Composites: Part B 45 (2013) 858–863

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Composites: Part B
journal homepage: www.elsevier.com/locate/compositesb

Effect of using walnut/almond shells on the physical, mechanical

properties and formaldehyde emission of particleboard
Hamidreza Pirayesh a,⇑, Hossein Khanjanzadeh b, Ayoub Salari b
a
Department of Wood and Paper Science & Technology, Faculty of Natural Resources, University of Tehran, P.O. Box 31585-4314, Karaj, Iran
b
Department of Wood and Paper Technology, Gorgan University of Agricultural Sciences & Natural Resources (GUASNR), Gorgan, Iran

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

Article history: In this study, the suitability of walnut/almond shells as renewable underutilized agricultural wastes for
Received 19 March 2012 wood based panel manufacturing was investigated. Particleboards containing different walnut/almond
Received in revised form 26 April 2012 shells particle ratios (0%, 10%, 20%, 30% and 100%) were made using urea–formaldehyde (UF) resin. Some
Accepted 4 May 2012
mechanical (modulus of elasticity, modulus of rupture and internal bond strength), physical (thickness
Available online 15 May 2012
swelling and water absorption) properties and formaldehyde emission of the particleboards were evalu-
ated. The addition of walnut/almond particle significantly improved water resistance of the panels and
Keywords:
greatly reduced their formaldehyde emissions. However, flexural properties and internal bond strength
A. Wood
B. Physical properties
decreased with increasing walnut/almond shells content in the panels. The walnut/almond shells can
E. Thermosetting resin be considered as an alternative raw material or filler in the manufacture of wood based particleboards
B. Mechanical properties used in indoor environment due to lower thickness swelling, water absorption and formaldehyde emis-
sion. Besides, using these underutilized materials in forest industry could decrease the pressure on forest
resources and some job opportunities can be created.
Ó 2012 Elsevier Ltd. All rights reserved.

1. Introduction
The social and economical developments of human beings are
depending on better utilization of available resources [14]. Forests,
the major sources of wood supply are declining at the alarming
rate of 13.0 million ha each year in developing countries [10].
The demand for composite wood products such as particleboard,
plywood, medium density fiberboard, hardboard and veneer prod-
ucts has recently increased distinguishably throughout the world
[7,34]. Environmental pressure managed to prohibit forest harvest-
ing; as a consequence, wood shortage-shut down of wood indus-
tries, unemployment, and etc. can be seen in some countries
including Iran. For instance, after closure of largest plywood plants
in Germany and France [39]; Iran’s plywood plants discontinued
their production either. Bio-based composites will become materi-
als to replace polymer based composites and wood in terms of
their attractive specific properties, lower cost, simple process tech-
nologies, eco-friendliness, and recyclability [7,14].
Iran as a developing country does not have sufficient raw mate-
rial to supply its forest industry demands. Consequently, several
researchers in Iran have investigated the suitability of some under-
utilized species as well as bio-based residues; date palm, mesquite,
salt cedar and eucalyptus wood [7], canola straw [6], almond shell
⇑ Corresponding author. Tel./fax: +98 2612220686.
E-mail address: h_pirayesh30@yahoo.com (H. Pirayesh).
[10], wheat straw [9] and walnut shell [32] in the production of
wood-based composites.
Walnut (Juglans regia L.) is an important crop that is cultivated
throughout the world’s temperate regions for its edible nuts [37].
Worldwide walnut production was approximately 2.2 million tons
from a total of 834 thousand ha in 2009 [17]. Walnut shell, an agri-
cultural waste, is the lingocellulosic material forming the thin
endocarp or husk of the walnut tree fruit. Farmers harvest grains
and burn or otherwise dispose the residues (shell, husk, stalks,
etc.).
Almonds are a very important crop throughout the world’s tem-
perate regions [29]. Worldwide almond production in 2009 was
about 2.31 million tons from a total of 1.7 million hectares [17]. Al-
mond (Prunus amygdalus L.) shell, a agricultural residue, is the
lingocellolusic material forming the thick endocarp or husk of
the almond tree fruit that upon processing the fruit to obtain the
edible seeds, is separated and since they have no important indus-
trial usages are normally incinerated or dumped [28]. Burning agri-
cultural residues causes environmental problems such as air
pollution, soil erosion and decreasing soil biological activity [24].
Utilizing agricultural residues not only prevents environmental
concerns but also can mean farmers second income from planta-
tion [9,27].
Urea formaldehyde resin is the most important type of adhesive
for manufacturing wood based composites [33]. Low price, good
technological properties, absence of colors in cured polymer and

1359-8368/$ - see front matter Ó 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.compositesb.2012.05.008
 H. Pirayesh et al. / Composites: Part B 45 (2013) 858–863 859

easiness of application for a variety of curing conditions are of Table 2

advantages of urea formaldehyde, while, formaldehyde emission Experimental design.

and poor water resistance are its main disadvantages [40,42]. With Board typea Raw material
rising economic standards, concerns about human health and the Walnut/almond shells (%) Wood (%)
environment have been raised due to the increasing demand for
A 0 100
wood based panels [34]. Formaldehyde (HCOH) is a suspected hu- B 10 90
man carcinogen that is known to be released from pressed-wood C 20 80
products used in home construction, including products made with D 30 70
urea–formaldehyde (UF) resins [36]. Formaldehyde has also been E 100 0
F 100 0
found to produce nasal carcinomas in mice and rats after exposure
to 14.1 and 5.6 ppm of formaldehyde, respectively, over a long per- Panel type E included 100% almond shell.
iod of time [36]. Formaldehyde emission from panels in service is Panel type F included 100% walnut shell.
a
The density of the boards made from walnut/almond shells and wood chips was
caused by residual formaldehyde present in the UF bonded panels
0.70 g/cm3.
trapped as gas in the structure and formaldehyde dissolved in the
water in the boards [2,33].
Iran with a walnut and almond production of 150,000 and
Table 3
110,000 tons respectively ranks as the world’s third biggest pro-
Production parameters of particleboards.
ducer of these crops [10,32]. Walnut shell comprises 67% of the to-
tal weight of the fruit [15], hence, around 1.5 million tons of Parameter Value
walnut shell is left behind each year. Furthermore, almond shell ac- Press temperature (°C) 180
counts for 35% to 75% of the total fruit weight [30], consequently, Pressing time (min) 5
Peak pressure (kg/mm2) 25
around 0.8 to 1.7 million tons of almond shell is left. Due to their
Thickness (mm) 16
similarities and closeness in light of nature, chemical composition Dimensions (mm) 420  420
and physical structure, combination of these materials could pro- 33% NH4Cl content (%) 1
vide considerable amount of wastes. Walnut/almond shells, as Outer layer (whole of board%) 35
bio-wastes, have no economical value or industrial usages in Iran Middle layer (whole of board%) 65
Number of boards for each type 3
and generally are discarded or burned in the stove in the winter.
Value-added wood-based panels made from these agricultural
wastes can be considered as optimum way of utilizing available re-
sources. Walnut/almond shells could play an important role in the wood particles were classified in laboratory shaker. Particles that
manufacture of value-added wood-based panels such as particle- remained between 3–1.5 mm sieve and 1.5–0.8 mm sieve were uti-
boards and may be more efficient use of these materials. There is lized in the core and outer layers, respectively. Particles were oven
no information on using walnut/almond shell particles in particle- dried at 100 ± 3 °C to reach the target moisture content (3%). Urea
board manufacturing; especially no information is available on formaldehyde (UF) resin at 9% and 11% levels (based on oven dry
formaldehyde emission of these materials as information on this weight of the particles) was used for the core and outer layers
property is of high value for industrialization of this kinds of respectively. One-percent ammonium chloride (NH4Cl) was also
products. Therefore, the aim of this study was to investigate some added to the resin as a hardener. Particleboard panels were manu-
physical, mechanical properties and formaldehyde emission of factured using standardized procedures that simulated industrial
particleboard containing particles of walnut/almond shells in production at the laboratory. The particles were placed in a drum
production of three-layer particleboard as a supplement and to blender and sprayed with urea formaldehyde and ammonium
alleviate the shortage of raw material in forest industry. chloride for 5 min to obtain a homogenized mixture. The shelling
ratio was 35%. The glued particles then were pressed into panel
2. Material and methods mat using a laboratory scale hydraulic hot press. Thickness of
panels was controlled by stop bars and panels target density was
The raw material of this study consisted of walnut (Juglans regia 0.7 g/cm3. Three panels were produced for each group. The exper-
L.) shell and almond (Prunus amygdalus L.) shell which collected imental design is shown in Table 2. The dimensions of the pro-
from the field right after walnut and almond harvest in Sfejir and duced particleboards were 42  42  1.6 cm. The produced
Faroj, Iran, respectively and wood particles (a 60:40 blend) consist- particleboards conditioned at 20 °C and 65% relative humidity to
ing of hornbeam (Carpinus betulus L.) and beech (Fagus orientalis L.) reach moisture content of about 12% before trimming to final
species were obtained from a particleboard plant in Gorgan, Iran. dimension of 40  40  1.6 cm. The panel production parameters
The adhesive was urea–formaldehyde (UF) which produced by a were also displayed in Table 3.
local plant with characteristics given in Table 1. Some mechanical properties; modulus of rupture (MOR) [18],
Walnut/almond shells were first cleaned of dirt and impurities, modulus of elasticity (MOE) [18] and internal bond strength (IB)
and then chipped by a knife ring flaker. Next the chipped shells and [20] and physical properties; thickness swelling (TS) and water
absorption (WA) [19] were determined for the produced particle-
boards. The average of 10 and 20 measurements were reported
Table 1 for mechanical and physical properties respectively. The formalde-
Properties of the UF adhesive. hyde emission of the samples was measured according to the EN
Properties UFa 717-3 standard [5]. Six sheets of test pieces (with dimensions of
Solid (%) 63
16  25  25 mm) were clamped 40 mm above water level using
Density (g/cm3) 1.273 a plastic support in a 500-ml polyethylene bottle containing
pH 7.6 50 ml of distilled water. The flask containing the specimens was
Viscosity (cps) 64 loaded in the oven at 40 °C for 180 min. Formaldehyde released
Free formaldehyde (%) 0.15
from the specimens was absorbed by the distilled water, which
Gel point (100 °C) 55
was subsequently used as the sample solution. The formaldehyde
a
Urea–formaldehyde. concentration in the sample solution was determined using
860 H. Pirayesh et al. / Composites: Part B 45 (2013) 858–863

acetylacetone–ammonium acetate solution and the acetylacetone

method, with colorimetric detection at 412 nm. The data obtained
was statistically analyzed using analysis of variance (ANOVA) be-
sides, Duncan’s grouping was included.

3. Result and discussion

3.1. Mechanical properties

Figs. 1 and 2 show the results of mechanical properties of pro-

duced panels. The highest MOR (16 MPa) and MOE (2327 MPa) val-
ues were measured for particleboard produced using industrial
wood particles. Besides, the lowest MOR (6.63 MPa) and MOE
(1208.9 MPa) values were determined for panels type F, including
100% walnut shell. The result indicated that the increasing walnut/
almond shells content in the mixture significantly decreased the Fig. 3. Average values of WA for 2 h and 24 h immersion in water.
MOR and MOE values of the particleboards. Significant differences
between groups were determined individually for these tests by
Duncan’s multiple comparison tests. The results of Duncan’s
grouping are shown in Figs. 1–4 and 6 by letters. All panel types
showed statistically meaningful differences (P < 0.01) in their
MOR and MOE properties from each other. Depending on the
amount of walnut/almond shells particle in the particleboards,
average decreases in MOR values varied from 6.9% to 58.6% as com-
pared to average of the panel type A (Fig. 5). MOE values showed
similar trends to result of the MOR. The average MOE values of
the particleboard with walnut/almond shells particles decreased
from 2% to 48% as compared to values of the panels made from
100% wood particles (Fig. 5). Addition of walnut/almond shells
particle in particleboards had more adverse effect on MOR than
MOE values. Panel types A, B, C and D satisfied the minimum
MOR requirements for general purpose use and interior fitments

Fig. 4. Average values of TS for 2 h and 24 h immersion in water.

Type of particleboards
B C D E F
0
Percent decrease of values (%)

-10

-20

-30

-40

-50

-60
Fig. 1. Average values of MOR and MOE of experimental panels.
-70

-80

MOE MOR IB WA2

WA24 TS2 TS24

Fig. 5. Percent decrease in average values of physical and mechanical properties of

the panel types.

including furniture manufacture required in the EN Standard

Fig. 2. Average values of IB of experimental panels.
[21]. Average MOE values of the panel types met the minimum
requirements for general purpose use and interior fitments includ-
ing furniture manufacture required in the EN Standard except for
panel types F and E.
IB values of the experimental panels ranged from 0.26 to
0.57 MPa. The highest IB value was observed for panel A while the
lowest was recorded for F type panel. IB values decreased with the
 H. Pirayesh et al. / Composites: Part B 45 (2013) 858–863
increasing the walnut/almond shells particle content in the panels.
The average decreases of IB value with incorporation of walnut shell
were 7.8% to 54.4% as compared to values of the panels made using
100% industrial wood particles (Fig. 5). All panel types showed sta-
tistically significant differences (P < 0.01) in IB values with each
other. IB values ranged from 0.43 to 0.70 MPa. The minimal require-
ment of internal bond strength for general purpose, interior fit-
ments and for load-bearing boards are 0.24, 0.35 and 0.50 MPa,
respectively [21]. All of the produced panels met requirement for
general purpose end-use while A, B, C, D and F type particleboards
met the minimum requirement for interior fitments including furni-
ture manufacture stated in the EN 312 standard. The properties and
the performance of the wood-based panels are determined by three
main parameters: (1) the wood, especially the wood surface, includ-
ing the interface between the wood surface and the bond line; (2)
the adhesive; (3) the working conditions and process parameters
[2]. Besides, the lower mechanical properties of panels containing
different walnut/almond shell particles can be attributed to lower
compactness of walnut and almond shell particles compared to
wood particles [10]. Walnut shell has much higher lignin and
extractives contents and much lower cellulose as well as hollocellu-
lose contents than its wood [2,14,25]. Similarlly, almond shell has
higher extractives content and lower cellulose as well as hollocellu-
lose contents than its wood [10]. High lignin content increases the
brittleness of the lignocellulosic material, whereas, high cellulose
content decreases its brittleness [13], besides, cellulose and hemi-
celluloses (hollocellulose) contain a large number of polar hydroxyl
groups [25]. The polar hydroxyl groups are predominantly respon-
sible for hydrogen bonds with polar adhesive polymers [27]. One
of the factors determining amount of adhesive bonds is surface wet-
tability [14]. The hydrogen bonding interactions have a determina-
tive role in surface wettability and absorption of the resin on the
lignocellulosics surface [10]. There is a positive relationship
between wood wettability and adhesion [26], hence, the lower
mechanical properties of panels containing different ratios of wal-
nut/almond shell particles can be also due to lack of good adhesion
between wood and walnut and almond shell particles as a result of
poor wettability of the latter’s. Besides, water-soluble extractives,
which their amounts in walnut and almond shells are high, have sig-
nificant effect on the UF resin gel time which is important in deter-
mination of the adhesion [25]. Extractives can have adverse effects
on the curing of adhesives, leading to poor particle–particle bond
strength and may cause blows and severely deteriorating the inter-
nal bond strength [2,27]. Furthermore, walnut and almond shells
contain high amounts of ash [10,32] which can result in weak bond-
ing between particles as well as very low internal bonding strength
within panels [9,16]. MDI is believed to work well with agricultural
residues because it is capable in particular of overcoming the prob-
lems associated with the waxy coatings prevalent on the tissues of
many materials [12]. Using MDI adhesive, particleboards water
absorption and thickness swelling decreased 60–75% compared to
those bonded with UF but the cost of the former adhesive is about
7–10 times higher than the latter [38]. As a result, mechanical prop-
erty of particleboards made from agricultural wastes can be im-
proved by additional treatments; chemical modification of the
particle [14,42], biological treatments of anaerobic digestion (AD)
[38], using MDI resin instead of UF [8], surface coating of the end
product [35] and using nanoparticles to improve the mechanical
properties of bio-based composites [40,41]. Similar results have
been reported for panels made using underutilized raw material
as well as agricultural wastes and residues [7,9,13,23–25,27].
3.2. Physical properties
The results of ANOVA and Duncan’s mean separation test
for WA and TS of particleboards made using the mixture of
861
walnut/almond shell particles and wood chips for 2 and 24 h water
immersion times are given in Figs. 3 and 4. With increasing the
walnut/almond shells particle usage in the particleboards, the TS
and WA values decreased. Based on EN standards, particleboard
should have a maximum TS value of 8% for 2 h water immersion.
Furthermore, according to EN 312-4 the maximum TS requirement
for 24 h water immersion is 15%. Wood contains numerous free –
OH groups present in the cellulosic cell wall materials, which are
responsible for interaction with water molecules by hydrogen
bonding. The water uptake of lignocellolusics can be mainly as-
cribed to hydrogen bonding of water molecules to the free hydro-
xyl groups presented in cellulose and hemicelluloses [11,22]. There
are three main regions where the adsorbed water in the composite
can reside: the cell wall, the lumen (via porous tubular), and the
voids between lignocellulosic material and resin in the case of
weak interface adhesion [1]. The holocellulose contain hydroxyl
groups and have hydrophilic characteristics that can absorb water
but lignin is totally amorphous and hydrophobic and do not absorb
water [11]. Extractives are comprised of tannins, pectins, fats,
waxes, gums, essential oils and volatile materials, and these mate-
rials cannot absorb water [22]. Extractives may act similar to wax
which is normally used to control water absorption and they could
results in a significant decrease in the degree of moisture absorp-
tion of the composite [1,32]. Decreasing water absorption by
increasing walnut/almond shells may be attributed to the presence
of more extractives and lower content of holocellulose in these
materials than its wood as discussed above. The positive role of
extractives on the water resistance has been mentioned by several
researchers [2,25,27]. The average TS and WA values of all panel
types showed significant difference (P < 0.01) from each other in
TS and WA after 2 and 24 h water immersion times. TS values of
all particleboard was found to comply with particleboard maxi-
mum property requirement of 14% for 24 h water immersion based
on EN 312 [21] for use in non load-bearing applications in humid
conditions except for panel types A (made with 100% wood parti-
cles) and B.
3.3. Formaldehyde emission
The addition of walnut/almond shells into particleboard signif-
icantly decreased formaldehyde emission value (Fig. 6). Depending
on addition of walnut/almond shells in the panels, the formalde-
hyde emission values ranged from 5.7% to 42.8% lower than the
panels made with 100% wood particles. The minimum value of
formaldehyde gas emission was measured for panels made with
100% walnut shell. In exact word, panel type F had the lowest
formaldehyde emission value with 4.9 mg/100 g (42.8% less than
panel type A) followed by panel type E (36.3%), panel type D
(16.3%), panel type C (13.2%), panel type B (5.7%) and finally panel
Fig. 6. Percent decrease in average value of formaldehyde emission of the panel
types.
862 H. Pirayesh et al. / Composites: Part B 45 (2013) 858–863
type A (10.2 mg/100 g) (Fig. 6). The results showed that the free-
formaldehyde emission values of the particleboard panel types (E
and F) for E1 class met the requirement of maximum 8 mg/100 g
[27]. The decrease in formaldehyde emission of the particleboard
panels with increasing walnut/almond shells can be attributed to
high amounts of extractives of the walnut and almond shells
[27]. The similar results were reported in previous studies [3,25].
They reported that decrease in formaldehyde emission values in
the panels may be due to the high amounts of polyphenolic extrac-
tives in bark, especially tannins. Alcohol-benzene solubility, 1%
NaOH solubility, Hot water solubility and cold water solubility of
walnut/almond shells are 3.2%, 35.2%, 10.2% and 7.6% respectively
[32]. Similarly, alcohol-benzene solubility, 1% NaOH solubility, Hot
water solubility and cold water solubility of almond shell are 2.8%,
30.2%, 9.1% and 6.3% respectively [10]. Hot-water procedure re-
moves a part of extraneous components, such as inorganic com-
pounds, tannins, gums, sugars, starches and fatty derivates [1].
Nemli and Colakoglu [4] found that incorporation of mimosa bark
particle greatly reduces formaldehyde emission of particleboards.
Post-treatment methods to decrease and minimize formaldehyde
release are based on compounds like ammonia, ammonium salts,
or urea [34]. Another effective way to reduce formaldehyde release
is the addition of formaldehyde-binding substances (‘‘scavengers’’)
to the resin or to the wood particles [27]. Ammonium chloride acts
as an acid catalyst of the curing reaction and as a formaldehyde
scavenger [34]. Coating panels’ surfaces with decorative overlays
are to eliminate the release of formaldehyde [31]. The environmen-
tally friendly tannin–formaldehyde resins are among the cheapest
binders and cause low-formaldehyde emission [25]. Besides, pro-
cessing condition of wood based panels have important role on
respective formaldehyde emission so that the higher the press cy-
cle time the lower the formaldehyde emission at service [33]. It is
to be noted that using nanoparticles such as nano-Sio2 and nano-
clay due to their strong absorbability and high barrier property
(shielding effect) as formaldehyde catchers is going to gain much
attention [40,41].
4. Conclusions
This study revealed that value-added particleboard panels con-
taining walnut/almond shells were not only environmentally
friendly but also an alternative solution for decreasing availability
of raw material in developing countries including Iran. Addition of
walnut/almond shells into particleboard panel significantly re-
duced their formaldehyde emission. Besides, incorporation of wal-
nut/almond shell particles highly improved water resistance of the
panels, however, the mechanical properties decreased with
increasing the content of these materials in the panels. Using agri-
cultural wastes like walnut/almond shells as raw material or filler
in manufacturing particleboards could contribute solution of raw
material shortage for particleboard industry as well as diminishing
environmental problems regarding their burning. Furthermore,
using these materials in particleboard manufacturing could mean
the farmers second income from plantation. Decreasing formalde-
hyde emission from particleboard containing walnut/almond shell
particles is considerable for furniture materials used in the indoor
environment. We recommend walnut/almond shells as alternative
raw material or filler in manufacturing particleboards used in in-
door environment due to lower thickness swelling, water absorp-
tion and formaldehyde emission.
Acknowledgments
The authors are grateful to the anonymous reviewers who pro-
vided useful comments to improve the clarity of the manuscript.
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