Composites Part C: Open Access 12 (2023) 100383

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Composites Part C: Open Access

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Comparative effects of different coastal weathering on the thermal,

physical, and mechanical properties of rubberwood–latex sludge flour
reinforced with polypropylene hybrid composites
Chainarong Srivabut a, Sriwan Khamtree b, Chatree Homkhiew c, *, Thanate Ratanawilai d,
Surasit Rawangwong c
a
Department of Industrial Engineering, Faculty of Engineering, Rajamangala University of Technology Srivijaya, Muang District, Songkhla, 90000, Thailand
b
Department of Industrial Technology, Faculty of Industrial Technology, Songkhla Rajabhat University, Muang District, Songkhla, 90000, Thailand
c
Materials Processing Technology Research Unit, Department of Industrial Engineering, Faculty of Engineering, Rajamangala University of Technology Srivijaya, Muang
District, Songkhla, 90000, Thailand
d
Department of Industrial and Manufacturing Engineering, Faculty of Engineering, Prince of Songkla University, Hat Yai, Songkhla, 90112, Thailand

A R T I C L E I N F O A B S T R A C T

Keywords: The influence of coastal weathering in tropical countries is a concern in terms of applications of wood-plastic
Wood-plastic composites composites (WPCs). Therefore, developing the WPCs into hybrid composites for increasing the resistance to
Latex sludge waste the coastal climate needs further investigation. The current work studies the effects of different coastal climates
Polymer degradation
(Gulf of Thailand and Andaman Sea), exposure times, and latex sludge contents on the properties of rubberwood-
Natural weathering
Statistics
latex sludge flour reinforced with polypropylene hybrid composites. The hybrid composites were manufactured
with a twin-screw extruder for mixing and a compression molding machine for forming. The results revealed that
the hybrid composites weathered for 12 months significantly (α = 0.05) decreased the modulus of rupture,
modulus of elasticity, screw withdrawal strength, and hardness with a maximum reduction of 218.6%, 207.4%,
84.2%, and 11.4%, respectively. However, adding the latex sludge flour of about 25 wt% increased crystallinity
degree and thermal stability as compared with the WPCs filling 50 wt% rubberwood flour. The hybrid composites
weathered under the Andaman Sea exhibited less loss of all the mechanical properties than that weathered under
the Gulf of Thailand. It is therefore suggested that the hybrid composites added to the latex sludge waste have the
potential to be used to produce the engineering products that were applied under the coastal climates.

1. Introduction alternative materials and develop composites reinforcing with more

agents than one type, resulting in a positive hybrid effect. Hybrid
Wood-plastic composites (WPCs) are composite materials consisting polymer composites are materials made by combining two or more
of plastic as a matrix, wood as filler, and other additives [1,2]. WPCs can different types of reinforcements in a common matrix [9], which have
be used for decorative purposes and as building materials in outdoor been gaining popularity with each passing year resulting from envi­
paving and wall panels [3]. Moreover, composites could also be used in ronmental, economic, and societal [2]. Moreover, hybrid composites are
doors, windows, furniture, deck floors, fences, and automotive in­ widely used in engineering, medical, defense, and other industries [10].
dustries [4,5]. The manufacturing sector of WPCs has grown rapidly in However, there are studies on the fillers of hybrid composites to improve
recent years. North America and China are the two largest producers, their properties. For example, Narupai et al. [11] studied the effect of
Europe being the third [6]. Especially, the global market of reinforcing with silica and carbon black hybrid filler of natural rubber
bio-composites is expected to reach an estimated $9.5 billion by 2027 (NR) composites. The results found that the physical and mechanical
[7]. Consequently, natural fiber-reinforced polymer composites have properties of NR composites can be improved by using silica and carbon
demonstrated great potential for many different applications in various black hybrid filler. Hayajneh et al. [12] studied the natural waste fillers
industries [8]. Previously, researchers attempted to find eco-friendly including lemon leaves and eggshells of the composites with

* Corresponding author.
E-mail address: chatree.h@rmutsv.ac.th (C. Homkhiew).

https://doi.org/10.1016/j.jcomc.2023.100383

Available online 14 July 2023

2666-6820/© 2023 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
C. Srivabut et al. Composites Part C: Open Access 12 (2023) 100383

polypropylene matrix. The results concluded that the eggshells com­ polystyrene and polypropylene (PP) are the best choices for applying
posites had the best values for both tensile and flexural tests while lemon wood-plastic composites which require resistance to high stresses and
leaves composites had the lowest values. Shahabaz et al. [13] studied natural weathering. In addition, the hybrid composites made from
the influence of nano-fillers (Al2O3 and SiC) in enhancing hybrid com­ thermoplastic matrix have shown improved mechanical properties [10].
posites. The results confirmed that adding nano-fillers produced supe­ Producing the material with a focus on improving aspects is very
rior tensile and hardness properties for carbon fiber-reinforced polymer important in various applications [26]. This work has been carried out
composites. Phunpeng et al. [14] studied hybrid composite materials on material waste reinforced plastic composites, wherein PP was chosen
which combined carbon fiber/epoxy with waste graphite fillers. The as matrix material.
results found that the hybrid composite materials provided higher Therefore, the novelty of this work aimed to enhance the perfor­
flexural strength and strength-to-weight ratio than the pure aluminum mance of the hybrid PP composites reinforced by the addition of rub­
alloy 6061. Moreover, there has been a growing interest in the use of berwood flour and latex sludge flour from concentrated latex processing
material waste which is considered reinforcing in the WPCs. Alternate and fresh latex ponds. Moreover, the comparison in degradation of the
materials or partial replacements should be developed by recycling hybrid composites under weathering conditions of different coastal cli­
waste materials. For example, Kaho et al. [15] valorized expanded mates between the Gulf of Thailand and the Andaman Sea in the South of
polystyrene (EPS) waste by developing composite materials from EPS Thailand was evaluated. Changes in surface color, thermal properties,
waste and wood waste. Mrowka et al. [16] investigated the impact of and mechanical properties were used as measures of the degradation in
wood waste (oak, hornbeam, beech, and spruce trees) on the mechanical the hybrid composites. The results obtained from this work are to in­
and biological properties of silicone-based composites. Basalp et al. [17] crease the efficiency of waste recycling and create more materials to be
studied the use of plastic and wood obtained from municipal bulky reused. Especially, hybrid material composites have the potential to be
waste for industrial manufacturing of WPC products. Nukala et al. [18] used to produce engineered products that have been tested for use in
developed the WPCs using recycled plastic waste generated from uni­ natural weathering conditions.
versity laboratories and recycled wood waste from construction. Hom­
khiew et al. [19] evaluated the potential of ground rubber tires and 2. Materials and methods
rubberwood sawdust waste for developing wood-polymer composites.
The results showed that the addition of wood waste enhanced the 2.1. Materials
modulus of elasticity, compressive modulus, and hardness of the com­
posites. In addition, the rubber industries generate a lot of sludge waste, The PP granules with the trade name 1100NK were obtained from
it is a by-product of the manufacturing process of concentrated natural IRPC Public Company Limited (Rayong, Thailand), and they had a melt
rubber latex [20]. The use of waste materials also reduces the problem of flow index (MFI) of 11 g/10 min at 230 ◦ C. Rubberwood flour (RWF)
land-filling, environmental, and health concerns [21]. Sludge waste is with 80-mesh size was acquired from Plan Creations Company Limited
incorporated to obtain a new composite material with reasonable me­ (Trang, Thailand). Sludge waste is a semi-solid slurry that is produced
chanical and physical properties as well as low cost. There are a few from processes of the rubber industries, including from the
studies related to sludge waste used as the reinforcement of WPCs and manufacturing process of fresh latex ponds and concentrated latex
other materials. Homkhiew et al. [22] evaluated and compared the processing. There were two latex sludge wastes from the different
potential of rubberwood flour and sludge waste as reinforcement in manufacturing processes of the fresh latex pond (FLSF) and concen­
recycled HDPE composites. It can be seen that the previous studies have trated latex processing (CLSF), which FLSF was from the sedimentation
focused on the effect of the reinforcing agents that enhanced the process at the bottom of the fresh latex pond and CLSF was from sludge
compatibility of the wood and polymer matrix resulting in improved passing through a centrifuge. They were collected from the rubber latex
properties of hybrid composites. Moreover, sludge waste has the po­ industry in Southern Thailand (Songkhla, Thailand). The FLSF mainly
tential to be a good filler. Therefore, the choice of wood waste and latex contains P2O5 (36.07 wt%) and MgO (20.43 wt%), while the CLSF is
sludge waste reinforcements in WPCs is proving to be a good alternative composed of 33.44 wt% of P2O5 and 18.21 wt% of MgO, and other
in this work. components are K2O, ZnO, CaO, SO3, SiO2, Al2O3, Fe2O3, and Rb [28].
WPCs are mainly used in outdoor applications for building and Before the hybrid composites mixing, these materials were oven dried at
construction purposes such as decking, siding, fencing, and cladding 110 ◦ C for 24 to reduce the moisture content except sludge waste was
[23]. The outdoor performance of WPCs is particularly concerned with dried in an oven at 120 ◦ C for 48 h. Further, the maleic anhydride
the resistance of coastal weathering in tropical countries. The rising sea grafted polypropylene (MAPP) with 8–10% of maleic anhydride (Mw =
levels, rising acidity of the sea, changing the intensity and frequency of 9100 and Mn = 3900) was used as a coupling agent. It was obtained from
storms, and warmer ocean temperatures of coastal weathering affected Sigma-Aldrich (Missouri, USA). The MAPP was used to enhance the
the properties of the WPCs [24]. In addition, natural weathering is interfacial bonding between the matrix and reinforcements in the
generally done to determine the durability of the material in natural composites.
conditions and common aspects of natural weathering including heat,
cold, moisture, sunlight, rain, and dew [5]. Fewer studies investigated 2.2. Composites processing
the effects of natural weathering on hybrid composites or other mate­
rials. For example, Wei et al. [25] examined changes in wood/polymer The formulation of the hybrid composites in the experiment is shown
composition, surface chemistry, and thermal properties of WPC decking in Table 1. Firstly, the PP granules, RWF, MAPP, and FLSF or CLSF were
with and without a co-extruded cap layer after 8–14 years of mixed using a co-rotating twin-screw extruder (Model CTE-D25L40 from
above-ground outdoor exposure at a sub-tropical site near Hilo, Hawaii. Chareon Tut Co., Ltd, Samutprakarn, Thailand). The barrel temperatures
Mohammed et al. [26] concluded that the tensile strength of the com­ ranged from 170 to 190 ◦ C were controlled from the feeding to die zone.
posites starts to decrease after the first weathering month through to the The screw speed is fixed at 50 rpm. The extruded compound was cooled
weathering periods with a constant reduction of tensile. At the end of the in air and then pelletized. After that, the hybrid composite pellets were
weathering period, almost 85% of the composite’s mechanical behavior placed in the compression molding. The plate mold was 200 mm × 250
is lost. Torun et al. [5] reported that the weathering exposure caused a mm and 4.8 mm in thickness. The temperature was fixed at 190 ◦ C under
slight decrease in the tensile and flexural strength of composites. a pressure of 6.89 MPa (1000 psi) for 15 min, followed by a water-
Moreover, the polymer band intensities decreased due to the degrada­ cooling system under pressure for 5 min. Three replicate plates were
tion, and the composites are in accordance with the surface roughness of produced for each hybrid composite formulation. Finally, the hybrid
composites after weathering. Ratanawilai et al. [27] reported that composite plates were cut according to the American Society for Testing

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Table 1 27″ N and longitude 99◦ 20′ 07′’E), as shown in Fig. 1. Southern Thailand
Formulation of the hybrid composites in the experiment. consists of two coastlines including the Gulf of Thailand on the east coast
Composite sample code Composition (wt%) and the Andaman Sea on the west coast. The Southwest monsoon is
occurred from May to October to cause lower pressure in China, while
PP RWF FLSF CLSF MAPP
the Northeast monsoon is caused by the high pressure from China be­
PP100 100 – – – – tween October-February. These two monsoons bring humid air from the
P46R50 46 50 – – 4
P46R25F25 46 25 25 – 4
seas and generate rainfall in Southern Thailand [29]. The average
P46R25C25 46 25 – 25 4 temperature in Songkhla and Trang Provinces ranged from 26.5 - 29.4
◦
C and 26.2–28.6 ◦ C, respectively, as well as the total rainfall value of
Notes; PP: Polypropylene; RWF: Rubberwood flour; FLSF: Latex sludge flour
1047 mm and 425 mm, respectively, as shown in Fig. 2. The weather
from fresh latex pond; CLSF: Latex sludge flour from concentrated latex pro­
cessing; MAPP: Maleic anhydride-grafted-polypropylene; wt%: Percent by
data for each month from July 2021 to June 2022 were collected from
weight. the Southern-East Coast Meteorological Center, Ministry of Digital
Economy and Society, Thailand.
and Materials (ASTM) standard for physical and mechanical tests.
2.4. Analytical techniques

2.3. Natural weathering testing

2.4.1. Thermal analysis
The thermogravimetric analysis of the hybrid composite samples was
Natural weathering tests under the coastal climate in the South of
employed by a Perkin Elmer (TGA-7, USA). The test was conducted in
Thailand were done according to the ASTM D1435 standard. The hybrid
the temperature range of 45 to 700 ◦ C at a heating rate of 10 ◦ C/min in a
composite samples were exposed to coastal weathering including the
nitrogen atmosphere. The continuous weight loss and temperature were
Gulf of Thailand and the Andaman Sea for a period of 12 months from
recorded and analyzed. Additionally, the hybrid composites were per­
July 2021-June 2022. The exposure consisted of the climatic conditions
formed using differential scanning calorimetry (DSC) analysis with
from the two annual seasons including the summer and rainy seasons in
Perkin Elmer (DSC-7, USA). The samples were heated from 20 to 500 ◦ C
the South of Thailand. The composite samples were attached to the
at the rate of 10 ◦ C/min. The percentage of crystallinity (χ c) from
aluminum racks at a 45◦ angle and placed on the roof of the Engineering
compounding between plastic matrix and filler wastes was calculated
Building at Rajamangala University of Technology Srivijava (Songkhla
from the DSC thermogram according to Eq. (1):
Province) with latitude 7◦ 12′ 3.1″ N and longitude 100◦ 36′ 4.7′’E) and
on the roof of the Engineering and Technology Building at Rajamangala
University of Technology Srivijava (Trang province) with latitude 7◦ 31′

Fig. 1. Locations of the test specimens being placed in different coastal weathering.

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1200 30
Songkhla Province Trang Province
Songkhla Province Trang Province
1000 29

Average Temperature (oC)

Rainfall Value (mm) 800 28

600 27

400 26

200 25

0 24
Jul-21 Aug-21 Sep-21 Oct-21 Nov-21 Dec-21 Jan-22 Feb-22 Mar-22 Apr-22 May-22 Jun-22

Fig. 2. Climate conditions during different coastal weathering testing showing rainfall values (solid lines) and average temperatures (dash lines).

ΔHm 100 not significant differences; difference superscripts indicate significant

χc = x (1)
ΔH0m W differences. All of the statistical analyses were performed at a 5% sig­
nificance level (α = 0.05).
where ΔHm is the enthalpy of fusion determined from DSC, ΔH0m is the
theoretical enthalpy of fusion of 100% crystalline plastic melting 148 J/ 2.5. Characterizations
g for PP [30,31], and W is the weight fraction of plastic in hybrid
composites. 2.5.1. Flexural test
The three-point flexural test was carried out using a Mechanical
2.4.2. Visual surface analysis Universal Testing Machine (Model NRI-TS500–50 from Narin Instru­
Changes on the sample surfaces of the composites were analyzed ment Co., Ltd., Samut Prakan, Thailand) at a crosshead speed of 2 mm/
before and after exposure under coastal climates of the Gulf of Thailand min with a span of 80 mm, according to the ASTM D790. The size of
and the Andaman Sea for 2, 6, and 12 months. The samples were samples was prepared following the standard about 13 × 100 × 4.8
observed using an optical microscope (Zeiss Axioskop, Oberkochen, mm3, which measured both un-weathered and weathered specimens
Germany). under coastal climates for 0, 2, 6, and 12 months. Data were collected
and used to calculate the MOR, MOE, and maximum flexural strain of
2.4.3. Colorimetric analysis the composites.
The color analysis of the hybrid composite samples was carried out
with a CHECK 3 portable spectrophotometer (Datacolor, USA). The 2.5.2. Screw withdrawal test
surfaces of samples were measured both before and after exposing the The composite samples for the screw withdrawal test were prepared
coastal climates of the Gulf of Thailand and the Andaman Sea. The color according to ASTM D1037 standard using the computer-controlled
was determined according to the CIE L* a* and b*color system. The L* Universal Testing Machine. The dimensions of the samples were
displays the lightness and varies from 100 (white) to 0 (gray); the approximately 50 × 50 × 4.8 mm3 (width × length × thickness). The
a*coordinate displays color components from red ( +a*) to green (-a*); wood screws with a diameter of 4.18 mm and threaded length of 50 mm
and the b* coordinate displays components from yellow ( +b*) to blue were applied, which have been driven through their face. The speed of
(-b*). There were three replications of each formulation and condition the loading crosshead was set at 1.5 mm/min for testing the specimens
for 0, 2, 6, and 12 months after weathering, and each sample was un-weathered and weathered for 2, 6, and 12 months.
measured at three locations. The color difference or discoloration (ΔE)
was calculated according to Eq. (2): 2.5.3. Hardness test
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅ The hardness measurement was performed on the un-weathered and
ΔE = ΔL2 + Δa2 + Δb2 (2)
weathered composite surfaces for 2, 6, and 12 months using a Shore D
where ΔL, Δa, and Δb represent the component differences between Durometer (Model GS-702 G from Teclock Corporation, Nagano, Japan),
before and after weathering, in respective coordinates of L*, a*, and b*. according to the ASTM D2240 standard. The composite samples were
prepared with approximate dimensions of 30 mm (length) × 30 mm
2.4.4. Statistical analysis (width) × 4.8 mm (thickness). All mechanical characterizations were
A student’s t-test was applied to detect significant differences be­ performed at ambient temperature (25 ◦ C) with five replications for
tween un-weathered and weathered (for 12 months) samples for each formulation and condition.
modulus of rupture (MOR), modulus of elasticity (MOE), screw with­
drawal strength (SWS), maximum flexural strain, and hardness of the 3. Results and discussion
composites. In addition, comparisons were also conducted within each
formulation exposed under the coastal climate between the Gulf of 3.1. Differential scanning calorimetry analysis
Thailand and the Andaman Sea. Superscript letters were used to denote
significance in tabulation; if the letters are the same, the means that are The DSC values of the hybrid composites reinforcing fillers at ratios
of 25 wt% RWF and 25 wt% FLSF or CLSF are presented in Table 2. The

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Table 2 3.2. Thermogravimetric analysis

Melting temperature, melting enthalpy, and crystallinity degree of the hybrid
composites after weathering. The TGA and DTG curves for rubberwood and latex sludge flour-
Sample Tm ( ◦ C) ΔHm (J/g) Crystallinity (%) reinforced polypropylene as the hybrid composites before and after
Peak I Peak II Peak I Peak II
coastal weathering are displayed in Fig. 3(a) and (b), respectively. The
study of the thermal stability of the hybrid composites was evaluated to
P46R50 165.5 465.8 41.86 242.04 61.48
analyze their future applications at high temperatures from the envi­
P46R50 (G) 149.3 447.8 88.79 268.70 130.42
P46R50 (A) 149.0 449.2 81.07 282.37 119.08 ronment including the weathering and melting from the extrusion and
P46R25F25 165.8 477.7 51.21 229.06 75.22 compression molding process [35,36]. It is well known that one of the
P46R25F25 (G) 150.5 449.2 95.17 320.31 139.79 limiting factors of the hybrid composites made from plastic and natural
P46R25F25 (A) 150.2 449.7 81.55 290.15 119.78 fillers as reinforcement was their low thermal stabilities. Thus, it is
P46R25C25 165.8 477.0 43.02 286.01 63.19
P46R25C25 (G) 149.5 451.0 95.10 327.75 139.68
necessary to evaluate their thermal stability for identifying filler types
P46R25C25 (A) 150.0 451.2 91.34 333.91 134.16 by comparing each condition [2,37]. However, the thermal stability
behavior of the hybrid composites is studied using TGA and DTG as
Notes; Tm is the melting temperature; ΔHm is the heat quantity obtained by DSC;
weight (%) values. According to the TGA curve (Fig. 3(a), the compos­
G: Gulf of Thailand; A: Andaman Sea.
ites reinforced with 50 wt% RWF both un-weathering and weathering
had higher weight loss in a temperature range of 100 to 700 ◦ C as
melting temperature (Tm), melting enthalpy (ΔHm), and crystallization
compared to those of the other composites. In addition, the hybrid
of the composites were measured before and after weathering under
composites produced from P46R25F25 and P46R25C25 had similar TGA
conditions of the Gulf of Thailand and the Andaman Sea for 12 months.
curves in a temperature range of 500 to 700 ◦ C, and the hybrid com­
Previous studies found that the use of reinforcing fillers into the com­
posites un-weathered displayed less thermal stability in the second stage
posites had a positive effect on thermal properties, but may decrease the
of the decomposition than that weathered under conditions of the Gulf
toughness and ductility of the filled plastic matrix [32,33]. The
of Thailand and the Andaman Sea, as shown in Fig. 3(a). This result
decomposition profiles of the hybrid composites are characterized by
explains that the coastal weathering under the Gulf of Thailand and the
two peaks in both the melting temperature and melting enthalpy. As can
Andaman Sea influenced the weight loss percentage of the hybrid
be seen from the melting temperature, the hybrid composites reinforced
composites, resulting in their more thermal stability in the second stage
with FLSF had higher melting temperatures than those of the RWF and
of the decomposition.
CLSF as fillers. The composites with 25 wt% FLSF (P46R25F25) indi­
The DTG curves of the hybrid composites with rubberwood and latex
cated values of 165.8 ◦ C for peak I and 477.7 ◦ C for peak II, which gave
sludge flour before and after coastal weathering are illustrated in Fig. 3
the highest melting temperature as compared to those of the other
(b). All of the DTG curves of the hybrid composites are characterized
samples. Further, the melting temperatures (165.8 ◦ C) in peak I of both
into three peaks in which the first peak is the decomposition of water or
P46R25F25 and P46R25C25 were similar to that of P46R50 (165.5 ◦ C).
oxygen components, while the second peak is the degradation behavior
Likewise, the results in peak II showed that the composites with 25 wt%
of the reinforcing filler, and the third peak is the decomposition tem­
FLSF (P46R25F25) had the highest melting temperature as compared to
perature of the plastic matrix [18,38]. As reported by Ratanawilai et al.
those of the other samples. This result is in agreement with Homkhiew
[39] revealed that the first stage corresponded to the release of moisture
et al. [28], who concluded that the composites made from FLSF as
content from materials and the second stage is the decomposition of
reinforcing filler had higher melting temperatures than the CLSF. These
components in the composites. The results indicated that, in the third
results could be explained that the FLSF is not combusted in the molding
peak, the hybrid composites with 25 wt% FLSF (P46R25F25) after
process including extrusion and hot-pressing processes, resulting in
weathering under the Gulf of Thailand showed the largest derivative
high-temperature resistance of such composites in thermal testing.
weight as compared with the other formulation and condition.
The melting enthalpy (ΔHm) was also presented to evaluate the
Compared to the hybrid composites weathered under different coastal
thermal performance of the hybrid composites, as indicated in Table 2.
weathering, the composites weathered under the Gulf of Thailand pre­
The endothermic peaks of the composites reinforced with rubberwood
sented a higher derivative weight than that under the Andaman Sea.
and latex sludge flour were characterized in the form of two peaks, as
same as the melting temperature. The composites made from
3.3. Color changes and cracked surface analysis
P46R25F25 under weathering of the Gulf of Thailand and P46R25C25
under the climate of the Andaman Sea had the highest melting enthalpy
The lightness (L*) and total color changes or discolorations (ΔE) of
values of 95.17 ◦ C (peak I) and 333.91 ◦ C (peak II) as compared to those
the hybrid composites are displayed in Fig. 4(a) and (b), respectively.
of the other samples. The thermal result of P46R25F25 was good in
The L* and ΔE values of the control sample (PP100) and those of the
terms of resisting the high temperature in DSC testing, in which melting
composites reinforced with RWF and latex sludge flour (both FLSF and
enthalpy can be observed from second peaks (peak II). Moreover, the
CLSF) un-weathered and weathered in different coastal weathering
melting enthalpy of both the first and second peaks reduced, but the
(Gulf of Thailand and Andaman Sea) for 2, 6, and 12 months are
crystallinity degree rose with an increase of FLSF and CLSF in the hybrid
investigated. Theoretically, the surfaces of the composites exposed to
composites. It is a good agreement with Srivabut et al. [34], who
the natural weathering observed changes in the form of color fading, in
concluded that the addition of filler contents into the WPCs resulted in
which the color changes in the L* values increased with the increment of
some decreases in the glass transition but increases the crystallization.
weathering exposure time in a similar way to the ΔE values [40]. The L*
After exposure to weathering of the Gulf of Thailand and the Andaman
and ΔE values are generally raised with an increase in the exposure time,
Sea, the addition of 25 wt% FLSF (P46R25F25) increased the crystal­
but the characteristics of surface color also depend on the reinforcing
linity degrees by about 139.73% and 119.78%, respectively, while 25 wt
filler contents [5,23,41]. This study revealed that the composite samples
% CLSF (P46R25C25) the crystallization degree increased about
rapidly increased the L* values in 2 months of exposure, except the
139.68% and 134.16%, respectively. Overall, the result suggests that the
control sample slightly increased. After that, all of the composite sam­
hybrid composites reinforced with 25 wt% FLSF effectively improved
ples insignificantly increased the L* values until 12 months of the coastal
the melting temperature, melting enthalpy, and crystallization, due to
exposure. This result is in agreement with Mohammed et al. [26], who
interface occurred and better compatibility between filler and plastic
concluded that natural weathering reduced some physical properties
matrix.
such as the color performance of composites, and more biodegradable
composites had less natural weathering resistance. Additionally, the

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Fig. 3. Curves of (a) TGA and (b) DTG for rubberwood-latex sludge flour reinforced with polypropylene hybrid composites before and after coastal weathering.

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Fig. 4. Effects of different coastal weathering on (a) lightness and (b) total color change of rubberwood-latex sludge flour reinforced with polypropylene
hybrid composites.

results showed that the L* and ΔE values of the composites samples weathered in different coastal weathering conditions for 2, 6, and 12
weathered for 2 months under the Gulf of Thailand were similar to those months are shown in Table 3. In general, the poor surface performance
of the Andaman Sea; however, after 6 months the hybrid composites of the composites is displayed by the presence of roughness and cracks
weathered under the Gulf of Thailand gave larger L* and ΔE than that on the surface [24]. As can be seen from the micrograph, the crack and
weathered under the Andaman Sea. The composition of P46R50 gave fracture were observed on the surfaces of the control sample and the
the lowest surface lightness under coastal weathering of the Andaman hybrid composites reinforced with RWF and latex sludge flour after
Sea, as displayed in Fig. 4(a). Further, the surface color change of exposure to the coastal climate. This study revealed that the fracture and
P46R50 was more pronounced at the initial stage, whereas that other crack on the surface increased with an increase in the exposure time, due
displayed a slight color change at the later stage of weathering exposure, to the increasing number of chain scissions. The polymer chain scission
which depends on the composition of the hybrid composites, as illus­ results in surface cracks and embrittlement of the plastic composites
trated in Fig. 4(b). It means that the composition types and content, [41]. The control sample had a higher fracture and crack on the surface
exposure times, and different coastal weathering conditions strongly than those of the hybrid composites weathered under the climate of the
affected the lightness and discolorations of the hybrid composites. Gulf of Thailand and the Andaman Sea. This is most likely due to the
The microscopy images of the composite surfaces un-weathered and brittleness of plastics when exposed to light during time of initial stage.

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Table 3
Optical microscopy images of the hybrid composite surfaces at different weathering stage.
Code Un-weathered Weathered for 2 months Weathered for 6 months Weathered for 12 months

PP100 (G)

PP100 (A)

P46R50 (G)

P46R50 (A)

P46R25F25 (G)

P46R25F25 (A)

P46R25C25 (G)

P46R25C25 (A)

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This result is in agreement with Wei et al. [25], who reported that weathering under the Gulf of Thailand and the Andaman Sea for 12
long-term outdoor weathering resulted in the poor surface in virgin months showed the highest MOE values of 1.30 GPa and 1.42 GPa,
plastic during time ranging from 1 to 2 months. Furthermore, the mi­ respectively. The highest loss in MOR and MOE values about 448% and
croscopy images showed that the hybrid composites, namely P46R50, 207.4% was determined for the control sample and the composites with
P46R25F50, and P46R25C50, gave similar fracture and crack on the 50 wt% RWF (P46R50), respectively, under the condition of the Gulf of
surfaces, whereas the surface of the hybrid composites displayed lower Thailand.
cracks than the control sample. The maximum flexural strain of the control sample and the hybrid
composites is also displayed in Table 4 and Fig. 6. The addition of the
3.4. Mechanical properties of the hybrid composites reinforcing fillers into the hybrid composites resulted in a lower flexural
strain than the control sample. This could be possible due to the elastic
3.4.1. Flexural properties deformation in which the atoms that moved and to the effects of stress
The flexural properties (MOR and MOE) of the control sample moved back to their original positions [9,44]. As can be seen in Table 4,
(PP100) and the hybrid composites reinforced with RWF and CLSF or the maximum flexural strain of 6.26% was determined in the control
FLSF un-weathered and weathered under different coastal weathering sample before coastal weathering, whereas after weathering for 12
(Gulf of Thailand and Andaman Sea) for 2, 6, and 12 months are dis­ months under the climate of the Gulf of Thailand and the Andaman Sea,
played in Table 4 and Fig. 5. The experimental results in different con­ it gave the flexural strain of 2.20% and 2.46%, respectively. Comparing
tents, coastal weathering conditions, and exposure times were analyzed the flexural strain in P46R50, P46R25F25, and P46R25C25, it is evident
to compare the performance of the composites. As can be seen in Table 4, that P46R25C25 had higher flexural strain than the P46R50 and
this study revealed that the compositions of the hybrid composites P46R25F25 in both of the coastal weathering. For example, the
significantly affected the flexural properties. Overall, the control sample maximum flexural strain of P46R25C25, P46R25F25, and P46R50
un-weathered had higher MOR values than those of the hybrid com­ weathered under the Gulf of Thailand for 12 months was 1.18%, 1.09%,
posites. The addition of RWF and latex sludge flour as reinforcement and 1.05%, respectively. All of the strain values in the hybrid composites
reduced the MOE values of the hybrid composite, as compared with the that were un-weathered were similar to those that were weathered, and
composites reinforced only RWF. It is a good agreement with Tian and they were lower compared to the control sample, as shown in Fig. 6. The
Xu [42], who concluded that the wood filler in composites brings a composites reinforcing with fillers either RWF or latex sludge waste gave
pronounced lower modulus. Further, comparing to P46R50, lower flexural strain as compared to the plastic matrix.
P46R25F25, and P46R25C25 un-exposed to the coastal weathering, the A two-sample t-test was applied to analyze the effects of different
MOR of the P46R50 (41.6 MPa) was the best tolerated, followed by coastal weathering conditions after weathering for 12 months of the
P46R25F25 (41.5 MPa) and P46R25C25 (38.1 MPa), respectively. This control sample and the hybrid composites, as shown in Table 4. This
result is in agreement with Srivabut et al. [34], who reported that rub­ study revealed that the coastal weathering conditions significantly (p <
berwood flour slightly increased the MOR in wood-plastic composites. 0.05) affected the flexural properties of the hybrid composites. For
For MOE values, the composites made from P46R50 had higher MOE example, in the formulation of the P46R25F25, the composites after
values than those of all the hybrid composites. The samples having the weathering under the Gulf of Thailand having 13.2 MPa (suffix a) had
composition of P46R50, P46R25F25, and P46R25C25 gave MOE values significantly lower MOR than that under the Andaman Sea with 14.5
of 3.40 GPa, 3.20 GPa, and 3.06 GPa, respectively. MPa (suffix b). Further, the two-sample t-test was also applied to analyze
In addition, the flexural properties decreased with coastal weath­ the effect of exposure time. The experimental results verified that the
ering exposure time for 2, 6, and 12 months, as displayed in Fig. 5. As flexural properties (both MOR and MOE) of the hybrid composites
expected, the degradation in MOR and MOE values of the hybrid com­ significantly (p < 0.05) reduced after weathering for 12 months. For
posites continually increased until 12 months, in which the MOR and example, in the formulation of the P46R25C25, the composites un-
MOE values slowly decreased in the initial period (2 months), and then weathered had a MOE of about 3.06 GPa (suffix A) which is a signifi­
they rapidly decreased until the 12 months. As reported by Rashdi et al. cantly higher MOE than that weathered under the Andaman Sea having
[43], it was concluded that the flexural properties slowly decreased in 1.42 GPa (suffix B).
the initial period until 2 months of the natural weathering. Further, the
hybrid composites (P46R25C25) gave the maximum MOR value as 3.4.2. Screw withdrawal property
compared to those of the other composites after weathering for 12 The screw withdrawal strength of the control sample and the hybrid
months. The MOR values of 14.3 MPa and 15.9 MPa were determined composites un-weathered and weathered in different coastal weathering
for the hybrid composites having 25 wt% CLSF after exposure to conditions (Gulf of Thailand and the Andaman Sea) for 2, 6, and 12
weathering of the Gulf of Thailand and the Andaman Sea, respectively. months is exhibited in Table 4 and Fig. 7. Generally, the aim of the screw
Moreover, the hybrid composites made from P46R25C25 after withdrawal test in the WPCs is to measure the maximum strength

Table 4
Effects of different coastal weathering on mechanical properties of the hybrid composites.
Condition MOR (MPa) MOE (GPa) Maximum strain (%) SWS (MPa) Hardness (Shore D)

0M 12 M % Loss 0M 12 M % Loss 0M 12 M % Loss 0M 12 M % Loss 0M 12 M % Loss

PP100 (G) 50.7 A 9.24 aB 448.5 1.72 A 0.62 aB 179.5 6.26 A

2.20 aB 184.0 54.9 A 17.0 aB 223.2 76.3 A 68.9 aB 10.6
PP100 (A) 50.7 A 9.82 aB 415.9 1.72 A 0.70 bB 145.9 6.26 A
2.46 aB 154.1 54.9 A 21.2 bB 159.5 76.3 A 70.2 bB 8.66
P46R50 (G) 41.6 A 13.1 aB 218.6 3.40 A 1.11 aB 207.4 1.55 A
1.05 aB 48.0 40.9 A 24.7 aB 65.4 78.7 A 71.4 aB 10.2
P46R50 (A) 41.6 A 15.5 bB 167.8 3.40 A 1.16 aB 193.4 1.55 A
1.16 bB 33.8 40.9 A 28.4 bB 43.9 78.7 A 73.7 bB 6.78
P46R25F25 (G) 41.5 A 13.2 aB 215.4 3.20 A 1.27 aB 151.7 1.57 A
1.09 aB 44.1 33.2 A 18.1 aB 84.2 80.1 A 71.9 aB 11.4
P46R25F25 (A) 41.5 A 14.5 bB 186.0 3.20 A 1.39 bB 130.4 1.57 A
1.15 aB 36.7 33.2 A 21.4 bB 55.1 80.1 A 72.2 aB 10.9
P46R25C25 (G) 38.1 A 14.3 aB 167.2 3.06 A 1.30 aB 135.3 1.59 A
1.18 aB 35.4 29.9 A 23.9 aB 25.1 78.0 A 72.2 aB 10.8
P46R25C25 (A) 38.1 A 15.9 bB 138.9 3.06 A 1.42 bB 115.8 1.59 A
1.25 aB 27.5 29.9 A 25.0 bB 19.9 78.0 A 73.0 bB 9.53

Notes: M: Month; G: Gulf of Thailand; A: Andaman sea; MOR: Modulus of rupture; MOE: Modulus of elasticity; SWS: Screw withdrawal strength; Means within each
column of each formulation at 12 M with the same superscripts a-b indicate a insignificant difference (α = 0.05) by the t-test. Different superscripts A-B of each property
and condition indicate significant difference (α = 0.05) between mechanical properties of the composites unweathered and weathered for 12 months;% loss was
calculated at 12 months of natural weathering.

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Fig. 5. Effects of different coastal weathering on (a) modulus of rupture and (b) modulus of elasticity of rubberwood-latex sludge flour reinforced with poly­
propylene hybrid composites.

required to pull a standard-size screw from the specimens, which de­ composites. The average screw withdrawal strength for the control
termines the useful service life in many applications, especially con­ samples was found value of 54.9 MPa. This could be possible due to the
struction and building [45,22]. The experimental results of this research thermoplastic matrix encapsulating the thread of the screw, allowing
used to evaluate the direct withdrawal of the screw for the hybrid continuous load transfer along the threaded length [46]. In addition, the
composites were a measure of the resistance of the samples under un-weathered WPCs (P46R50) having a value of 40.9 MPa had a higher
different coastal weathering conditions and exposure times. According screw withdrawal strength than the hybrid composites with 25 wt% of
to Table 4, this study revealed that the reinforcing filler types and both FLSF (P46R25F25) and CLSF (P46R25C25) having values of 33.2
contents significantly affected the screw withdrawal strength of the MPa and 29.9 MPa, respectively.
composites. It is evident that the addition of reinforcing filler reduced The screw withdrawal strength of the hybrid composites under
performance in the screw withdrawal strength of the composites. This different coastal weathering conditions (Gulf of Thailand and Andaman
result is in agreement with Srivabut et al. [45], who concluded that the Sea) for 2, 6, and 12 months are also illustrated in Fig. 7. It is observed
screw withdrawal resistance was reduced with an increase in wood that the different coastal weathering and exposure times led to more
contents. The control sample un-weathered had the highest screw significant changes in screw withdrawal property. The screw with­
withdrawal strength as compared to those of the WPCs and the hybrid drawal strength of the control sample and the hybrid composites

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Fig. 6. Effects of different coastal weathering on the maximum flexural strain of rubberwood-latex sludge flour reinforced with polypropylene hybrid composites.

Fig. 7. Effects of different coastal weathering on screw withdrawal strength of rubberwood-latex sludge flour reinforced with polypropylene hybrid composites.

continuously decreased with an increase in exposure time. The highest concluded that the control sample, the WPCs, and the hybrid composites
reduction of screw withdrawal strength values ranging from 54.9 MPa to weathered under the Gulf of Thailand degraded more screw withdrawal
17.0 MPa was determined in the control sample after weathering under strength than that weathered under the Andaman Sea.
the Gulf of Thailand for 12 months. The highest loss about 223.3% and
159.5% was found in the control sample after weathering under con­ 3.4.3. Hardness property
ditions of the Gulf of Thailand and the Andaman Sea, respectively. The The evaluation of strength on the surface of the hybrid composites
reason for such an extra reduction of the screw withdrawal strength may un-weathered and weathered for 2, 6, and 12 months under different
be found in the fact that the plastic brittleness under natural weathering coastal weathering conditions (the Gulf of Thailand and the Andaman
degraded the surface layer, which contributes less to the strength [23, Sea) is presented by hardness properties. The experimental results of
26,41]. In addition, when comparing the screw withdrawal strength of each condition are shown in Table 4 and Fig. 8. It is a known fact that the
the hybrid composites with latex sludge flour and RWF as reinforcing hardness of the composites made with the reinforcing filler was signif­
fillers under both coastal weathering conditions, the hybrid composites icantly higher than those of the control sample. As reported by Nukala et
with 25 wt% FLSF (P46R25F25) had a higher loss percentage than those at. [18], it was concluded that the hardness values of the composites
of the WPCs and P46R25C25. The loss in screw withdrawal strength of increased with the increasing wood waste content and higher hardness
P46R25F25 after weathering under conditions of the Gulf of Thailand values than those of recycled plastic waste. As expected, the hybrid
and the Andaman Sea for 12 months was 84.2% and 51.1%, respectively. composites reinforced with both RWF and CLSF or FLSF as fillers had
Furthermore, it was found that different coastal weathering condi­ higher hardness values than the pure PP. As can be seen in Table 4, the
tions (the Gulf of Thailand and the Andaman Sea) significantly influ­ reinforcement with FLSF had a better hardness value than the compos­
enced the screw withdrawal strength of the hybrid composites. It is ites with CLSF and RWF. This is due to the latex sludge flour from FLSF
observed from the P46R25C25 weathered for 12 months that the hybrid absorbing large amounts of energy and good stress transfer during the
composites weathered under the Gulf of Thailand could hold worse deformation process [32]. It is also found that the hybrid composites
screws than the Andaman Sea, in which loss of their screw withdrawal with 25 wt% FLSF (P46R25F25) un-weathered had the highest hardness
strengths was 84.2% and 55.1%, respectively. These results could be values of 81.1 shore D, while the average hardness value for the control

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C. Srivabut et al. Composites Part C: Open Access 12 (2023) 100383

Fig. 8. Effects of different coastal weathering on the hardness of rubberwood-latex sludge flour reinforced polypropylene hybrid composites.

samples was found about 76.3 shore D. These results could be explained RWF, while the hybrid composites weathered under the coastal cli­
that the reinforcing fillers has a considerably higher hardness values mates gave larger crystallinity degree and thermal stability than
than the plastic matrix [18,28,39]. those that were un-weathered.
Additionally, the hardness values of the hybrid composites with • The hybrid composites rapidly increased the lightness and total color
different coastal weathering (Gulf of Thailand and Andaman Sea) for 2, change after weathering under the coastal climates for 2 months, and
6, and 12 months are also displayed in Fig. 8. Theoretically, the hardness then insignificantly increased until 12 months of coastal exposure
values greatly decreased with an increase in the exposure times [41,45]. due to bleaching in photo-oxidation of the wood component.
This study also revealed that the degradation in hardness values of the • The degradation in mechanical properties, such as MOR, MOE, SWS,
hybrid composites and the control samples increased after the coastal and hardness, of the hybrid composites after weathering under the
weathering exposure for 2 months and then decreased rapidly after 6 coastal climates continually increased until 12 months. This is
months until 12 months. Compared to the hybrid composites in the because of continuous chain scissions of the plastic matrix with
formulation of P46R50, P46R25F25, and P46R25C25 weathered under increasing exposure times.
the Gulf of Thailand and the Andaman Sea for 2, 6, and 12 months, the • The hybrid composites weathered under the Andaman Sea showed
hardness values of the P46R25C25 were the best tolerated, followed by higher MOR, MOE, SWS, and hardness than those weathered under
P46R25F25 and P46R50, respectively. This can be explained that the the Gulf of Thailand, which resulted in less loss of mechanical
latex sludge flour as reinforcement had lower moisture absorption than properties after weathering under the coastal climate. This is because
RWF, which could be well inserted into the matrix, resulting in low the weather of the Gulf of Thailand had more average temperature
degradation from coastal weathering. and total rainfall than that of the Andaman Sea.
Moreover, it is also found that the different coastal weathering (the • The WPCs and the hybrid composites indicated a lower loss per­
Gulf of Thailand and the Andaman Sea) affected the hardness values of centage of the mechanical properties than the control sample
the hybrid composites because climate conditions, as shown in Fig. 2, (PP100), after weathering under the coastal climates for 12 months.
decrease different toughness and ductility of the hybrid composites [45].
The hybrid composites weathered under the Gulf of Thailand had higher The knowledge gained from this study would facilitate informed
hardness degradation than that Andaman Sea. The hybrid composites decisions that were appropriate for applications under the coastal cli­
weathered under the Andaman Sea in the formulation of P100, P46R50, mates of the hybrid composites, especially, the building and construc­
P46R25F25, and P46R25C25 had a loss of hardness values of about tion materials, such as railing, fencing, flooring, and decking, normally
8.66%, 6.78%, 10.09%, and 9.53%, respectively, while those weathered applied under the coastal weathering. Additionally, this finding supports
under the Gulf of Thailand had a loss of the hardness of about 10.6%, the effective application of naturally-sourced fillers in plastic compos­
10.2%, and 11.4%, and 10.8%, respectively, as shown in Table 4. Also, ites. The use of latex sludge waste from the rubber latex industries in
the composites with P46R25F25 weathered under the Gulf of Thailand reinforcing fillers will also allow the improvement and development of
had the highest loss of hardness values of about 11.4%, as compared to green material products that can be decomposed naturally.
those of the other samples. Hence, all of the composites weathered under
the Gulf of Thailand for 12 months gave lower hardness values than Declaration of Competing Interest
those weathered under the Andaman Sea.
The authors declared that they have no known competing financial
4. Conclusions interests or personal relationships that could have appeared to influence
the work reported in this paper.
In this study, the hybrid composites’ thermal, physical and me­
chanical properties were characterized before and after weathering Data availability
under different coastal climates, i.e., the Gulf of Thailand and the
Andaman Sea, for 2, 6, and 12 months. We draw the following conclu­ Data will be made available on request.
sions based on the results obtained:

• The hybrid composites added to the latex sludge flour had higher
crystallinity degree and thermal stability than the WPCs with 50 wt%

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