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Vol. 8. Issue 4.
Pages 3389-3398 (July - August 2019)
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Vol. 8. Issue 4.
Pages 3389-3398 (July - August 2019)
Original Article
DOI: 10.1016/j.jmrt.2019.03.015
Open Access
Impact-resistant polypropylene/thermoplastic polyurethane blends: compatible effects of maleic anhydride on thermal degradation properties and crystallization behaviors
Ting An Lina,b, Bao Limina, Mei-Chen Lina,b, Jan-Yi Linb, Ching-Wen Louc,d,e,f,g, Jia-Horng Line,f,g,h,i,j,k,
Corresponding author

Corresponding author at: China Medical University
a Department of Science and Technology, Graduate School of Medicine, Science and Technology, Shinshu University, Nagano Prefecture, 390-8621, Japan.
b Laboratory of Fiber Application and Manufacturing, Department of Fiber and Composite Materials, Feng Chia University, Taichung City, 40724, Taiwan.
c Department of Medical Research, China Medical University Hospital, China Medical University, Taichung, Taiwan
d Department of Bioinformatics and Medical Engineering, Asia University, Taichung, 41354, Taiwan
e Innovation Platform of Intelligent and Energy-Saving Textiles, School of Textiles, Tianjin Polytechnic University, Tianjin, 300387, China
f College of Textile and Clothing, Qingdao University, Shangdong, 266071, China
g Fujian Key Laboratory of Novel Functional Textile Fibers and Materials, Minjiang University, Fuzhou, 350108, China.
h School of Chinese Medicine, China Medical University, Taichung City, 40402, Taiwan.
i Department of Fiber and Composite Materials, Feng Chia University, Taichung City, 40724, Taiwan
j Department of Fashion Design, Asia University, Taichung City, 41354, Taiwan
k Tianjin and Ministry of Education Key Laboratory for Advanced Textile Composite Materials, Tianjin Polytechnic University, Tianjin, 300387, China
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Figures (5)
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Tables (2)
Table 1. Melting and crystalline behaviors of MPP/TPU/MA blends.
Table 2. Degradation temperatures and weight loss of MPP/TPU/MA blends.
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In this study, impact-resistant polypropylene (MPP), thermoplastic polyurethane (TPU) and polypropylene-grafted maleic anhydride (MA) are made into MPP/TPU/MA blends using melt-compounding and injection methods. The blending morphology, crystallization behavior, and melting and thermal behaviors of the blends are evaluated in terms of the content of TPU and MA, examining the influences of the parameters. The scanning electron microscope (SEM) observation shows that 1wt% of MA can effectively enhance the interfacial adhesion and compatibility between MPP and TPU. The differential scanning calorimetry (DSC) results show that the crystallization temperature and melting temperature of the blends are not dependent on the content of TPU or MA. However, using TPU and MA adversely affect the crystalline and melting enthalpy of the blends. The thermogravimetric analysis (TGA) and derivative thermogravimetry (DTG) curve both show that the higher the MPP, the greater the thermal stability of TPU. Likewise, using MA as compatibilizer also has a positive influence on the thermal stability of the blends. The X-ray diffraction (XRD) analyses confirm that the addition of TPU decreases the diffraction intensity of MPP, but does not harm the crystalline structure of MPP. Moreover, the addition of MA improves the compatibility between MPP and TPU. MA marginally decreases the peak value and does not influence the crystallinity degree of MPP. It is expected that the results of SEM, DSC, TGA, DTG, and XRD can serve as a valuable reference for the design of composites with improved thermal and crystallization behaviors.

Impact-resistant polypropylene
Thermoplastic polyurethane
Maleic anhydride
Thermogravimetric analysis
Derivative thermogravimetry
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Polypropylene (PP) is a semi-crystalline and thermoplastic polymer. It is a compound of repeatedly arranged propylene units with a higher crystallization due to the well-arranged molecular chains. PP is characterized with advantages, including ease of processing, chemical resistance, high rigidity, a light weight and a low cost, as well the disadvantages, including high shrinkage ratio, high brittleness at lower temperatures, and low impact resistance [1–5]. The modification of adding soft ethylene units to PP reduces the degree of crystallinity, strengthening the impact resistance of PP. Likewise, adding thermoplastic elastomer to PP also enhances the impact resistance of PP [6–8]. Thermoplastic polyurethane (TPU) is composed of multi-block copolymer where soft segments and hard segments are crossed. The soft and hard segments are incompatible, which leads to phase separation. Namely, the hard segments are separately distributed in soft segments because hard segments are physical-crosslinking agglomerates via intramolecular hydrogen bonding. Soft segments are composed of flexible polyol of ester groups or ether group, providing the composite with rubber-like elasticity. Hard segments are composed of urethane that is a result of reaction between diisocyanate and diols, contributing mechanical reinforcement to the composites [9,10].

Polymer blending is a well-developed manufacturing process with features of efficient production, ease of processing, and good controllability [11–14]. It can effectively modify and adjust the properties of polymer in order to have greater mechanical, thermal, and physical properties, and thus has been commonly used to make functional polymer materials [9,15]. However, the differences in polarity as well as poor interfacial compatibility between PP and TPU provide PP/TPU blends with less comparable functionalities to that of pure PP or TPU [16]. PP-g-MA, PE-g-MA, and PP-g-NH2, are used as a compatilizer in order to improve the interfacial compatibility and difference in polarity between the immiscible and incompatible polyolefins polymers (PP) and TPU [17–21]. In the present study, MPP and TPU are blended at different ratios, after which 0, 1, 3, or 5wt% MA is added as a compatilizer. The blending morphology, melting behavior, crystallization behavior, and thermal properties of the MPP/TPU/MA blends are evaluated, examining the influence of the content of TPU on the blending morphology of MPP matrix as well as the influence of the content of MA on the interfacial compatibility between MPP and TPU.


Impact-resistant polypropylene (MPP) (Prime Polymer, Taiwan) is a copolymer that has good impact resistance, a melt index of 14g/10min (230°C, 2.16kg) (ISO1133), and a density of 0.91g/cm3. Thermoplastic polyurethane (TPU) (Headway Polyurethane, Taiwan) is an ester-type copolymer that has a melt index of 7.03g/10min (175°C, 2.16kg) and a density of 1.23g/cm3. Polypropylene grafted maleic anhydride (MA) (DuPont, US) is a PP pellet that is modified using maleic anhydride, and has a melt index of 49g/10min (190°C, 1.0kg) (ISO1133) and a density of 0.903g/cm3.

2.2Manufacturing process of MPP/TPU/MA blends

A single-screw extruder (SEVC-45, Re-Plast Extruder Corp., Taiwan) is used for the preparation of MPP/TPU/MA blends. The melt-compounding method is used to produce MPP/TPU/MA blends. The ratios of MPP to TPU are 90:10, 80:20, 70:30, and 60:40. The content of MA is 0, 1, 3, and 5wt%. The temperatures of the four processing stages in order are 200, 210, 210, and 210°C. The rotary speed is 25rpm. Fig. 1 shows the manufacturing process of MPP/TPU/MA blends.

Fig. 1.

Schematic diagram of manufacturing process of MPP/TPU/MA blends.

2.3Tests2.3.1Scanning electron microscopy (SEM)

A scanning electron microscope (SEM, Phenom Pure+, Phenom World, Jing Teng Tech, Taiwan) is used to observe the fractured cross-section of sixteen types of MPP/TPU/MA blends. The distribution of TPU in the PP matrix is observed. Moreover, the blending morphology and particle size are observed in order to examine the influence of the content of MA.

2.3.2Differential scanning calorimetry (DSC)

A differential scanning calorimeter (DSC, Q20, TA Instruments, USA) is used to measure the difference in enthalpy. The DSC analyses show how TPU affects the crystallization behavior and melting behavior of MPP, the results of which are used to compare to the crystallization and melting properties of MPP/TPU/MA blends.

2.3.3Thermogravimetric analysis (TGA) and derivative thermogravimetry (DTG)

TGA is used to investigate the relationship between the weight of sample and the difference in temperature, examining the thermal stability of polymer. Samples are placed in the ceramic plate of the scale, and then heated at increments of 10°C/min until 600°C in an oven filled with nitrogen. The TGA results indicate how the content of TPU influences the thermal stability of MPP. To further explore the weight of MPP/TPU/MA blends, the TGA curve is computed with first order of differential to obtain the DTG curve, and the inflection point of TGA reflects the highest peak value of DTG curve.

2.3.4X-ray diffraction (XRD)

Samples are trimmed to be 1cm×1cm, and then scanned at 2°/min in a range of 10–30° using an XRD tester. The diffraction peaks of the materials are recorded, thereby determining whether the amorphous TPU has an impact on the structure crystalline phase of MPP.

3Results and discussion3.1SEM observation

The fractured samples are collected from the impact test. The morphology of the fractured site is observed using SEM images. There are four MMP/TPU ratios (90/10, 80/20, 70/30, and 60/40 as seen in four rows in Fig. 2) and four MA contents (0, 1, 3, 5wt% as seen in four columns in Fig. 2), creating sixteen types of MMP/TPU/MA blends. With zero MA, increasing the TPU content provides the blends with a rough surface and a large TPU granule size (Fig. 2(a, e, i, and m)) [22]. MPP is a non-polar polymer while TPU is a polar polymer. Due to the differences in polarity and interfacial tension, MPP and TPU are two polymers that are incompatible. For the groups with 30 or 40wt% of TPU (Fig. 2(i and m)), the TPU granules resemble narrow fibers. This phenomenon is ascribed to the interaction force under a flow field caused by the single-screw extruder [2]. Moreover, 30 or 40wt% TPU also intrigue the apparent presence of voids, which is evidence that the poor adhesion triggers TPU granule to detach from the MPP matrix [9,23].

Fig. 2.

SEM images (500×) of MPP/TPU/MA blends with various compositions.


Regardless whether the MA content is 1, 3, or 5wt% the blends that are made with MPP/TPU ratios of 90/10 and 80/20 (Fig. 2(b–d, f, g, and h)) display a multi-layer structure and random cracks, suggesting that using MA as an effective compatilizer that improves the surface tension between the TPU and MPP. Moreover, the absence of intra-layer shadow indicates shortened distance between laminates. As MPP and TPU do not have jointed chemical bonds, MA is used to improve the polarity of MPP as well as to react with isocyanate that is the dissociated urethane bond of TPU during the melt-blending process, thereby forming grafting copolymer between MPP and TPU's interphase, eventually enhancing the diverse functionalities of the blends.

Fig. 2(i–l) shows images of the MPP/TPU/MA blends with specified 30wt% of TPU and 0, 1, 3, and 5wt% of MA. A high MA content contributes to the interfacial compatibility between MPP and TPU. With the content of MA increasing from 0wt% to 5wt%, the size of TPU particles significantly decreases and the blends have an even morphology, proving that using MA as a compatilizer improves interfacial bonding between TPU and MPP. In particular, 3wt% of MA exhibits the optimal improvement on the interfacial compatibility [24]. However, for 60/40 group (Fig. 2(m–p)), the addition of 1 or 3wt% of MA cannot inhibit the large size and detachment of TPU granules until 5wt% of MA is used. 5wt% MA is found to stabilize the interfacial bonding between MPP/TPU/MA blends composed of 40wt% of TPU [25]. To sum up, MA is an effective compatilizer for immiscible and incompatible TPU and MPP, and using MA is even more crucial when the MPP and TPU are blended with similar amounts. Moreover, isocyanate that is caused by the interaction of MA and TPU also contributes to the adhesion of MPP and TPU as well as better transmission of stresses [26].

3.2Differential scanning calorimetric (DSC) analyses

Fig. 3 shows the crystalline and melting behavior of MPP/TPU/MA blends, and Table 1 shows the crystallization temperatures, crystallization enthalpy, melting temperature, and melting enthalpy. MPP and TPU are both co-polymers. When they are melt-blended, the melting and crystallization properties of the blends are subjected to the influences exerted by the intrinsic properties. Polypropylene is a compound of propylene as monomers and is semi-crystalline polymer with a high rigidness but low impact resistance. MPP is the modified polypropylene that is polymerized with a few amount of flexible ethylene unit. MPP thus has improved impact resistance at low temperatures and reduced arrangement of crystallinity. The crystalline characterization peak occurs at 62.51°C for TPU and 130.02°C for MPP, and the melting peaks occur at 145.56°C for TPU and 165.64°C for MPP. The marginal difference in enthalpy of TPU causes insignificant peak values. In addition, the crystalline and melting enthalpy of pure TPU (100wt%) are 5.59 and 7.80J/g, and those for pure MPP (100wt%) are 83.70 and 87.22J/g.

Fig. 3.

Crystalline and melting behaviors of MPP/TPU/MA blends, (A) (a) MPP/TPU/MA blends without addition of MA, (B) (b) MPP90/TPU10 blends, (C) (c) MPP80/TPU20 blends, (D) (d) MPP70/TPU30 blends, and (E) (e) MPP60/TPU40 blends, with addition of 0, 1, 3 and 5wt% MA.

Table 1.

Melting and crystalline behaviors of MPP/TPU/MA blends.

  Crystallization temperature (°C)  Crystallization enthalpy (J/g)  Melting temperature (°C)  Melting enthalpy (J/g) 
TPU100  62.51  5.59  145.56  7.797 
MPP100  130.02  83.70  165.64  87.22 
MA-0  129.56  83.61  165.77  88.27 
MA-1  130.15  77.09  165.61  79.21 
MA-3  128.12  71.87  166.21  72.3 
MA-5  127.66  84.12  165.19  85.29 
MA-0  130.43  70.97  166.05  75.65 
MA-1  128.64  76.82  165.33  79.5 
MA-3  128.28  72.86  165.39  75.27 
MA-5  127.28  77.15  165.14  80.04 
MA-0  128.32  70.32  165.07  75.52 
MA-1  128.66  73.33  165.37  75.30 
MA-3  127.16  77.30  165.09  81.36 
MA-5  126.78  70.70  165.18  74.23 
MA-0  126.59  56.37  165.07  60.83 
MA-1  127.52  58.57  165.12  62.82 
MA-3  126.79  58.54  164.68  64.01 
MA-5  126.01  67.18  164.93  70.67 

Fig. 3(A) shows that the crystallization temperature of MPP/TPU/MA blends is not dependent on the content of TPU, but the crystallization enthalpy decreases when the content of TPU increases [27]. The phenomenon is ascribed to the fact that MPP is polypropylene with a low crystallization level and TPU is non-crystalline polymers. The soft segments of TPU account for a greater ratio in the system, and their dynamic flow enter the crystalline phase and disorganized structure of MPP. Consequently, the mobility and diffusion of MPP chains decrease [26]. The crystallization enthalpy of MPP60/TPU40/MA0 is 56.37J/g, which is 27.3% lower than that of pure MPP.

Fig. 3(B–E) shows the crystalline behavior of MPP90/TPU10, MPP80/TPU20, MPP70/TPU30, and MPP60/TPU40 as related to different amounts of MA. MA has a marginally negative influence on the crystalline enthalpy of MPP/TPU/MA blends, indicating that the crystalline enthalpy of the system primarily depends on MPP, rather than TPU. Based on Table 1 and Fig. 3(a), increasing TPU only slightly left-shifts the melting temperature of the MPP/TPU/MA blends, but the reduction in melting enthalpy makes the melting characterization peak flatter [9]. Moreover, adding TPU deteriorates the α-relaxation peak of MPP as great amount of TPU adversely affects the mobility of the crystalline-phase chains and the heat fusion of MPP [26].

Fig. 3(b–e) shows that the presence of MA does not affect the melting temperature of the blends, and more TPU renders the melting enthalpy with a decreasing trend. Being a non-crystalline polymer, more TPU damages the crystallization structure of MPP that serves as continuous-phase polypropylene in the blends. Consequently, it requires only a low heat to break molecular bonding. During the melt-blending process, the soft segments of TPU in a dynamic flow enter the amorphous domain, which damages the molecular interaction of MPP. The enhanced activity and flexibility of MPP soft segments undermines the overall crystallization ability [28].

3.3TGA and DTG

Table 2 shows the thermal degradation temperature with corresponding weight loss; Fig. 4 shows the TGA and DTG results of MPP/TPU/MA blends. The pure TPU and pure MPP have two-step thermal degradation and one-step thermal degradation, respectively. Two-step thermal degradation of TPU occurs at 302.6°C and then 395°C, which respectively show the degradation of hard segments and soft segments. The decomposition of urethane bonds may cause the dissociation of isocyanate, alcohol, primary amines, olefins, and carbon dioxide [26]. Moreover, MPP reaches the highest thermal decomposition peak at 445°C, which starts from the formation of free radicals and ends at chain scission. Given the aforementioned discussion, MPP has greater thermal stability than TPU [26].

Table 2.

Degradation temperatures and weight loss of MPP/TPU/MA blends.

  1st degradation temperature (°C)  Weight loss (wt%)  2nd degradation temperature (°C)  Weight loss (wt%)  3rd degradation temperature (°C)  Weight loss (wt%) 
TPU100  302.59  14.18  395.29  66.72  –   
MPP100  –  –  –  –  441.09  70.82 
MA-0  338.77  4.82  –  –  456.94  58.82 
MA-1  341.64  5.65  –  –  456.79  60.46 
MA-3  348.78  5.66  –  –  456.97  61.15 
MA-5  350.67  8.52  –  –  456.61  60.18 
MA-0  314.28  4.07  352.11  10.84  459.62  58.94 
MA-1  317.93  3.76  356.99  11.00  462.49  63.75 
MA-3  319.60  4.86  356.60  12.82  460.38  63.80 
MA-5  323.68  4.03  357.72  10.39  461.94  62.64 
MA-0  321.08  5.62  365.59  16.35  467.06  66.35 
MA-1  324.76  5.56  363.13  14.26  467.58  65.25 
MA-3  322.81  5.59  364.22  15.25  466.57  65.70 
MA-5  326.61  5.02  368.71  13.75  470.58  65.42 
MA-0  329.05  6.69  377.45  20.24  470.56  69.38 
MA-1  321.53  6.53  382.45  23.26  471.68  71.90 
MA-3  324.58  3.81  375.35  11.69  468.79  63.38 
MA-5  325.82  4.73  374.71  15.04  468.80  65.99 
Fig. 4.

TGA and DTG analysis of MPP/TPU/MA blends, (A) (a) MPP/TPU/MA blends without addition of MA, (B) (b) MPP90/TPU10 blends, (C) (c) MPP80/TPU20 blends, (D) (d) MPP70/TPU30 blends, and (E) (e) MPP60/TPU40 blends, with addition of 0, 1, 3 and 5wt% MA.


Table 2 and Fig. 4(A) (a) show that except for MPP90/TPU10 blends, the thermal degradation of the remaining MPP/TPU/MA blends is divided into three stages. MPP90/TPU10 blends exhibit an unclear second-stage thermal decomposition that is mostly like to be the decomposition of remaining hard segments in the first-stage thermal decomposition, which is surmised due to the limited 10wt% of TPU. Noticeably, more TPU retards the occurring of the first- and third-stage thermal decomposition, but advances the occurring of the second-stage thermal decomposition. The first stage of thermal decomposition involves the hard segments and the second stage involves the breakage of molecular chain of MPP. MPP has relatively higher thermal stability and helps postpone decomposition of urethane bonds of TPU hard segments. Additionally, the advanced second-stage decomposition is due to the high crystallization of MPP's molecular chains, which damages the molecular chain of TPU's soft segments. The temperature of thermal decomposition thus has an advanced presence, and the thermal stability of soft segments is reduced. Although MPP and TPU are incompatible, MPP still distinctively improves the thermal stability of TPU [26].

Table 2 and Fig. 4(B–E) (b–e) show that it is positive to use MA to MPP80/TPU20 and MPP70/TPU30 blends in terms of improving the thermal stability and postponing the thermal decomposition at higher temperature. However, using MA only slightly decreases the thermal stability of MPP60/TPU40 blends, and does not influence that of MPP90/TPU10 blends. Namely, the compatilizer can reduce the difference in polarity as well as interfacial interaction, reinforcing the adhesion of two materials. When MPP and TPU are blended with a similar amount (i.e. MPP60/TPU40), a limited amount of compatilizer is unable to adhere the immiscible materials. Moreover, compared to pure TPU and pure MPP, MPP/TPU/MA blends composed of more TPU and less MPP have a lower weight loss, suggesting that MPP's high thermal stability positively improve TPU's low thermal stability.

3.4XRD analyses

Fig. 5 shows the XRD analyses of MPP/TPU/MA blends, indicating that MPP has high degree of crystallinity and TPU has low degree of crystallinity. MPP is semi-crystalline isotactic and has characteristic peaks of a stable monoclinic system (α-phase). TPU is amorphous polymer and observed to have a low peak value that is a result of superimposed amorphous diffraction halo [7,29]. Fig. 5(A) shows that pure MPP exhibits the Bragg diffraction peak values of (110), (040), (130), (111), and (131) when 2θ is at 14.1°, 16.8°, 18.5°, 21.3°, and 21.8°. By contrast, TPU exhibits a broad diffraction peaks with a center of 20.7° when 2θ is between 16° and 26° [30]. In addition, the intensity of characteristic peaks decreases when the MPP/TPU/MA blends are composed of more TPU. This finding is attributed to the amorphous TPU: more TPU exerts a negative influence on the crystalline structure of the semi-crystalline MPP, decreasing the crystallinity and peak intensity.

Fig. 5.

XRD analysis of MPP/TPU/MA blends, (A) MPP/TPU/MA blends without addition of MA, (B) MPP90/TPU10 blends, (C) MPP80/TPU20 blends, (D) MPP70/TPU30 blends, and (E) MPP60/TPU40 blends, with addition of 0, 1, 3 and 5wt% MA.


Fig. 5(B–E) shows that the control group (i.e. 0wt% of MA) and experimental group have similarly slight decrease in characterization peak values. The urethane bond of TPU graft reacts with MA to form isocyanate, which occurs in amorphous phase and does not affect MPP's crystalline structure. The purpose of adding MA is only to improve the difference in polarity and interfacial tension between MPP and TPU. The positive influence on the diffraction peaks is too marginal to discuss, making MA an irrelative factor in this case. In sum, TPU (dispersive phase) and MA (the compatilizer) are both excluded being a nucleating agent for MPP (continuous phase) and there are no dominant influences on the crystalline structure but only marginal improvement on characteristic peak intensity.


This study manufactures MPP/TPU/MA blends with continuous phase material (MPP), dispersive phase material (TPU), and a compatilizer (MA) using melt-blending and injection method. The blending morphology and thermal, melting, and crystalline behavior of the blends are investigated. SEM results indicate that 1wt% of MA significantly improves the adhesion between incompatible TPU and MPP. DSC results indicate that TPU and MA only slightly decrease the crystalline and melting enthalpy of the blends, but are proved not to be correlated with the crystalline and melting temperature. Based on the results of TGA and DTG, the thermal stability of TPU is proportional to the content of MPP. The compatilizer has a positive influence on the structural stability, improving the thermal stability. XRD analyses show that though adding TPU helps with the diffraction intensity of MPP, TPU does not serve as a nucleating agent that affects the crystalline structure of MPP. The addition of MA facilitates the poor interfacial compatibility between the immiscible MPP and TPU, while improving the crystallinity degree and peak intensity. The experimental design is adjustable and expected to meet the demands of diverse applications.


The authors would especially like to thank Ministry of Science and Technology, Taiwan, for financially supporting this research under Contract MOST 107-2632-E-035-001.

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