Construction and Building Materials 211 (2019) 502–516

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Construction and Building Materials

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

Review

Recent development in binderless fiber-board fabrication from

agricultural residues: A review
M. Nasir a, D.P. Khali b, M. Jawaid c, P.M. Tahir c,⇑, R. Siakeng c, M. Asim c,⇑, T.A. Khan d
a
Forest Products Utilization, College of Forestry, Banda University of Agriculture and Technology, Banda (BUAT), 210001 U.P., India
b
Forest Product Division, Forest Research Institute, Dehradun 248006, India
c
Laboratory of Biocomposite Technology, Institute of Tropical Forestry and Forest Products (INTROP), UPM, Serdang, Selangor 43400, Malaysia
d
Lab. of Adhesion & Bio-Composites, Program in Environmental Materials Science, College of Agriculture and Life Sciences, Seoul National University, Seoul 151-921, Republic of Korea

h i g h l i g h t s

Agriculture residues as an abundant resource for fiberboard.

Chemical, biological and mechanical methods of pretreatments.

Effect of particle size, pressing time and temperature on boards.

Mechanism of binderless fiberboards.

Physical, Mechanical, Thermal properties of binderless fibreboards.

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

Article history: The manufacturing of fiberboard from wood fiber with the help of adhesive is highly developed and
Received 22 November 2018 widely commercialized technique. However, with an increasing concern over health issues and biomass
Received in revised form 31 January 2019 conservation, the fiber boards from agriculture residues with or without using adhesives are under inten-
Accepted 22 March 2019
sive investigation. In last three decades, several researches have been done various methods and tech-
Available online 27 March 2019
nique dealing the development of binderless fiberboards such as wet process and dry process. This
review article also covered pretreatments of fiber which helps to find out optimum criteria for fabrication
Keywords:
of fibreboards. Fibre sizes in fibreboard were studied and found that the dimensions of fibres effect the
Agriculture waste
Binderless fiberboard
physical, mechanical and thermal properties. The pressing time and temperature influence the internal
Pretreatments bonding of binderless fibreboards. The mechanical and thermal properties of binderless fibresboard were
Pressing temperature discussed on various pressing time and temperature and compared with different type fibreboards. Effect
Mechanical properties and physical of hygrothermal properties on the physical, mechanical and thermal behavior of binderless were also dis-
properties cussed. This review summarized various aspects of self-bonding mechanism in binderless fibresboard
with a focus on agriculture residues based raw materials. Various aspects of binderless fiberboard man-
ufacturing such as raw material suitability, effects of pretreatments and manufacturing process on phys-
ical, mechanical and thermal properties are discussed. The chemical changes in fiber during
pretreatments and hot pressing is also discussed in detail. These binderless fiberboard showed the suit-
ability in use for indoor applications due to its non-toxic characteristics.
Ó 2019 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 503
1.1. Binderless fiberboards. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 504
2. Raw materials form agricultural residues. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 504
3. Lignin/enzymatic hydrolysis lignin (EHL) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 504
4. Pretreatment technique of binderless fibreboard. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 505

⇑ Corresponding authors.
E-mail addresses: parida.introp@gmail.com (P.M. Tahir), khanfatehvi@gmail.com (M. Asim).

https://doi.org/10.1016/j.conbuildmat.2019.03.279
0950-0618/Ó 2019 Elsevier Ltd. All rights reserved.
 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516 503

4.1. Steam explosion pretreatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 505

4.2. Steam injection pretreatment. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 506
4.3. Chemical pretreatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 506
4.4. Enzymatic pretreatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 506
5. Manufacturing process of binderless fibreboard . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 507
5.1. Effect of particle size. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 508
5.2. Effect of pressing temperature and time . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 508
6. Mechanism of binderless fiberboards . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 508
7. Properties of binderless fiberboards . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 509
7.1. Physical properties of binderless fibreboards . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 509
7.2. Mechanical properties of binderless fibreboards. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 510
7.3. Thermal properties of binderless fibreboard . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 511
7.4. Hygro-thermal properties of binderless fibreboards . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 512
7.4.1. Mechanical and thermal properties. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 513
8. Application . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 513
9. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 513
Conflict of interest. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 513
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 513
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 513

1. Introduction properties of binderless fibreboard should be done at a tempera-

Worldwide demand of renewable materials is due to wood scar-
city, demerits of synthetic materials. New environmental regula-
tions have stimulated and forced board manufacturers to seek
alternative sources of lignocellulosic fibers [1]. In such concern,
agricultural residue and its bioproducts from agro-industries were
high priority to the researches [2]. In development of biodegrad-
able composites such as fiberboards and particleboards, synthetic
adhesive are commonly used for building materials and structural
purposes [3]. Adhesive is an essential component of wood compos-
ite manufacturing. The formaldehyde based adhesives are the most
common adhesives, widely used in the industrial scale due to its
desirable performance and low cost [4,5]. Although, formaldehyde
has been categorized as carcinogenic and restricted to use in many
developed countries, it is still in practice due to non-availability of
suitable alternative [6]. The research and engineering interest has
been shifted from the above-mentioned materials to new bio-
based resins due to environmental concerns [7] and eventually to
self-bonding boards, free of synthetic adhesives [2,8].
A complete or partial replacement of formaldehyde based adhe-
sives with starch and protein is also under intensive investigation
[9,10]. However, the technique to fabricate fiberboards without
adhesives has promising hope in prospect the economic as well
as environmental. The initiative for binderless fiberboards was
started around three decades before, when industrial waste
bagasse was used to prepare composite through self-bonding tech-
nique [10] and a patent for the binderless fiberboards fabrication
for a pilot scale production [11].
Binderless fibreboard is developed high density fiberboard
(HDF), which can be produced without any adhesive. The process
of manufacturing HFD is basically two conditions wet process
and dry process. The bonding strength of board without additional
adhesive work on two distinct phenomenon; lignin-lignin and
lignin-polysaccharides cross-linking reactions that occur at high
temperature and other is work on the deformation condition of
the system under pressure because wood is a heterogeneous mate-
rial and have little contact area between adjacent wood elements.
To produce wood-wood contact, wood must deform to produce a
good adhesive bonding. The enhancement of contact area with
the polymers (present in the wood) due to deformation, work
under the minimum pressure called ‘‘the rubbery state” [12]. The
binderless or auto-adhesion fibreboards normally do not reach
the mechanical properties equivalent to phenolic based fiber-
boards. The research considers the improvement of mechanical
ture higher than the glass transition temperature (Tg) of all poly-
mers. In HDF manufacturing process, the temperature is
generally provided nearly 200 °C to softening the polymer and
increase the contact area [13]. Many researchers have discussed
that pressing temperature influenced the binderless boards’ prop-
erties significantly [14,15]. Other researcher found the lignin and
hemicellulose decomposition and chemical changes during hot
press process of self-bonding process [16].
Some researchers [3,17] worked on self-bonded materials to
develop binderless fibreboard made up of leaflets, rachis, leaf
sheath and fibrillum of date palm tree by-products. Initially, chem-
ical composition and morphological properties of binding material
were studied. Further, mechanical, physical and thermal properties
were studied. Hashim et al. [18] investigated the properties of
binderless fiberboard manufactured from oil palm trunk as a func-
tion of various temperatures. The prepared fibre board were inves-
tigated the mechanical, physical, structural, morphology and
thermal properties and found the effect of temperature during
preparation fibre board. Another study of binderless particleboard
from oil palm trunk biomass was analyzed based on various tem-
perature and pressure time on physical and mechanical properties
[19]. Based on the mechanical and physical results, the thickness
swelling, water absorption and internal bond strength of the pan-
els improved with reduction of the panel thickness. Kenaf core
materials were used conventional dry-manufacturing process to
develop binderless fiberboards to study various moisture content
(MC) and hot press time [20]. In the 30% MC, binderless fiberboards
exhibited better dimensional and mechanical properties than air-
dried binderless fiberboards. The pressure timing showed its effect
on the internal bonding and longer pressure timing effect the
thickness swelling as well. Another research based on the steam
exploded pretreatment of Miscanthus sinensis and produced
binderless fiberboard [21]. In this research pretreatment, pressing
time and mechanical properties were studied thoroughly. The
fiberboards obtained were of very good mechanical and physical
properties and revealed that decrease in hemicelluloses is clearly
related to the increase in the dimensional stability of the boards.
Although, many research researches have been done on laboratory
scale or pilot scale fabricating binderless fiberboard, but the poor
mechanical performance and lower water resistance of such
boards have limited their application in the industries [22–25].
This review paper deals with the increasing environmental con-
cern over forest and biodiversity conservation, it is requirement of
time to look for an alternative source of cellulosic materials to
504 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516
produce fiberboards. The non-woody raw materials, specifically
agriculture residues are suitable source for various methods of
self-bonding mechanism of fibreboards. The fiber surface modifica-
tion as well as lignin modification of cellulosic fiber through vari-
ous chemical and enzyme methods are studied its effect on the
properties of fibreboards. The physical, mechanical and thermal
properties of binderless boards were analyzed and found that lig-
nocellulosic materials can be used as raw material for fiberboard,
but all are not suitable for the economic and commercial produc-
tion due to various chemical composition. The hygro-thermal
study on physical, mechanical and thermal properties of binderless
fibreboards were also studied.
1.1. Binderless fiberboards
Many theories have been proposed on self-bonding mechanism
of binderless fiberboards, but the research is still restricted to the
laboratory scale [1,25,26]. The reason is the complicated mecha-
nisms involved in self-bonding during the hot pressing of fiber-
board. Therefore, a detailed study on self-bonding mechanism is
necessary for the standardization of manufacturing procedure for
an industrial application. In addition to study fiber modification,
another aspect to enhance self-bonding mechanism is in-situ lignin
modification.
In manufacturing process, hot press is one of the most important
parameter to influence the fiberboard properties. Without synthetic
resin, binderless fibreboard is mainly accomplished using naturally
occurring materials within fibres. Okuda et al. [27] has revealed the
hemicelluloses and lignin decomposition process during the hot
pressing. The self-bonding mechanism in fibreboards work based
on the condensation reactions of lignin and glucose content of the
boards decreased with increasing pressing temperature. Another
study by Bouajila et al. [12], revealed that mechanical strength of
binderless fibreboards are depend on the lignin-lignin and lignin-
polysaccharide cross-linking reactions that reaction activate at the
high temperature and deformation of the system under pressure.
The chemical activation reactions and physical consolidation of par-
ticles under applied heat and pressure can develop self-bonding
reaction in binderless fibreboards [14]. Breakage of hemicelluloses
and cellulose produce simple sugar which contribute in self-
bonding in boards [28]. Crosslinking of carbohydrate polymers and
lignin may also cause of bonding [27]. Another researcher Chao
[29] reported that internal bonding in binderless panels made from
bark arose from particle consolidation. Various theories have been
proposed such as: soy-lignin based adhesive[30], condensed
organosolv lignin based [24,31]and lignin-furfural linkages
[25,32]. Furthermore, the physical properties of lignin such as plas-
ticizing at high temperature and condensed at low temperature is
also contributes into the self-bonding mechanism [12,33].
In binderless board fabrication, the fiber surface, its composition
and assembly procedures are the major factors determines the self-
bonding. Various instruments are used to assess the changes in
properties of binderless boards for example; thermo-gravimetric
analysis (TGA), fourier infrared spectroscopy (FT-IR), X-ray diffrac-
tion (XRD), Nuclear magnetic resonance (NMR) and gas chromatog-
raphy–mass spectrometry (GC–MS). Although the chemical changes
before and after pressing can be examined. Since, the board pressing
is a dynamic process and depends on the pressing time and platen
temperature, the product properties change accordingly [24]. Thus,
an optimum manufacturing process is to be develop dealing a corre-
lation between functional groups and manufacturing variables.
2. Raw materials form agricultural residues
Agricultural residues are the leftover parts of produce, accumu-
lated after the harvesting annual crops and it is available only in
seasons. Being an agrarian economy, India produce a wide range
of crops along with their residues. It is estimated that more than
500MT of residues are produced annually from major crops in India
[34]. Although, 65% of these residues are utilized for animal feed-
ing, bio-manuring, soil mulching, temporary homes and fuel for
domestic and industrial use but a major portion is remained
unused [34]. Nowadays, burning of rice residues on-farm for clear-
ing the field is a serious concern in northwest India. Table 1 exhi-
bits the comparative availability of agriculture residues in India
and around the world. In general, non-woody fibers such as agri-
culture residues contains higher proportion of hemicellulose as
compare to woody fibers which makes it more susceptible to mois-
ture [35]. However, in contrast to its hygroscopic nature, the high
amount of hemicellulose helps in better fiber to fiber binding.
There are many examples where agriculture residues which have
been used in fiberboards fabrication with addition of various
adhesive.
The relevant information of agriculture residues as raw material
in composite industry is scattered and scarce compared to the
wood. However, this abundant natural and renewable resource
has a great potential for solid wood replacement, if the chemical
structural and composition of cellulose and lignin and their modi-
fications are studied in detail [36]. Utilizing agriculture waste such
as rice straw [37], wheat straws [1], oil palm [23,25], coconuts [22],
bagasse [8], bamboo [38], banana bunch [39] and kenaf fiber [40].
Although, many researches and theories have been proposed on
binderless boards fabrication from various non-woody fibers, but
the dimensional stability is a challenge for such boards.
3. Lignin/enzymatic hydrolysis lignin (EHL)
In woody materials, lignin acts as permanent bonding agents
between cells to provide the definite composite structure with out-
standing resistant of biological effects and physical such as impact,
compression, and bending [42]. Lignin is naturally one of the most
abundant materials and renewable resources, it is phenylpropane
derivative based an amorphous natural polymeric material. It is
extracted from three hydroxy-cinnamyl alcohols or monolignols
of phenolic polymer derivative by free radical generation followed
by chemical coupling process such as p-coumaryl alcohol (MH),
coniferyl alcohol (MG) and sinapyl alcohol (MS) [36,43] shown in
Fig. 1. Several researches have been conducted on lignin such as
structural features, constitutional and mechanism of formation to
define lignin. The definition of lignin has never been as clear as that
of other natural polymers such as cellulose and protein due to
extremely complicated isolation, compositional analysis and struc-
tural characterization [43].
Lignin has a class of phenolic natural polymers with broad com-
positions and a variety of linkages between units though it is
Table 1
Comparative table of major agriculture crop residues produce in world and India
[25,34,41].
Raw Material World Agricultural India Agriculture
Residue (MT) Residue (MT)
Cotton (Linters, Staple, Stalks) 89 75.9
Sugarcane Bagasse 102 11.6
Sorghum Stalks 252 17.6
Corn Stalks 750 35.8
Mustard and rapeseed – 12.7
Flax (oil seed) 2 0.3
Rye 40 12.7
Oat 55 –
Barley 195 1.6
Rice 360 154
Wheat 600 131.1
Total Residues 2445.2 552.3
 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516 505

binderless fiberboard made from steam-exploded non-wood

Fig. 1. Three primary lignin monomers: (a) monolignols p-coumaryl alcohol, (b)
coniferyl alcohol and (c) sinapyl alcohols [36] (with permission).
defined as a compound. By nature, lignin has no regularly repeat-
ing multi-unit structures, variation in composition and structure
form its origin which is main reason of lack of precise definition
for lignin [43]. Ralph et al. [44] studied that lignin is biopolymers
consisting of phenylpropanoid units with an oxygen atom at the
p-position (as HO or O–C) and with none, one or two methoxyl
groups in the o-position to this oxygen atom. Lignin is a natural
adhesive that act as binding force between cellulose fibers. Many
researchers have proposed lignin-based bio-adhesives and applied
in fiberboard [38,45]. When agriculture residues are heated, lignin
plasticization and reacts with furfural that forms a lignin-furfural
complex which is believed to participate in self-bonding [46].
Therefore, the addition of lignin in binderless fiberboard fabrica-
tion further enhances the dimensional stability and the mechanical
strength. The kraft lignin performed better among all other kind of
lignin [47].
Since the large molecules of lignin are hydrophobic in nature
it resists water penetration, thus it reduces the water absorption
and thickness swelling of fiberboards. furthermore, being a natu-
ral component of cellulosic fiber, the lignin provided more reac-
tive sites to treated cellulose (activated fibre surface), thus
increasing the links between cellulose fibers [48]. In another
experiment, Velasquez et al. [47] investigated that the mixing
of kraft lignin before pretreatment improved the properties of
fibers. The enzymatic hydrolysis lignin (EHL) obtained from pre-
treatment of poplar fibers was utilized for binderless fiberboards
fabrication [49]. The fiberboards exhibited significant improve-
ment in physical and mechanical properties. Nasir et al. [50]
treated rubber wood fiber with laccase enzyme and separated
EHL formed in reaction. That EHL was further go through con-
densation to remove excess of moisture and reused in fiber-
boards fabrication. The result was attributed to have double
benefit; first enzyme activated the cellulosic fiber surface and
second the condense EHL is acting as an adhesive. The obtained
fiberboards were passing the minimum required strength but not
good enough to with stand in water resistant test.
4. Pretreatment technique of binderless fibreboard
The synthetic adhesive used in fiberboards are the sole binding
force between the fibers. It provides sufficient mechanical and
physical properties along with the desired dimensional stability.
Therefore, the fabrication of fiberboards without adhesive is diffi-
cult to convince. In last two decades many chemical and enzymatic
pretreatments techniques have been developed which has proven
their role in fiber to fiber bonding through different procedure
[24,39,48,51]. Table 2 summarized the recent developments in fab-
rication of binderless board from agriculture residues. In most of
the cases the focus of pretreatments is to exposure of lignin and
hemicellulose onto the surface of cellulosic fiber that will further
participate in reaction during hot pressing. Recently, the pretreat-
ment processes such as steam explosion, steam injection, chemical
pretreatments, enzyme pretreatments are under intensive study
which are claimed to enhance the self-bonding in fiberboards
(see Table 3).
4.1. Steam explosion pretreatment
Mason [60], used the steam explosion (SE) method to separate
cellulosic fiber into their main components i.e. cellulose, lignin

Table 2
Binderless fiberboard prepared from various pretreatment process from various agriculture residues.

Raw material Pretreatments Binderless board Properties Reference

Oil Palm Steam explosion Boards prepared from steam explosion have positive impact on strength however a severe steam [25]
explosion results into poor strength
Miscanthus sinensis Steam explosion/ Very good quality binderless boards were prepared with high modulus of elasticity [47]
lignin addition
Kenaf core Steam injection Board produced from higher steam pressure and 30% moisture content had higher IB strength [52]
Coconuts Chemical Fiberboard is prepared from lignin utilized as intrinsic thermosetting binder [22]
treatments
Cynaracardunculus Steam explosion Optimized the pretreatment conditions for binderless board manufacturing [15]
Banana bunch Steam explosion Studied the chemical changes during steam explosion and concluded that the decrease in xylans amount [39]
increase the dimensional stability of the fiberboards
Bamboo Steam explosion Role of intermonomer linkages of lignin, i.e. b-aryl-ether linkage is formed during steaming [53]
wheat straw Fenton’s reagent Fiberboard pass the minimum required strength [1]
Cotton stock Electromagnetic High frequency (HF) electromagnetic (EM) radiation with frequencies above 400 MHz was used during [54]
radiation board pressing
Corn stock Trametes hirsute Board had almost double strength when compared to untreated boards [55]
corn stover Enzyme hydrolysis The platen temperature must have kept as high as Tg value of EHL [33]
lignin (EHL)
Plantain Laccase Studied the laccase induced phenoxy radicals of lignin which can generate covalent bonds [2]
Cotton stalks Nano-size Particle Prepared binderless green nanocomposites from the fine fraction of cotton stalks [16]
Rice straw Hot pressing The internal bonding strength of binderless boards made from rice straw was relatively higher than other [37]
residues due to presence of wax-like substances on the epidermis of rice straw
Triarrhenasacchariflora White-rot fungus The fibreboard prepared from optimized bio-pretreatment parameters was stronger than the untreated [56]
fiberboards
Wheat straw In-situ spent Results showed further increase in overall properties if soda lignin was added externally [57]
liquors
Wheat straw Laccase Fiberboard was manufactured successfully at optimized laccase-pretreatment conditions [58]
Tomato and maize Thermo-pressing The material with had very low internal binding and very high ash content. Raw material is not [59]
material recommended for binderless boards
506 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516
Table 3
Manufacturing process of binderless fibreboards [17,20,95].
Wet process
The moisture content of lignocellulosic materials increased up to 30% by
spraying water
Wet-forming process involves the distribution of cellulosic materials into
water
Steam explosion technique used for efficiently expose components for
further reaction in hot pressing
While a wet process to produce binderless fiberboards from a combination
of fibers and particles has been patented in 2013
Main disadvantage- low density, limited strength of fiberboards, along with
waste water pollution
and hemicellulose, to produce hardboard and the process was
described as Masonite. In this method, cellulosic materials are
exposed to high pressure saturated steam, followed by suddenly
reduction in pressure. That results into an explosive decomposition
of cellulosic materials. In this decomposition process, the lignin
starts depolymerizing and consequently the hemicelluloses are
hydrolyzed easily [61]. Thus, most of the hemicelluloses are dis-
solved into solution while the cellulose fraction remains intact
[62]. The efficiency of this method depends on time (t), tempera-
ture (T), and particle size (S) [38]. This method claims to be one
of the most successful pretreatment methods for separating ligno-
cellulosic materials into their major components and it further
enhance the susceptibility towards enzymatic hydrolysis [63].The
thermal gravimetric analysis (TGA) and differential scanning
calorimetry (DSC) reveals that the softening temperature of sepa-
rated lignin was lower than original [64]. The ozonation and
NMR analysis confirms that lignin molecules had cleavage of b-
O-4 linkages [53]. Due to linkage breakdown, the steam treatment
creates more reactive sites of phenolic hydroxyl ends and that sites
are believed to contribute in self-bonding during fiberboard fabri-
cation. The scanning electron microscope revels that the liberated
lignin is deposited on the surface of fibers of hemicelluloses and
cellulose, which restrict the water absorption [65]. Consequently,
the dimensional stability of binderless fiberboards is improved.
Although, the steam explosion method is an environmentally
friendly and requires low capital investment, the degradation of
cellulose, hemicelluloses and lignin is difficult to control.
4.2. Steam injection pretreatment
In steam treatment fibers are exposed to high pressure and
temperature that leads to the formation of acetic acid [12]. Conse-
quently, it initiates the degradation of fiber components i.e. hemi-
cellulose, lignin, and amorphous cellulose. In this degradation
reactions the hemicellulose generates furfural products, which
plays a significant role in fiber to fiber bonding of self-bonded
fiberboards [12]. Moreover, at high temperature the lignin become
soft and form lignin-furfural due to condensation reaction which is
further adding to the binding strength [33]. Although the proce-
dure of steam explosion and steam injection are similar, but the
degraded components are washed away with water in case of
steam explosion, while all the fractions are remained in the fibers
in steam injection process [66].
Geimer and Price [67] prepared the particle boards through
steam injection pressing of southern hardwoods particles. There-
after, this technology was applied to fabricate various binderless
fiberboards from softwood, hardwood and/or mixed wood
[68,69]. Although the obtained bonding strength was poor, but it
had improved dimensional stability. Many researchers [52,70]
used steam injection pressing technique to fabricate particleboards
from kenaf core. It was observed that steam injection has direct
Dry process
Hydrogen bonds formation and thermosetting adhesive behavior of lignin are
expected during heating and drying processes
Moisture content of cellulosic materials is reduced via drying process before hot
press
Industrial manufacture of binderless fiberboards is mainly based on dry-forming
process without resins addition
Microwave pretreatment is applied to the dry-forming process. It increased
temperature and assist binderless fiberboards with a high density and thickness,
as well as acceptable properties, were obtained
relation with bonding strength. The panel showed improved IB
strength as compared to the boards made by hot pressing, but it
performed poor in TS test [52]. The research on binderless fiber-
boards fabrication through steam injection technique is still under
progress.
4.3. Chemical pretreatment
The Fenton’s reagent is the composition of ferrous chloride and
hydrogen peroxide, it is use to activate the cellulosic fiber surfaces
[71]. In this oxidation pretreatment, the hydroxyl radicals are con-
tinuously generated from decomposition of hydrogen peroxide in
presence of ferrous ions. Consequently, the hydroxyl radicals are
reacting with lignin on fiber surface to form reactive components
[72]. These activated chemical components form a covalent bond
with other activated low-molecules and contributes to self-
bonding in binderless fiberboards [73]. Furthermore, the diffusion
of degraded low-molecular components into lumen within cell
walls developed an intra-fiber crossing links. These intra-fiber links
are believed to enhance the dimensional stability of fiberboards
[1,74]. Halvarsson et al. [1] fabricated binderless fiberboards from
wheat straw treated with Fenton’s reagent. The mechanical prop-
erties and water resistance of the binderless boards was further
enhanced when the percentage of hydrogen peroxide was
increased from 2.5 to 4.0%. Furthermore, Henao et al. [75] per-
formed the fenton’s reagent oxidation on oil palm keeping hydro-
gen per oxide 4% and the treated fibers were pressed at 190 °C
temperature to fabricate binderless fiberboard. The obtained
boards exhibited lower thickness swelling and water absorption
35% and 48%, respectively which was less than the wheat based
binderless fiberboard [75]. Thus, it was concluded that the raw
material selection is an important factor that determine the
strength of binderless fiberboards. Although, the result of chemical
pretreatments is interesting, it has several weaknesses such as the
properties of fiberboards deteriorated with time due to high perox-
ide charges, insufficient mechanical strength and instability of
board quality [74].
4.4. Enzymatic pretreatment
Enzyme treatments are generally involved a mild reaction con-
dition compared to chemical treatments, which is harsh and gener-
ates many by-products. Thus, the interest in enzymatic treatments
of cellulosic fibers is recently growing [76–78]. White-rot fungi are
natural agent that secrete lignin-degrading enzymes such as lac-
case (EC 1.10.3.2), lignin peroxidase (EC 1.11.1.14), and manganese
peroxidase (EC 1.11.1.13) [79]. Laccase enzyme is widely dis-
tributed in white rot fungi, has been studied intensively for delig-
nification in the pulp and paper industry. Laccase efficiently
degrade and mineralize lignin into CO2 and H2O [55]. It catalyzed
one-electron oxidations in lignin and generate free radicals that
 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516 507

Fig. 2. Simplified reaction mechanism, describing the free radical polymerization [83].

Fig. 3. SEM image of fiber surface: A- untreated, B- laccase treated [4].

can react with other phenolic components, and intimate cross-
linking [80].
Based on this theory, a laccase treated lignin-based adhesives
was produced and fiberboards were manufactured made from
laccase-oxidized wood fibers [81]. Laccase mostly being a large size
dose not react with intercellular lignin but oxidized the extracellu-
lar lignin [82] and generates free radicals on the fiber surface. Fig. 2
shows the simplified reaction procedure of lignin. These free radi-
cals in the form of lignans and lignons act as potential reactive sites
for further cross-linking reactions and form large polymer chain of
lignin. Felby et al. [26] studied lignin obtained from the surface of
laccase-treated fiberboards and concluded that the increase in
molecular weight is an indication of lignin polymerization.
Felby et al. [84] prepared the fiberboards from laccase-treated
beech fibers and compared the wet strength to the boards made
from untreated fiber. The improve bonding strength was believed
to be due to deposition of oxidized lignin on the fiber surface
[4,17]. Nasir et al. [24] prepared binderless fiberboards from rubber
fibers treated with laccase at different concentration and time.
Fig. 3 exhibits the rubberwood fiber treated with laccase, a smooth
and thick layered was observed when compare to untreated fibers
[50]. The prepared fiberboards improved mechanical strength in
acceptable range when treated at 9 U/g concentration for 1 h.
Furthermore, it was concluded that the optimization of enzyme
treatment is necessary an excessive amount of enzyme or time will
lead to poor performance of fiber [50,55]. In addition to enzyme
treatment of fibers other parameters of fiberboards manufacturing
is to be considered such wood fiber type and effect of preheating
temperature to improve the self-bonding [85,86]. Although enzy-
matic treatment has the potential to improve bonding strength,
but the commercial application is still difficult due to its biological
nature, enzyme behave differently in different reaction condition.
5. Manufacturing process of binderless fibreboard
Fiberboards are manufactured through two separate process,
namely ‘‘wet-process’’ and ‘‘dry-process’’. In wet-process, the
water-distributed cellulosic fibers are pressed at high temperature
with or without adhesive. Thus, the hydrogen bonding and lignin
plasticizing are the only bonding forces, formed during heating
and drying processes of wet-process [87]. In wet process, lower
mechanical strength and poor water resistance are the main disad-
vantage, along with the waste of water in the process. In dry-
process, cellulosic fibers are dried first followed by addition of
resins and finally pressed at curing temperature [87]. The industry
follows mainly dry-process manufacturing procedure with an
508 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516
addition of synthetic resins. The raw material rich in lignin and
hemicelluloses are preferred for binderless fiberboards prepara-
tion. The pretreatments such as steaming, chemical or enzyme pre-
treatments modifies the fiber composition which is believed to
play an important role in self-bonding. Thus, the binderless boards
manufacturing involves two major processes: pretreatment fol-
lowed by hot-pressing. Several theories such as furan-lignin pro-
cess [88,89], the steam explosion process before hot pressing
[25,90] and steam injection pressing [52,70] and laccase treatment
[26,84,91] methods have proven their suitability. So far, the steam
treatment is believed to be the most effective method of binderless
board formation gives better strength and dimensional stability.
During hot pressing, the cellulosic components undergoes to many
changes and achieve self-bonding. The cleavage of b-O-40 linkages
of lignin during steam explosion and formation of lignin-furfural
contributes to self-bonding of lignocellulosic materials. Thus, the
pressing parameters such as temperature, pressure and time are
important factor to be studied in detail. The effect of pressing tem-
perature has been studied on various biomass such as Miscanthus
sinensis [47], oil palm fiber [90,92] and kenaf core [93]. It was
observed that properties of boards are affected by some most
important manufacturing parameters such as pressing tempera-
ture. Boon et al. [94] analyzed the temperature, time and pressure
and concluded that pressing temperature was the most influential
parameter, however, the pressure and time were not very effective
after a certain stage. However, the temperature should be kept
below 200 °C to avoid fiber burning. Apart of these parameter, fiber
moisture is also a crucial factor that determines the heat transfer
during pressing time. The permissible range of moisture content
is 5–20 wt% of fiber whereas the high moisture contents have a
negative on modulus.
5.1. Effect of particle size
Under heat and pressure, fiberboards consist of various shape
and sizes of fibres bonded together with an adhesive [92]. The
impact of fibres size on the properties of the boards were measured
significantly [96]. Binderless fiberboards are composition of parti-
cles of different dimensions of lignocellulosic materials and the
internal binding forces originate from the activation of chemical
components by applying heat and pressure [69,97]. Miyamoto
et al. [98] studied that particle dimension affect the linear expan-
sion of particleboard. Though, Sackey et al. [99] found out that
the both fines content and the ratio of all particle-size fractions
strongly influenced the internal bond strength of the samples.
Lamaming et al. [100] reviewed the role of particle size in particle
boards and found that particle dimensions affects board character-
istics including linear stability, surface roughness, water absorp-
tion, thickness and mechanical strength. Boards of fine particles
required higher energy and time in production but gives smooth
surface. Many researchers [18,101] investigated that the particle
dimensions have significant part in improving the properties of
board rather than the actual strength of the fibers. Frybort et al.
[96] found the variation in dimensions of particle also influences
overall panel properties and dimensional variation can build major
impact on the properties of boards. As the particle dimensions
influencing the performance and properties of the boards, deter-
mining the range of particle size used in making the board was
an important parameter [100]. A study [18]on roughness profile
on various press temperature were suggested that when the press
temperature increased the surfaces of the samples became
smoother due to higher densification of the surface layer with
increasing temperature. The morphological effect of rice straw par-
ticles and whole powder on binderless board investigated and
found the panel made by particles could be easily break and
divided into particles by using hand pressure only, resulting in fall-
ing apart before testing. However, the boards made up of rice pow-
der were successfully manufactured by a simple method based on
grinding and hot-pressing process.
5.2. Effect of pressing temperature and time
In manufacturing process of boards, pressing temperature of is
one of the very important parameter that influence the properties
of boards. Without synthetic resin, the temperature help in binding
the binderless board through activating chemical reaction of lignin
available in the fibers. Okuda et al. [93] described that during the
pressing process hemicellulose and lignin were decomposed, self-
bonding mechanism initiated in board when condensation reac-
tions of lignin occur and with increasing pressing temperature
the sugar content of the boards decreased. Bouajila et al. [12] stud-
ied on bonding properties of binderless board and found that
lignin-lignin and lignin-polysaccharide cross-linking reactions
occur at high temperature and deformation of the system under
pressure. Another researcher Hashim et al. [18] reviewed that
binderless boards are developed by sorghum which is sugar-
containing lignocellulosic materials, pressed at a temperature of
180 °C or higher to achieve satisfactory bonding. Salvadò et al.
[102] studied the pretreatment and various pressing temperature
on the board and found improvement in properties. The process
of hemicellulose degradation and partially degradation of cellulose
produce simple sugar that contribute to bonding in binderless
boards made from steam-exploded materials [18]. Baskaran et al.
[19] studied the pressing temperature and time on oil palm trunk
biomass and found that the improvement in internal bond strength
of particleboard were due to increasing press temperature,
Whereas the increase in the press time caused adverse effect on
internal bond strength.
This result justified that press temperature more likely influ-
ence the internal bonding of boards. Further study based on thick-
ness, the lower thickness of board showed higher internal bond
strength values compared to the higher thickness, it might be
due to the higher compaction ratio of particles in lower thickness
board.
6. Mechanism of binderless fiberboards
The white rot fungi produce a group of enzymes that degrade
cellulosic compounds. The laccase enzyme specifically acts on lig-
nin molecules and degrades it to smaller molecules which leads to
the free radical reaction. However, the chemical changes during
enzyme reaction and their role in self-bonding is still needed to
study in detail [17]. The mechanical, chemical, biological pretreat-
ments can be employed separately or in combination, to obtain the
best physical and mechanical properties of binderless boards. The
self-bonding between fibers, differs with chemical, physical and
morphological properties of raw materials as well as manufactur-
ing process followed [103]. At the time of hot pressing, several
reactions such as dehydration, hydrolysis and oxidation reaction
are observed. Being a poor thermally stable compound, hemicellu-
loses are believed to be decomposed first into organic acid, acetone
and furfural followed by lignin and cellulose [52,104]. Okuda et al.
[93] studied the binderless fiberboards from kenaf fiber and
observed a little role of furfurals-lignin bonding. Furthermore, it
is suggested that the condensation reactions in lignin and chemical
reaction from conjugated carbonyl compounds played an impor-
tant role in self-bonding.
Alvarez et al. [68] studied the effect of extractives of leaf plan-
tain on self-bonding and observed that the organic extractives
decreases the self-bonding of fibers when deposited on the surface.
However, in contrary the water extractives exhibited a positive
 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516
effect on the mechanical properties when it is deposited on the
fiber surfaces. The water-based extractives with lower molecular
weight eased the formation of stable free radicals that results into
better bonding. Sun et al. [69] compared lignin molecule in original
raw materials as well as in binderless fiberboards prepared by hot
pressing. The obtained enzymatic/mild acidolysis lignin (EMAL)
was analyzed under gel permeation chromatography (GPC) analy-
sis and observed revealed that molecular weight of lignin mole-
cules was decreased from 2210 to 1630 g/mol. Furthermore, the
NMR result exhibited increase in number of b-O-4 linkages after
fabrication of binderless fiberboards [69]. The self-bonding mech-
anism by steam exposition method is more complex due to the
variations in steam treatment conditions. The degradation of hemi-
celluloses is highly dependent on temperature, moisture content,
time of treatment and the composition of raw materials.
7. Properties of binderless fiberboards
7.1. Physical properties of binderless fibreboards
In physical properties of binderless boards, water absorption is
one of the main issue to encountered with natural fibers and
polysaccharide based materials [105,106]. A research based on
unripe coconut husks binderless fiberboards showed increasing
in the pressing temperature decreased the swelling and the water
uptake of the fiberboards. The covalent crosslinking bonds present
in inter-fiber are main responsible for moisture resistant than
hydrogen bonding in water molecules [107]. Non-crystalline
region of the cellulose chains and hemicelluloses are very hydro-
philic due to the availability of hydroxyl groups, the hydrophilic
character of hemicellulose in the biomass can be reduce by thermal
degradation [108]. The hydrogen bonding attracts hydroxyl groups
and hold water molecules, this discussion agrees with the FTIR
result showed in Fig. 4. Fiberboards processed at 220 °C, 230 °C,
and 240 °C showed the smallest values for the studies characteris-
tics. The fiberboards processed above this temperature 215 °C a
complete cure reaction due to exothermic event. This temperature
define the homogeneity as well as the lower swelling and water
uptake of the fiberboards [107]. Another study based of binderless
Fig. 4. FTIR graph of coconut husk fibers and fibreboards on various press temperature [107] (with permission).
509
particleboard made from oil palm trunk on various press tempera-
ture found thickness swelling and water absorption of the boards
produced ranged from 18% to 109% as shown in Fig. 5 [18]. The
water absorption (WA) and thickness swelling (TS) of the panels
decreased with increasing press temperature. According to Japa-
nese Industrial Standards [109], thickness swelling of board should
not exceed 12%, though, in spite of increasing the temperature,
none of sample reached to the standard TS requirement. Higher
percentage of thickness swelling in boards made up of agricultural
materials may be due to their internal structure [110].
A study [20] based on the TS of binderless fiberboard showed
the TS values of binderless fiberboard after 24 h of immersion in
water at 20 °C. 0.8 MPa/30 min refined condition fibreboard
showed 11.7% TS at 0.5 g/cm3 board density. A study [111] based
on dimension stability of steam-pretreated board indicated the
reduction in hygroscopicity and improved dimensional stability,
due to the changes in hemicelluloses percentage affected in steam
pretreatment. The improved dimensional stability also contributed
to reductions of elasticity. Another study [90] revealed that severe
steam explosion conditions for high dimensional stability lost elas-
ticity of fibres through destruction of the aromatic nuclei of lignin.
Physical properties of Binderless particleboards developed from
heartwood and sapwood of sugi (Cryptomeria japonica D. Don)
was investigated the effect of pressing time and temperature on
the TS and WA at a constant density of 1.0 g/cm3. With increasing
pressing time and temperature, water absorption capacity was
reduced and enhanced the dimension stability, and heartwood
board showed lower WA and TS than sapwood due to better inter-
nal bonding. Overall pressing time, temperature and density
showed very important role in physical properties of binderless
particle board [112]. Another study of binderless fiberboards from
Arundo donax L. investigated the physical properties on various
pressing pressure and density [113]. The pressing pressure
15 MPa showed highest density and very less voids. In general,
for the same fibers weight, fiberboard pressed at higher pressing
pressure can hold less volume, and consequently the density is
increased. According to the European standard (EN317), WA and
thickness swelling (TS) of fibreboard were investigated after
immersing in water for 24 h at room temperature. The steam
510 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516
Fig. 5. water absorption (a) and thickness swelling (b) at different press temperature [18] (with permission).
exploded fibres in fibreboard showed minimum TS (13.3%) at pres-
sure 10 MPa and according to the European standard (EN317), the
TS and WA of fibreboard should be less than 20% and 30%, respec-
tively. The hydrophobic characteristic of steam-exploded Arundo
donax fibers improved the improved the dimension stability of
fibreboard. The steam explosion reduced extractives and hemicel-
luloses contents of the raw material and the lignin can easily exude
from the cell wall to the fiber surface [64] which prevent water to
enter into the fiber’s molecular chains and consequently improved
the water resistance of the boards [114]. Another reason of water
resistant is lignin content in cell wall, which makes cellulose
hydrophobic. In addition, the non-polar hydro-carbon chains and
aromatic rings in the lignin molecule at fiber surface are able to
improve the water resistance of fiberboards [115,116]. The same
effect was observed when adding exogenous Kraft lignin as green
adhesive in fiberboards made from other agricultural wastes
[57,115].
7.2. Mechanical properties of binderless fibreboards
Unripe coconut husks binderless fiberboards were developed at
210 °C pressing temperature exhibited the highest modulus of rup-
ture (MOR) and highest modulus of elasticity (MOE), 3410 MPa,
among all fibreboards. According to Japanese standard Association
(JIS A 5908: 2003) [117], minimum requirement of MOR of the
boards must have 18 MPa. Higher thermal condition of boards
can degrade lignin content which negatively affect the mechanical
properties of the fiberboards [39].
Back [118] studied thermal effect on the MOR and MOE of
binderless fiberboards and found the tensile strength of the fiber-
boards was reduced at 230 °C than that of other samples. Though
the modulus of elasticity was increased due to auto-crosslinking
of wood polymers, since hydrolytic reactions produces failure
points where stress concentration occurs on loading, it reduces
the tensile strength. Decomposition of cellulose occurs at high
temperature negative impact on mechanical properties, the types
of bond formation influence several factors such as load, the mod-
ulus of elasticity, the bending stiffness and the impact strength
[107]. Binderless cellulosic fibreboards from microfibrillated ligno-
cellulosic flex fibre were investigated the effect of pretreatment on
mechanical properties [119]. After increasing refinement time
revealed a clear improvement of both flexural modulus and flexu-
ral strength shown in Fig. 6. A longer refinement time showed
slight reduction in flexural properties which showed the massive
mechanical treatment lead to destruction and cutting of the fibrous
microstructure and a subsequent loss of mechanical properties.
The length of fibres also influence the mechanical properties of
board, it is presumed that initially higher lengths of fibre may also
have higher fibre lengths after fibrillation, potentially leading to
higher strengths. On the similar context, long, micro or nanocellu-
lose fibres of high aspect ratio are desired as reinforcement mate-
rials in fibreboards as they are more effective in transferring loads
and to stopping cracks [120,121]. Another study of oil palm trunk
as binderless particleboard were investigated the mechanical prop-
erties on various press temperature [18]. The board pressed at
200 °C revealed highest MOR values of 5.73 MPa and it showed
That MOR values of the samples improved while enhancing the
press temperature. Though the internal bond strength of board at
200 °C was slightly lower than panel pressed at a temperature of
180 °C. The MOR value at 200 °C showed 28.3% lower than the min-
imum required MOR value as stated by Japanese Standards [109].A
comparative study of mechanical properties of binderless panels
manufactured from oil palm fibre board and softwood fibre board
were investigated [18,64]. Oil palm fibres has higher density
 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516
Fig. 6. Effect of refining time on flexural strength and modulus [119] (with permission).
compared to the softwood species are responsible for non-uniform
contact between fibers, making lower bending strength of the pan-
els inevitable. It showed lower press time is insufficient to create
strong bonding between the fibers. Pretreated wheat straw binder-
less fibreboards were compared with melamine modified UF resin
based on mechanical strength [1]. The medium-density fibreboard
(MDF) produced from straw and melamine modified UF resin with
density above 800 kg/m3 showed the MOR, MOE and internal bond
(IB) were lower than those of conventional developed wheat straw
fibreboards but close to the requirements of the MDF standard (EN
622-5: 2006). The H2O2 activated straw fibreboards showed rela-
tively high-water absorption properties but after addition of CaCl2
into the defibrator system as a water-repelling agent it reduced by
25%. Mechanical and physical properties of the straw fibreboard
improved after increasing level of hydrogen peroxide.
Pretreated banana bunch binderless fiberboard were investi-
gated the MOR based on various treatments with various pressing
temperatures [39]. The treatments were showed its effectiveness
at high temperatures of pressing rather than at low temperatures.
The lignin fluidity on fibers was increased at higher pressing tem-
perature, it homogenized the lignin distribution in fibreboards and
formed better inter-fiber bond. When severities for M. sinensis
superior results were observed, the quality of banana bunch fiber-
board were decreased at high severities treatment [21], It may be
because of increment in the molecular weight of lignin that causes
a diminution in the binder lignin properties [122], therefore, sever-
ities higher to 3.5 are not recommended.
Mechanical properties of Binderless particleboards developed
from heartwood and sapwood of sugi (Cryptomeria japonica D.
Don) was investigated the relationship between board density
and internal bonding pressed at 200 °C for 20 min [112]. The inter-
nal bonding of heartwood particleboards was twice than sapwood
particleboard. The general phenomenon of internal bonding of
binderless boards used to enhance with increasing the board den-
sity. A study based on low density binderless particleboards of
kenaf core using steam injection pressing showed internal bonding
of 0.1 MPa at a density of 0.2 g/cm3 [123].Okuda and Sato [124]
found kenaf core binderless board with an internal bonding of
5.7 MPa at a density of 1.0 g/cm3 by hot-pressing. The comparison
of sugi with kenaf core showed that sugi binderless particle board
can make higher internal bonding if the density is relatively high.
7.3. Thermal properties of binderless fibreboard
Many researchers have been reported the thermal properties of
binderless fibreboards. Binderless fiberboards made from unripe
511
coconut husks indicated that differential scanning calorimetry
(DSC) curves revealed exothermic peak from 140 to 210 °C in
the heating cycle which corresponds to the cure reactions of lignin
[107]. Adhesion of fibres in fibreboard occurred around 140 °C due
to formation of hydrogen bonds and covalent bonds [17,97] and
above the 180 °C under applied pressure, the auto-crosslinking
reactions on the polymer chains started [118]. DSC curve of the
fiberboards revealed significant reduction of the exothermic inten-
sity peak at 275 °C when the pressing temperature were increased
shown in Fig. 7.
The exothermic peak of raw materials at this temperature could
attributed to the carbonization of biomacromolecules in the fiber
and the pith [125]. In case of fibreboard, when the fiberboards
are thermopressed, some carbonization occurs which reduced the
intensity of the exothermic peak of thermopressed boards at
higher temperatures (see Fig. 8).
Thermogravimetric analysis of unripe coconut husks based
fibre board was observed the mass loss in the temperature range
of 50–500 °C. The raw material showed weight loss at lower
temperature attributed water molecule present. In range of
230–475 °C, fibreboards revealed significant mass losses which
indicated the pyrolysis of the raw materials also indicated the
dependency of thermal stability on the pressing temperature.
Many researchers [126–128] reported the thermal degradation
of the plant biomacromolecules in temperature range 200–
260 °C for hemicellulose, for cellulose and lignin 240–350 °C
and 280–500 °C, respectively. High pressing temperature shifted
mass loss at higher temperature. Another thermal study on fibre-
board at various press temperature showed initial weight loss
between 200 °C and 300 °C [18]. The initial decomposition could
be due to the evaporation of hydroxyl group and partially
decomposition of hemicellulose [129]. The manufactured board
at 160 °C and 180 °C showed higher weight loss while at
200 °C had the highest initial degradation temperature and low-
est weight loss (Fig. 9).
Dynamic mechanical analysis of all fiberboards made from corn
stalk biomass gave better results than the commercial product.
Incorporation of cellulose nano reinforcement produced a superior
complex modulus [130,131] and the stiffness decreased with
increasing temperature. Both commercial and fibreboards showed
decrease of rigidity with temperature, constantly, however nano
fibre reinforced fibreboards behaved differently.
Between the temperature 60–70 °C, low molecular weights
compounds and lignin start softening and mobility increased due
to this the stiffness of fibreboard were reduced. After 100 °C, com-
plex modulus seems to stabilize and the slope decrease is very low
512 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516

Fig. 7. DSC curves of raw materials and fibreboard at different temperatures [107] (with permission).

Fig. 8. Dynamic mechanical analysis of corn fiberboard [132] (with permission).

Fig. 9. Some application from lignocellulosic materials (Source: https://ecofiberboard.wordpress.com/2013/11/12/the-story-of-oil-palm-mdf/).

due to the small stiffening in some formulation, may be caused by 7.4. Hygro-thermal properties of binderless fibreboards
the evaporation of hydroxyl group from the board that stops the
loss of rigidity of fiberboards [133]. The complex modulus clearly In building construction, the inner air quality is serious concern
diminished above190°C and the material began degradation [130]. for the life cycle of the structure. Higher moisture level or humidity
 M. Nasir et al. / Construction and Building Materials 211 (2019) 502–516
can be risky for the building’s energy performance such as mould
growth, and loss of the insulation properties of insulate on materials
[134]. For the environmental quality consideration, hygrothermal
study is good way to improve materials with low environmental
impact and high moisture-buffering capacity. The moisture buffer
capacity is the capacity of adsorbing and desorbing moisture of
materials which can be used for heating and cooling by decreasing
the ventilation rate and improving indoor air quality [135,136].
Literature of hygrothermal properties on different materials
have been found. The moisture diffusion was characterized by
using vapor permeability or vapor diffusion resistance factor [137].
The isothermal vapor sorption is also a technique to evaluate
hygrothermal properties, the equilibrium moisture content or accu-
mulated moisture in material is related with the ambient relative
humidity which determined by the sorption curve of adsorbed water
vapor or desorbed under different levels of relative humidity [138].
The thermal conductivity (k-value) is also evaluate the
hygrothermal properties of insulation materials. By using low
thermal-conductivity materials, energy used for space heating
and cooling can be decreased. Density, porosity, moisture content
and temperature of insulation materials effect the k-value and
higher temperature show higher k-values at higher density mate-
rials and moisture content [139,140].
7.4.1. Mechanical and thermal properties
The insulating materials were developed by using lignocellulose
materials, found that water vapour permeability and accumulation
of moisture in lignocellulose materials were absorb from air [141].
The lignocellulosic materials have capacity of absorbing moisture
content in pores when the humidity increased and in dry condition
the pores release moisture gradually into the surroundings with
decreasing air humidity [142]. This process maintained the air
humidity in close area, in prolonged periods of winter may experi-
ence low air humidity.
Hydrothermal pretreated of Eucalyptus wood fibres were used
in making binderless board and study the mechanical strength
and mechanism of self-bonding [143]. The hydrothermal pre-
treated binderless fibreboard revealed high number of hydrogen
bond intensity, total crystallinity index and limiting oxygen index
than without hydrothermal pretreated binderless fibreboard. Cel-
lulose of Eucalyptus wood have high ordered crystalline structure,
higher crystallinity of cellulose increases provides a great stability
to the cellulose chains and protects them against acid attack during
hydrolysis [144]. However, the pretreatment partially break the
inter- and intra-bonding of hydrogen [145]. Hydrothermal treat-
ment of blended soft and hardwood of different maturities with
krafted lignin manufactured binderless fibreboard was studied
the effect of heterogeneous water and temperature distribution
in the sample thickness and avoid degradation mechanisms the
process temperature at 200 °C [12]. Another studied based on time
variation of the glass transition thickness gradient compared to the
time variation of the temperature gradient. The fibers are at a rub-
bery state during a limited period that depends on the position
within the sample thickness: the period is shorter near the side
where water vapor is evacuated, due to lower water content at this
location within the thickness [12].
8. Application
The reviewed literature mainly focused on the different type of
agro-waste fibres to utilize as construction materials. The litera-
ture based on physical, mechanical and thermal properties of these
binderless fibreboards materials signify huge variation in the
behavior. An international benchmarking can further be done for
better application of these innovative construction materials
513
[146]. Binderless fibreboards work as bridge of structural boards
and non-structural boards, these boards are very light in weight
due to lower density and no emission of any kind of harmful chem-
icals it makes it very suitable material for indoor applications.
There are many applications such as partition wall, false ceiling
and base of decorative items. Machining operation is easy on
binderless fibreboards and it reduce energy consumption which
makes it cheaper. These fibreboards are very flexible to use in fur-
niture such as table top, shoes rack and other light duty application
machining process. The demonstrative model houses can be
designed and developed over the specific study area to evaluate
the environmental performance. Water absorption and thickness
swelling are the great concern and it needs further study and
improvement.
9. Conclusion
In binderless fibreboards, various type of agricultural residue
and its bioproducts from agro-industries were utilized that have
potential for solid wood replacement due to the good amount of
hemicellulose and lignin though the dimensional stability is a chal-
lenge for such boards. Large molecules of lignin are hydrophobic in
nature it resists water penetration, thus it reduces the water
absorption and thickness swelling of fiberboards which passed
the minimum required strength but not good enough to with stand
in water resistant test. For the improvement in mechanical and
physical properties, pretreatment is used to expose the lignin
and hemicellulose onto the surface of cellulosic fiber which partic-
ipate in reaction during hot pressing. During manufacturing pro-
cess some variation such as particle size, pressing temperature
and time affect the mechanical and physical properties, signifi-
cantly. Pressing temperature between 200 and 220 °C is considered
optimum temperature for physical and mechanical properties of
binderless fibreboards, though, WA and minimum requirement of
MOR could not reach up to Japanese standard. The thermal proper-
ties revealed that in range of 230–475 °C fibre boards revealed sig-
nificant mass losses which indicated the pyrolysis of the raw
materials and also indicated the dependency of thermal stability
on the pressing temperature but still there is no concrete result
that can replace the adhesive bonded boards. There were limited
works reported on hygrothermal studies of binderless fibreboards,
the hygrothermal property is needed to be studied thoroughly.
Some factors create obstacle in the fully commercialization of
self-bonding mechanism of binderless fiberboards such as dimen-
sional stability and effect of moisture content on internal bonding.
An integrated approach of binderless fiberboards fabrication
should be investigated, involving enzyme-mediated approach dur-
ing pretreatment such as steam injection/explosion and chemical
oxidation.
Conflict of interest
The authors declare no conflict of interest.
Acknowledgement
The authors are thankful to Banda University of agriculture and
technology (BUAT), Banda, India and Ministry of Higher Education,
Malaysia for providing HICOE Grant No: 6369109 to INTROP,
Universiti Putra Malaysia (UPM), Malaysia to support this research.
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