coniferyl. At lignin contents (0, 1, 2.5 & 5 wt%). The fiber content in the com-
the moment, lignin is mainly utilized as fuel for energy balance for posites was 20.68e22.46 wt%. The 2.5 wt% addition of lignin
the pulping process but recent findings have shown that lignin significantly increased the tensile modulus and ultimate tensile
derivatives have significant potential for value-added products (Liu strength of the composites. Enhancements were also observed in
et al., 2014). the flexural properties of the composites after the lignin addition,
Lignin has been investigated as a compatibilizer and as antiox- the optimum lignin level being 2.5 wt%. The highest impact
idant in NFPCs. The presence of both non-polar aliphatic and polar strength was observed for the composite containing 5 wt% of lignin.
groups justifies the use of lignin as a compatibilizer since these may The optical microscopy and SEM analyses indicated that the addi-
provide compatibility between the polymer matrix and the fibers tion of lignin the bonding between the composite constituents,
(Rozman et al., 2000). The use of lignin as an antioxidant is due to which is in agreement with Acha et al., 2009, and Rozman et al.,
its similar structure to hindered phenols that are used as primary 2000. However, in contrast with the other studies, the results ob-
antioxidants in polymers (Pouteau et al., 2003). tained by Wood et al., 2011, showed that the inclusion of lignin in an
Acha et al., 2009, used lignin as a compatibilizer in jute fabric-PP NFPC improves the mechanical properties of the composite. This
composites. The composites consisted of 25 wt% jute fabric rein- rather contradictory finding can be explained by the differences
forcement with 5 wt% of lignin and 70 wt% of PP. Even though their between the polymer matrices as well as by the different
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T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596 591

manufacturing methods. In addition, the type of the fiber may also had positive effects on the tensile and flexural properties but not in
have an effect; lignin content in hemp fiber is typically 3e10%, the Izod impact properties or hardness. The structural and thermal
where as in coir it is 40e45% (Bogoeva-Gaceva et al., 2007; Espert analyses showed that the addition of IESF induced the crystalliza-
et al., 2004; Faruk et al., 2012; Lilholt and Lawther, 2000; Liu tion orientation of PP along the b-axis as well as had a restraining
et al., 2012; Narendar and Priya Dasan, 2012; Reddy and Yang, effect on the crystallization on the b-phase. Because IESF acted as
2005; Rowell et al., 2000). Therefore, the interfacial bonding nucleating agent, the composites possessed quicker crystallization
mechanisms between the fiber and lignin may differ. The relative rate and lower crystallization supercooling degree during the
compositions (matrix/reinforcement/lignin) of the composites crystallization process. The addition of IESF increased the crystal-
were also somewhat different. lization and melting temperature of the material. Among the
Overall, the authors could have tested composites with composites, the IESF-PP composites coupled with MAPP had the
decreasing PP contents while increasing the lignocellulosic content greatest values of enthalpy during the crystallization process. Paper
to observe if there were any improvements with these formula- sludge-PP composites have poor fire resistance but the incorpora-
tions. In addition, substituting a higher share of the polymers with tion of flame retardants can enhance the flame retardancy of the
lignin could have provided different results. In order to avoid composite system (Jang and Lee, 2000). However, this could
compromises in the mechanical properties of NFPCs having lignin counter the positive effects of IESF on the mechanical properties of
as an additive, new ways to prevent the fiber agglomeration in the the composites as the addition of fire retardants severely com-
composites should be developed. promises the strengths of the composites (Subasinghe and
Bhattacharyya, 2014).
3.3. Sewage sludge Hamzeh et al., 2011, 2012, tested paper sludge and ink-
eliminated sludge (IES) as an additive or filler in HDPE/wood
Sewage sludge is a waste residue generated in great quantities flour-composites. The rationale of these studies was to find addi-
from, e.g., the pulp and paper processing or wastewater treatment tional use for these waste materials along with using them as an
processes. Typically, most of the sludge is either landfilled or energy source. The compositions of the composites were varied as
incinerated but some of the sludge is also utilized in farming follows: the paper sludge, IES and wood flour content ranged from
(Hamzeh et al., 2012). The sludge typically consists of fine cellulosic 0 to 60 wt% and the polymer content was either 37 wt% or 58 wt%.
fibers (fibers are too short to be retained on fiber screens and paper Enhanced flexural properties were achieved after the addition of
machines) and inorganic materials, such as kaolin, clay and calcium paper sludge even in the absence of coupling agent. This is an
carbonate (Hamzeh et al., 2011). The fine fibers have a high aspect important finding as the incorporation of coupling agents is typi-
ratio, causing minimal abrasion to the processing equipment and cally a prerequisite in order to produce NFPCs with an adequate
providing high strength to the composite (Son et al., 2001). mechanical strength. The comparison of paper sludge and IES as
Son et al., 2001, prepared paper sludge-thermoplastic (PP, high fillers show that the composites made with IES had better physico-
impact polypropylene (HIPP), high-density PE (HDPE) and low- mechanical properties compared to paper sludge filled composites.
density PE (LDPE)) composites with different sludge particle sizes The water absorption and thickness swelling values of the com-
and extrusion temperatures. The thickness swelling and water posites decreased with increasing sludge content, showing con-
absorption of the composites increased when the size of the paper trasting behavior when compared with wood flour content. The
sludge particles decreased. Even though the larger particles had presence of either wood flour or sludge expectedly resulted in the
higher cellulose contents, which would hypothetically increase the higher weight loss of composites when exposed to white-rot fungi,
water absorption of the composites with larger particles, the au- which is due to the higher content of organic materials available for
thors suggested that the porosity of the particles affected the water the fungus to feed on (Hamzeh et al., 2011). The studies by Hamzeh
absorption more. Thus, the composites with smaller particles were et al. clearly demonstrate the high potential of waste sludge as
less dense and thus their water absorption values were higher. reinforcement for thermoplastics composites, either individually or
Increasing the particle size increased the tensile and flexural as filler in other NFPCs systems.
strengths of the composites despite some outlying data. This was
due to the higher cellulosic fiber content in the larger particles. In 3.4. Animal fibers
addition, the authors hypothesized that the reduction in the
amount of inorganic materials in the paper sludge with a larger Animal fibers are the second most important source of natural
particle size positively affected the interfacial adhesion between fibers after plant fibers. Although these fibers are not as abundantly
the fiber reinforcement and the polymer matrix. The higher cellu- available as plant fibers and their prices are usually higher
losic fiber content in the larger particles also positively influenced compared with plant-derived fibers (Table 2), they have shown to
the composite notched impact strengths when the thermoplastic be effective reinforcements for polymers (Shubhra et al., 2010).
polymer was either HIPP or HDPE. No trends were observed in un- Examples of animal fibers include silk, wool, hair and feather. Silk
notched impact strength with respect to the thermoplastic polymer fiber is synthesized by silk gland cells and stored in the lumen of
types, which was due to the fact that the un-notched impact the silk glands, after which it is converted into silk fibers. Overall,
behavior is controlled by fracture initiation processes that are silk fibers exert high strength, extensibility and compressibility,
dominated by stress concentrations in the composite system. The and thus they are attractive raw materials alternatives for com-
authors also observed that the increase in the extrusion tempera- posites. Wool is another alternative to be used as a composite
tures positively affected the dimensional stabilities and tensile reinforcement. Wool fibers are obtained from mammals, and fibers
properties of the composites. The effect of the extrusion tempera- find their primary use in textile industry. However, the utilization
ture on the impact properties varied depending on the formulation. of wool in NFCPs has drawn attention because wool exert, in
Ink-eliminated sludge flour (IESF) has been tested as a filler for contrast to many other animal fibers, fairly good thermal proper-
PP (Qiao et al., 2003). The addition of IESF in PP decreased the Izod ties; the rates of flame spread and heat release are low, and also the
impact properties of the composites substantially (up to over a 92% heat of combustion is low (Ramamoorthy et al., 2015). Furthermore,
decrease). Furthermore, a decrease in the tensile strength was significant amounts of chicken feather are annually generated as a
observed. However, hardness and the flexural properties were by-product from the poultry industry (Amieva et al., 2015). Their
enhanced after the IESF addition. The compatibilization with MAPP reinforcement ability has been evaluated by a number of
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researchers. better mechanical properties than the ones reinforced with quill
Shubhra et al., 2010, prepared NFPCs from plant and animal fi- fibers. For example, if the composites with the same fiber contents
bers to compare their mechanical and degradation properties. The (40e50%) are compared, the impact resistance of the jute fiber
composites consisted of silk fibers þ PP and jute fibers þ PP. The reinforced composites was 82% higher when compared with quill-
results showed that composites having jute fibers as reinforcement PP composites. In addition, the tensile properties of the jute-PP
(20 wt%) absorbed more water than the ones reinforced with silk composites were over three times higher than those of quill-PP
fibers (20 wt%). This was due to the hydrophilic nature of jute fibers. composites. The inferior properties of quill-PP composites were
However, silk fibers are hygroscopic, meaning that instead of due to the considerably lower aspect ratio of the fibers despite the
bonding to the water molecules in the material, these fibers attract better compatibility between quill fibers and the PP matrix. The
and absorb water without actively bonding to the molecules. The different dispersion of the fibers could also explain the findings.
comparative studies on mechanical properties of the composites Interestingly, the optimized flexural properties for these compos-
showed that the composites reinforced with silk fibers exhibit ites were achieved with rather different fiber contents; for quill-PP
better mechanical properties than jute fiber reinforced composites, composites, the optimal fiber content was 35% whereas 60% con-
which was due to the better adhesion between the silk fibers and tent was optimal for jute-PP composites. With these contents, the
the PP matrix. Similarly, the silk fiber reinforced composites flexural strength of quill-PP composites was higher (10.2 MPa)
retained greater mechanical strength than jute-based composites compared with jute-PP composites (9.0 MPa). In addition, quill-PP
because of the less degradative character of silk fibers. In practice, composites had superior acoustical properties compared to jute-PP
the costly nature of silk fibers outweighs its advantage of better composites, indicating that these composites could be ideal mate-
reinforcing ability when compared to jute fibers (Table 2). In rials for acoustic panels and headliner substrates. Jime nez-Cer-
contrast to the results by Shubhra et al., 2010, Taşdemır et al., 2008, vantes Amieva et al., 2015, also prepared quill-PP composites.
found that PC reinforced with cotton fibers exerted better me- However, the quill loadings in their composites were 5, 10 and
chanical properties compared with the silk fiber reinforced com- 15 wt%. The hydrophobic nature of quill fibers resulted in a good
posites. The authors suggested that the adhesion between the distribution and impregnation into the PP matrix, which was
cotton fibers and the PC matrix was better than between the silk confirmed in SEM and dynamic mechanical analyses (DMA). The
fibers and PC. The SEM investigations confirmed these findings. The results suggest that small amounts of quill (5e10 wt%) was optimal
differences between these findings could be explained by the in terms of density and mechanical properties of the composites.
different fiber contents; Taşdemır et al., 2008, fabricated the com- This could also explain the results obtained by Huda and Yang,
posites with 3% fiber loading whereas the composites prepared by 2008; the 20e50% loading of quill in PP leads to matrix over-
Shubhra et al., 2010, contained 20 wt% of fibers. loading, which reduces the efficient load transfer. The TGA analyses
Wool fibers have been used in several NFPC formulations. The showed that the thermal behavior of the composites was enhanced
addition of wool fibers in PP improves the fire retardancy of the only for the composites with 10 wt% quill content. Cheng et al.,
material by increasing thermal stability and char residue, and 2009, assessed mechanical and thermal properties of chicken
decreasing HRR (Bertini et al., 2013; Kim et al., 2014; Kim and feather fiber (CFF)-PLA composites. The addition of CFFs in PLA
Bhattacharyya, 2016). The addition of ammonium polyphosphate resulted in a deterioration of tensile strength but the 2 wt% content
(APP) can further improve the fire retardant properties of the of CFFs improved the elongation at break significantly. The 5 wt%
composites (Kim and Bhattacharyya, 2016) but the high price CFF content was ideal in terms of the elongation at break. The DMA
(13e14 US$/kg) and the ecological concerns related to the use of analyses showed that the incorporation of CFFs considerably
APP limits the use of this constituent in NFPCs. The addition of wool increased the stiffness of the composites and decreased the me-
fibers also improves the tensile properties of the composites, and chanical loss factor, indicating the reinforcing effect of CFFs on the
the improvement can be further enhanced by the addition of MAPP PLA matrix. The thermal stability of the composites was also
because of the improved interfacial adhesion between wool and PP enhanced as compared to pure PLA.
(Kim et al., 2014; Kim and Bhattacharyya, 2016). Improvements in The utilization of animal fibers seems to be a viable choice for
elastic modulus have also been observed (Bertini et al., 2013; the development of new NFPCs. However, the high cost (Table 2)
Conzatti et al., 2013). and the low availability as compared to plant fibers are major issues
Barone and Schmidt, 2005, prepared NFPCs consisting of keratin when considering the more widespread use of these fibers
fibers obtained from chicken feathers and LDPE. The Vf of keratin (Ramamoorthy et al., 2015). As is the case with plant fibers, the
feather fiber varied between 0 and 0.5. The results from the me- heterogeneity of animal fibers may become a concern when pro-
chanical test showed that the inclusion of keratin feather fibers in ducing composites for more demanding applications. The produc-
LDPE improved the elastic and specific modulus of the composites tion of NFPCs with multiple fiber types, i.e., hybridization with
as well as lead to an enhancement in the yield stress. However, the animal and plant fibers, could be a logical step in the development
yield strain of the composites decreased along with the increasing novel NFPCs. Namely, if the good thermal resistance and low water
fiber content. In addition to the improved mechanical properties, absorption of wool were combined with the excellent reinforcing
the incorporation of the fibers decreased the density of the com- ability of, e.g., jute fibers, it could be possible to overcome the
posites by 2%. The microscopic evaluations indicated that there was aforementioned problems associated with NFPCs.
some interaction between the fibers and the polymer even in the
absence of the coupling agent. Huda and Yang, 2008, prepared 3.5. Hybridization with multiple fiber types
NFPCs with two different fiber reinforcements, jute and ground
chicken quill, to compare their reinforcement ability. Quill is one of Hybrid composites are developed by using more than one type,
the three basic parts of the feathers. In terms of weight, half of the shape or size of reinforcement (Ashori and Sheshmani, 2010). The
feather is quill, and it consists mainly of keratin protein with pri- popularity of these materials is constantly increasing due to their
marily b-sheet (Amieva et al., 2015). The quill content in quill-PP capability of providing freedom of tailoring composites and
composites ranged from 20 to 50% whereas in jute-PP composites achieving properties that cannot be attained in composite systems
the jute fiber content varied between 40 and 70%. In terms of containing only one type of reinforcement (Kumar et al., 2015). The
mechanical performance, the comparison of these composites typical aim of producing hybrid NFPCs is to maintain the advan-
clearly shows that the jute fiber reinforced composites exhibited tages of the fibers and alleviate some disadvantages (Swolfs et al.,
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T. Va €nen et al. / Journal of Cleaner Production 149 (2017) 582e596 593

2014). Another aim of the composite hybridization is also to reduce holocellulose and higher lignin content in PWF.
the price of the final composite product. Although the use of natural Composites consisting of cork, coir fibers and HDPE also
fibers in composites is less expensive compared with the conven- demonstrate positive hybrid effect (Fernandes et al., 2013); the
tional reinforcements, there are considerable differences in the 10 wt% addition of coir fiber into the composite in the presence of
prices of natural fibers, as shown in Table 2. For example, the price coupling agent resulted in an increase of 30% on the tensile
of wood fibers may be as much as 14 times lower than the price of maximum strength and 39% on tensile modulus when compared
cotton fibers. A partial substitution of cotton fibers with wood fi- with the composites consisting of cork, HDPE and coupling agent.
bers could provide significant advantages in terms of the perfor- Overall, the reinforcing effect of coir fibers in these composites was
mance of the composite as well as in the production costs. evident.
Several types of hybrid NFPCs have been studied. The hybridi- In summary, the hybridization of NFPCs represents an efficient,
zation of wood flour-PP composites with waste cone flour sustainable and economical way of waste utilization. In many cases,
(20e40 wt%) negatively affected the flexural properties and water the presence of a compatibilizer is still a necessity in order to obtain
resistance of the composite (Ayrilmis et al., 2010). However, a 10 wt adequate enhancements in the characteristics of the composites.
% addition of pine cone flour into the composite did not have sig- The choice of the compatibilizer needs to be addressed more in the
nificant effect on the flexural or water absorption properties. Thus, future studies. In addition, more studies are needed to test the
adding low amounts of pine cone flour into wood flour-PP com- suitability of other fibers types for NFPC hybridization. For example,
posites seems to be a noteworthy choice in order to produce hybrid the hybridization of NFPCs with animal and plant fibers needs to be
composites with adequate properties. The production of hybrid explored more in the future. The preliminary results from Ganesh
composites consisting of polyester, short banana fibers and sisal and Rekha, 2013, show the positive hybridization effect at high fi-
fibers also results in a positive hybrid effect for tensile and flexural ber contents (over 30%) when polyester resin is reinforced with
properties (Idicula et al., 2005). The tensile strength of the com- chicken feather and rice husk fibers.
posite is increased as the Vf of the banana fiber is higher. Similar
trend cannot be observed with respect to the flexural strength; the 4. Future trends
optimum level for the flexural strength can be obtained when the Vf
of banana fibers is approximately 50% of the total fiber content (40 Due to the interest in renewability and sustainability, research
Vf). The impact strength of the composites reduced as the banana and development on NFPCs is constantly increasing and their use is
fiber content increased but increasing the total fiber content in the expanding into new areas of applications. The low price, biode-
composites positively affected the impact strength of the com- gradability, wide availability and low density of natural fibers act as
posite. The reduction in the impact strength after the inclusion of catalysts in the substitution of conventional reinforcements of
banana fibers was due to the lower microfibrillar angle of banana composites, such as glass and carbon, into these greener alterna-
fibers (11 ) compared to sisal fibers (20 ), and also due to the better tives. Despite the above-mentioned favorable properties of NFPCs,
compatibility between banana fibers and the polymer matrix. This there exist some drawbacks that may limit their expansion into
can be attributed to the fact that the better compatibility decrease wider use. In this review, the limited mechanical durability, excess
the possibility for fiber pullout that would positively affect the water absorption, poor thermal properties and challenges in the
impact properties due to the, e.g., frictional forces. This also ex- processing and production of homogeneous NFPCs were identified
plains the increase in impact strength when the Vf of the fibers was as the four major drawbacks associated with NFPCs.
higher. Venkateshwaran et al., 2012, also prepared hybrid NFPCs In light of the recent advancements on this field, it is evident
using banana and sisal fibers as reinforcements in an epoxy resin. In that the challenges associated with NFPCs are increasingly being
contrast to the results by Idicula et al., 2005, the optimum amount approached with bio-based solutions because the use of substances
of banana fibers with respect to the tensile properties of the com- produced by environmentally harmful and energy intensive tech-
posites was 50% of the total fiber content, which was also fixed to niques does not represent the values that the consumers, industries
40% Vf. and governmental bodies have adapted during the past decades. An
Ashori, 2010, showed that the use of fibers with substantially expanding approach in this field is the utilization of waste and
different morphologies can be advantageous with respect to the residue materials, and by-products from industrial processes as the
performance of NFPCs. NFPCs containing 66e70% of PP and 30 wt% composite constituents. Not only could this approach address the
of lignocellulosic materials were prepared. The lignocellulosic challenges associated with NFPCs, but it would also represent a
material consisted of newspaper fiber (NF) and/or wood flour (WF). novel way for waste utilization and solve the challenges concerning
The results of the study showed that the addition of lignocellulosic traditional waste treatment methods, such as landfilling. However,
fibers clearly enhanced the tensile and flexural modulus of the there are still potential renewable materials to be utilized in NFPCs
composites. The addition of WF (aspect ratio 5.6) deteriorated the and it is therefore crucial to continue the research on finding new
properties of the composite whereas the inclusion of NF (aspect sustainable alternatives for petroleum-derived and ecologically
ratio 47.7) had a less dramatic effect due to the different mor- unfriendly NFPCs substituents, such as polymers and additives.
phologies. However, the thermal stability of the composites was Certain bio-based alternatives have shown immense potential:
enhanced as the WF content in the composites was higher, which addition of wool was found to be beneficial for the lowering of
was probably caused by the high thermal stability of lignin present composite’s flammability due to its char forming ability. On the
in the WF. Ashori and Sheshmani, 2010, prepared hybrid NFPCs other hand, biochar was reported to enhance the mechanical
from recycled PP, recycled newspaper fibers (RNF) and poplar wood properties while also simultaneously reducing the combustibility
flour (PWF). PP content in the composites ranged from 66% to 70% and production costs of the resulting composites. Hybridization
whereas RNF and PWF contents varied between 0% and 30% while with multiple bio-based reinforcements has been identified as a
maintaining the total fiber content at 30%. The aim of the study was promising technique to produce cheaper composites with certain
to assess the moisture absorption and thickness swelling behavior. mechanical properties enhanced.
The lowest values for the water absorption and thickness swelling More comprehensive practices are needed in order to solve the
were obtained for the composites with the highest quantities of challenges associated with NFPCs. It is both economically and
PWF whereas the opposite results were obtained for the compos- ecologically reasonable to seek for new materials and processing
ites with high amounts of RNF. This finding is due to the lower methods that are able to simultaneously solve several challenges
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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 wood flour on the properties of PP/wood composites. Compos Part A-Appl. Sci.
2, 199e206.
problem. On the other hand, the consideration of environmental
Das, G., Biswas, S., 2016. Effect of fiber parameters on physical, mechanical and
aspects has become an essential part in the research and devel- water absorption behaviour of coir fibereepoxy composites. J. Reinf. Plast.
opment of new materials, i.e., the raw materials used in NFPCs Compos 8, 644e653.
should be obtained from renewable sources and the processing of Das, O., Bhattacharyya, D., Hui, D., Lau, K., 2016a. Mechanical and flammability
characterisations of biochar/polypropylene biocomposites. Compos Part B - Eng.
the composites should be based on sustainable practices. The 106, 120e128.
concept ‘Think global, act local’ should be adapted as an essential Das, O., Bhattacharyya, D., Sarmah, A.K., 2016b. Sustainable ecoecomposites ob-
mindset in NFPC industry. tained from waste derived biochar: a consideration in performance properties,
production costs, and environmental impact. J. Clean. Prod. 129, 159e168.
Das, O., Sarmah, A.K., Bhattacharyya, D., 2016c. Biocomposites from waste derived
biochars: mechanical, thermal, chemical, and morphological properties. Waste
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