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Article

A Comparative Study on the Compatibilization of Thermoplastic Starch/Polybutylene Succinate Blends by Chain Extender and Epoxidized Linseed Oil

by
Ke Gong
1,2,*,
Yinshi Lu
2,
Alexandre Portela
3,
Soheil Farshbaf Taghinezhad
2,
David Lawlor
2,
Shane Connolly
2,
Mengli Hu
4,
Yuanyuan Chen
2 and
Maurice N. Collins
1
1
Bernal Institute and SFI BiOrbic, University of Limerick, V94 T9PX Limerick, Ireland
2
Polymer, Recycling, Industrial, Sustainability and Manufacturing (PRISM), Athlone Campus, Technological University of Shannon: Midlands Midwest, N37 HD68 Westmeath, Ireland
3
Department of Environment & Climate Action, Tipperary County Council, E45 YW31 Dublin, Ireland
4
College of Chemistry and Materials, Jiangxi Normal University, Nanchang 330022, China
*
Author to whom correspondence should be addressed.
Macromol 2025, 5(2), 24; https://doi.org/10.3390/macromol5020024
Submission received: 21 March 2025 / Revised: 18 April 2025 / Accepted: 7 May 2025 / Published: 12 May 2025
(This article belongs to the Collection Advances in Biodegradable Polymers)
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Abstract

:
The immiscibility of thermoplastic starch (TPS) and polybutylene succinate (PBS) complicates the thermal processing of these materials. This study provides the first comparative assessment of two compatibilizers with differing reaction mechanisms, Joncryl® ADR 4468 and epoxidized linseed oil (ELO), for the optimization of biobased TPS/PBS blends. A total of 13 batches, varying in compatibilizer and blend composition, were processed via hot melt extrusion and injection molding to produce pellets. Blends were analyzed using tensile and impact testing, differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR), rheology, and scanning electron microscopy (SEM). The findings suggest that both compatibilizers can improve the compatibility of these blends, as evidenced by higher glass transition temperatures (Tg) compared to the reference batch (100-0-N/A). Joncryl® ADR 4468 batches exhibit superior tensile strength and Young’s moduli, while ELO batches demonstrate greater elongation at break. The enhanced processability observed in Joncryl® ADR 4468 is attributed to the increased polymer chain entanglement and molecular weight, whereas ELO facilitates greater chain mobility due to its plasticizing effect. These differences arise from the distinct mechanisms of action: Joncryl® ADR 4468 promotes chain extension and crosslinking, whereas ELO mainly enhances flexibility through plasticization. Overall, this study provides a comparative assessment of these compatibilizers in TPS/PBS blends, laying the groundwork for future investigations into optimizing compatibilizer concentration and blend composition.

1. Introduction

Environmental pollution caused by plastic waste has become an increasing concern among the public due to the widespread use of plastic materials [1]. In response to this issue, biodegradable polymers are being increasingly employed in various applications, including agricultural films [2], food packaging [3], farming [4] and wound healing [5]. These developments suggest that biodegradable polymers with improved properties could serve as viable alternatives to conventional non-degradable plastics. Thermoplastic starch (TPS), a modified form of starch that has undergone decrystallization or complete structural disruption [6], is widely investigated in current research due to its promising biodegradability [7]. However, the practical application of TPS is hindered by its inherent limitations, including poor water resistance and insufficient mechanical strength [8]. To address these challenges, TPS is often blended with other biodegradable polymers, such as polylactic acid (PLA) [9,10], polybutylene succinate (PBS) [11,12], and poly(butylene adipate-co-terephthalate) (PBAT) [13,14]. Among them all, PBS has gained significant attention in various fields due to its thermomechanical and physical properties, which are comparable to those of polypropylene [15,16], as well as its excellent biodegradability, melt processability, and chemical resistance [17]. Consequently, blending TPS with PBS offers a promising approach to developing biodegradable materials with enhanced mechanical properties and improved processability [18,19,20,21]. Given the growing market presence of TPS/PBS composites, addressing their miscibility (chemically opposite) remains a critical challenge, with starch as a hydrophilic polymer and PBS as a hydrophobic polymer [22]. Therefore, the development of compatibilizers to enhance interfacial interactions between TPS and PBS has become a key area of research.
To date, both ex situ [22] and in situ [23] compatibilization strategies have been explored to enhance the interfacial interactions between TPS and PBS. Among these, in situ compatibilization is more widely adopted, as it involves generating the compatibilizing agent directly during the mixing process. In this approach, compatibilizers with a low molecular weight and melting viscosity are particularly advantageous due to their cost-effectiveness and ability to diffuse efficiently at the blend interface [24]. For instance, maleic anhydride-grafted compatibilizers, such as MA-g-PCL and MA-g-PBS, have been utilized in PBS-starch blends, leading to a noticeable reduction in the dispersed phase size [23]. In a study by Lopez-Galindo et al. [25], dicumyl peroxide (DCP) and tartaric acid (TA) were employed as coupling agents in TPS/PBS blends, with glycerol serving as a plasticizer. Their findings revealed that DCP enhanced tensile strength and ductility without inducing chemical interactions between TPS and PBS, whereas TA contributed to increased ductility but reduced tensile strength due to the formation of new bonds within the carbonyl groups of PBS. Furthermore, Fahrngruber et al. [26] examined two compatibilization approaches based on native starch and pre-plasticized starch within TPS/PBS blends. Their study revealed that the pre-plasticized batch exhibited improved TPS incorporation into PBS, along with superior tensile strength and tear resistance.
In addition to these compatibilization techniques, the incorporation of a chain extender represents another promising strategy for enhancing blend interfacial adhesion due to its polyfunctionality and thermal stability. Sufficient processing time enables chain extenders to fully react with the polymer blend [27], making them highly suitable for industrial applications. During the melt processing of polymers containing chain extenders, the molecular weight of the polymers can be preserved or even increased, as the chain extenders facilitate the reconnection of polymer chains that undergo degradation during processing [28]. Following chain extension, the resulting increase in molecular weight contributes to improved mechanical properties and the thermal stability of the polymer system [29]. Among the various chain extenders available, multifunctional styrene–acrylic oligomeric chain extenders, marketed under the tradename Joncryl® ADR, are the most widely used. Originally patented by Johnson Polymer LLC [30] and later acquired by BASF SE [31], these chain extenders typically react with the functional groups present at the polymer chain ends, thereby facilitating the chain extension process. Therefore, they can significantly improve the processability and properties of recycled polymers [32,33]. For example, Nofar et al. [34] demonstrated that incorporating 0.25 wt.% of Joncryl® ADR 4368 effectively mitigated the thermal degradation sensitivity of recycled polyethylene terephthalate (PET), where a further increase in the chain extender concentration led to a substantial reduction in the melt flow index of the recycled PET batches. Moreover, multifunctional styrene acrylic Joncryl® ADR chain extenders have been shown to enhance the properties of various polyester blends, including TPS with polybutylene adipate-co-terephthalate (PBAT) [35,36] and PLA [10,37], respectively. Nevertheless, the incorporation of Joncryl® leads to reactions with polymer chain ends, resulting in increased brittleness in the finalized material, particularly in PLA/TPS blends [10]. To address this issue, linseed oil, a naturally derived plasticizer, has been proposed as an alternative due to its ability to enhance compatibility while improving flexibility [38], toughness [39], and even biodegradability [40] within polymer blends.
In the context of the aforementioned studies, a comparative study was conducted here to determine the performances of the TPS/PBS blends compatibilized using Merginat ELO 8,510,100 Linseed Oil and Joncryl® ADR 4468 chain extender. Initially, the tensile and impact properties of both formulations were analyzed, followed by an investigation of morphological characteristics and rheological behavior to comprehensively assess the overall performance of these compatibilizers when processing these biopolymer blends.

2. Materials and Methods

2.1. Material

Thermoplastic starch (TPS) pellets (Solanyl® C1201) and BioPBSTM pellets (FZ91) were purchased from Solanyl Rodenburg Corporation (Oosterhout, The Netherlands) and Mitsubishi Chemical Group Corporation (Tokyo, Japan), respectively. The selected compatibilizers, Joncryl® ADR 4468 and Merginat ELO 8510100, were supplied by BASF SE Corporation and HOBUM Oleochemicals GmbH Corporation, both based in Ludwigshafen Am Rhein and Hamburg Germany, respectively. The characteristics of raw materials (TPS and PBS) are shown in Table 1.

2.2. Sample Fabrication

For the preparation of the composite materials, Joncryl® ADR 4468 was first measured at 1 phr and subsequently blended with the raw materials during the compounding process. In the case of linseed oil-containing formulations, a one-channel syringe pump, preloaded with 1 phr of linseed oil, was utilized to ensure precise dosing during compounding.
The composition of the compounded composites is outlined in Table 2. The compounding process was conducted using E-LAB 22 High Temperature Twin-Screw Compounder (EuroTech Extrusion Machinery SRL, Tradate VA, Italy). The temperature profile across zones 1 to 8 was adjusted according to the blend composition, as detailed in Table 3. Following compounding, the extrudates were cooled in a water bath before being pelletized. These pellets were subsequently processed via injection molding (IM) using an Arburg Allrounder Molding Machine to fabricate specimens for further experimental analysis, including mechanical testing (tensile and impact), morphological characterization, and rheological assessment. The specific parameters used in the IM process are summarized in Table 4.

2.3. Tensile Test

Figure 1 shows the geometry of tensile specimens. Tensile tests were performed at room temperature using a 2.5 kN Lloyd LRX Universal Tester (Lloyd Instruments Ltd., Bognor Regis, UK) at a constant crosshead speed of 50 mm/min. The dimensions of the tensile specimens were measured using a vernier caliper prior to the tensile tests. Data acquisition and calculations, including maximum tensile strength (σ), Young’s modulus (E), and elongation at break, were conducted using Nexygen software 3.0. Five replicates of specimens were produced at each condition for each mechanical experimental measurement.

2.4. Impact Test

Charpy impact testing was carried out on cuboid specimens measuring 127 × 12.7 × 6 mm using a Ceast 6545 impact tester (Zwick/Roell, Germany) equipped with a 1-Joule pendulum [41]. The tests were performed in accordance with ASTM D6110-10 standards. Five specimens from each batch were tested in a flatwise orientation on a specimen support with a span of 71.9 mm under ambient conditions. Five replicates were carried out here in purpose of data analysis.

2.5. Differential Scanning Calorimetry

Differential scanning calorimetry (DSC) tests were conducted using 214 polyma (NETZSCH) machine from Selb, Germany for the thermal performances of all compounded materials. All specimens weighed ~8 mg and were placed in non-perforated aluminum pans, with an empty crimped aluminum pan employed as the reference batch. The thermal ramp was set as −90 °C to 200 °C at the rate of 10 °C/min while the cooling rate was −5 °C/min. The glass transition temperature (Tg), the cold crystallization temperature (Tcc) and the melting temperature (Tm) were all determined using Standard ISO 11357-2 2020 [41].

2.6. Fourier Transform Infrared Spectroscopy (FTIR)

FTIR analysis was performed using a Thermo Fisher Scientific ATR Nicolet iZ10 spectrometer (Waltham, Massachusetts, USA), scanning in the wavenumber range of 400 cm−1 to 4000 cm−1. Each spectrum was obtained by averaging 16 scans at a resolution of 4 cm−1.

2.7. Rheological Test

Rheological characterization was conducted using a Discovery Hybrid Rheometer from TA Instruments (New Castle, DE, USA) equipped with a 25 mm diameter parallel plate geometry. Prior to testing, dynamic strain sweep experiments were performed to determine the linear viscoelastic region. Angular frequency sweep tests were then carried out at a fixed strain amplitude of 1%, with an angular frequency range from 0.04 rad/s to 600 rad/s and a testing temperature of 165 °C.

2.8. Fracture Observation

A scanning electron microscope (Mira SEM from Tescan Oxford Instruments, Abingdon-on-Thames, United Kingdom) with the magnitude of X200 was employed in this study to observe the fractured cross sections of tensile bars. All fractured sections were first gold-coated using an Agar sputter coater from Agar Scientific c/o Calibre Scientific, Rotherham, UK.

2.9. Statistical Analysis

The experimental data obtained from tensile and impact tests were analyzed using GraphPad Prism 9 Software based on the analysis of variance (ANOVA) method. The p-value was employed here to determine the degree of significance of material variations. Differences were considered significant if a p value under 0.05 was obtained [42].

3. Results

3.1. Tensile Test

Figure 2 and Figure 3 present the tensile properties of all TPS/PBS blends examined in this study. Results demonstrate that an increase in PBS content enhances elongation at break, rising from 3.1% to 93.8% in the Joncryl® ADR 4468 batches and from 3.2% to 94.1% in the ELO batches, which aligns with the findings of Li et al. [43]. Additionally, higher PBS content generally improves tensile strength, except for the 40-60-oil in the ELO batches. Figure 2 further illustrates the brittle tensile behavior observed in blends containing 100% and 80% TPS, while a progressive increase in ductility is noted from the 60-40-4468 and 60-40-oil batches to the 0-100-4468 and 0-100-oil batches. In terms of Young’s modulus, a declining trend is evident, with the highest values recorded for 100-0-4468 (184.3 MPa) and 100-0-oil (177 MPa), while the lowest values can be observed in 0-100-4468 (75.8 MPa) and 0-100-oil (75.7 MPa). This reduction in stiffness can be attributed to the greater flexibility of PBS relative to TPS, leading to the formation of a continuous and dominant PBS phase as PBS content increases. The presence of this continuous phase composed of a more flexible polymer results in an overall reduction in blend rigidity. Furthermore, Figure 2 reveals that the elongation values of TPS/PBS blends remain relatively low when comparing 20-80-4468 and 20-80-oil with 0-100-4468 and 0-100-oil, respectively. This phenomenon can be attributed to the inherent incompatibility between TPS and PBS [44]. However, the results suggest that ELO may serve as a potential compatibilizer when enhanced elongation is required, as demonstrated by elongation values of 26% for 20-80-4468 and 43.8% for 20-80-oil. Conversely, the tensile strength and Young’s modulus results indicate that Joncryl® ADR 4468 is a more suitable compatibilizer for the TPS/PBS blending process.
Meanwhile, ANOVA analysis indicates that the p-values for both terms (polymer composition and compatibilizer) are 0. This suggests that these factors have a statistically significant effect on tensile strength and Young’s modulus. However, the interaction between composition and compatibilizer does not exhibit a significant impact on tensile strength (p = 0.116 > 0.05) or Young’s modulus (p = 0.167 > 0.05).

3.2. Impact Test

Impact strength is a key parameter for evaluating the mechanical performance of materials, as it directly influences their durability in various applications [45]. An initial assessment of the results in Figure 4 reveals noticeable variations in impact strength across all batches. Specifically, TPS/PBS blends exhibit a significant increase in impact strength with higher PBS content, as evidenced by the differences between the 20-80-4468 and 0-100-4468 batches, as well as between the 20-80-oil and 0-100-oil batches. This improvement can be attributed to the superior ductility of PBS, which effectively counteracts the intrinsic brittleness of TPS.
Regarding the statistical significance of composition, compatibilizer, and their interaction on impact strength, ANOVA analysis indicates that composition has a significant effect (p = 0). However, neither the compatibilizer (p = 0.52 > 0.05) nor the interaction between composition and compatibilizer (p = 0.072 > 0.05) exhibit a statistically significant impact on impact strength.

3.3. Differential Scanning Calorimetry

Figure 5 presents the thermal performances of 100-0-4468, 100-0-oil, and 100-0-N/A (no compatibilizer added). It can be found here that the Tg, Tcc, and Tm values of 100-0-N/A are slightly lower than those of 100-0-4468 and 100-0-oil, indicating a positive impact of the compatibilizer on the blended materials.
For other compositions, batches with Joncryl® ADR 4468 exhibit higher Tg values than the ELO counterparts with the same composition, as shown in Figure 6a,b. For instance, the Tg of 80-20-4468 is −2.7 °C, whereas that of 80-20-oil is −9.1 °C. Similarly, the Tg of 20-80-4468 is −25.6 °C, compared to that of −26.6 °C for 20-80-oil. This difference may be attributed to two key factors: (1) the high concentration of unsaturated fatty acids in ELO, which acts as a plasticizer, increasing the free volume and molecular mobility of the polymer matrix [46], and (2) the ability of ELO’s fatty acids to integrate easily with the polymer matrix, thereby reducing blend rigidity, whereas Joncryl® ADR 4468 facilitates crosslinking [47] and increases molecular weight [48], resulting in a more rigid structure.
Additionally, a downward trend in Tg is observed with increasing PBS content, ranging from −2.7 °C to −31.2 °C for Joncryl® ADR 4468 batches and from −9.1 °C to −32.8 °C for ELO batches. This decrease can be attributed to the disruption of hydrogen bonding within PBS molecular chains and weakened intermolecular forces within TPS.
With respect to Tcc, a comparison between Figure 5 and Figure 6 reveals that crystallization parameters during the heating stage are only observed in 100% TPS batches. For the remaining blends (Figure 6c,d), these parameters are only discernible during the cooling stage. This finding is consistent with previous research [49] and is likely due to the insufficient time available for PBS to crystallize during the cooling process.
Regarding Tm, two distinct melting temperatures are evident in the blended batches (Figure 6e,f). This phenomenon is primarily attributed to (1) the distinct melting points of the individual components, with TPS melting at approximately 155 °C and PBS melting at around 110 °C, and (2) the formation of separate crystalline regions due to phase separation.

3.4. Fourier Transform Infrared Spectroscopy

The FTIR spectra of TPS/PBS blends as a function of the Joncryl® ADR 4468 chain extender and linseed oil as a function of compatibilizer content are shown in Figure 7. The spectra indicate the presence of C–H bond stretching (alkane) across all samples, with wavenumbers ranging from 2924.56 to 2946.3 cm−1 in Joncryl® ADR 4468 blends and from 2942.8 to 2946.88 cm−1 in ELO blends [50,51]. Additional functional groups, including alkenes, esters, and aromatic compounds, were identified in the analyzed samples. Specifically, C–O stretching was observed within the range of 1042.31 to 1154.58 cm−1, while C=O stretching appeared between 1712.5 and 1737.41 cm−1 [52,53]. Furthermore, as shown in Figure 7a,b, minimal variations were detected in the C=O absorption vibration peaks across all samples, which aligns with the findings of previous research [53]. This finding suggests a lack of significant chemical interactions between TPS and PBS, a conclusion further supported by the mechanical test results. Additionally, a comparison of the C=O absorption peaks in Figure 7a,b indicates that batches containing Joncryl® ADR 4468 exhibited higher wavenumbers than those containing ELO, with values such as 1737.41 cm−1 for 100-0-4468 and 1736.83 cm−1 for 100-0-oil. This shift may be attributed to the increased interaction between oxygen atoms in the C=O groups and hydroxyl (-OH) groups from TPS, facilitated by the chain extension effect of Joncryl® ADR 4468. Moreover, the FTIR analysis revealed no distinct characteristic peaks associated with either Joncryl® ADR 4468 or ELO, indicating that neither compatibilizer triggered reactions leading to the formation of new functional groups, despite evidence of hydrogen bond weakening.

3.5. Rheological Result

Rheological analyses were performed to assess the storage modulus, loss modulus, and complex viscosity of all TPS/PBS blends, with the results presented in Figure 8 for Joncryl® ADR 4468 batches and Figure 9 for ELO batches. The findings demonstrate shear-thinning behavior across all batches, where viscosity decreases under high shear rates and increases during the cooling and solidification stages in injection molding.
A first glance at the complex viscosity, a reduction with increasing angular frequency was observed for all blends. Additionally, the Joncryl® ADR 4468 batches exhibited consistently higher complex viscosity values than the ELO batches, with the exception of a slight difference between 100-0-4468 and 100-0-oil. This disparity can be explained by the presence of more entangled molecular chains and higher molecular weight present in the Joncryl® ADR 4468 batches compared to that in the ELO samples [54,55]. However, it should be noted, based on Figure 8c and Figure 9c, that an optimized blend composition of TPS/PBS should be investigated in the next stage due to their inconsistent viscosity behaviors. This can be explained from the dispersed droplets or co-continuous structures shown in immiscible blends (e.g., PLA loaded over 2.5 wt% with poly (butylene adipate-co-terephthalate [56,57]). Therefore, an optimized loading concentration between the TPS and PBS should be investigated due to the potential benefits to the final quality.
Furthermore, the storage modulus and loss modulus values for Joncryl® ADR 4468 batches were higher than those of ELO batches, aligning with the DSC results. This difference is attributed to the formation of a more interconnected network facilitated by Joncryl® ADR 4468. However, ELO batches exhibited more stable storage moduli, likely due to the plasticizing effect of ELO [46]. A slightly greater value in storage modulus was observed between 100-0-4468 and 100-0-oil due to the induced chain extension and interfacial interaction effects, which is in line with the findings of other studies focusing on chain extenders [58,59]. Notably, a greater gap can be observed in the TPS-PBS blends, which indicates increased reactivity with individual polymers and a more effective interphase compatibilization role in Joncryl® ADR 4468 [55,60]. In contrast, linseed oil primarily acts as a plasticizer, without substantially enhancing phase compatibility.

3.6. Morphological Observation

The microstructure and interfacial adhesion of all blends were analyzed using SEM, as illustrated in Figure 10. The SEM images demonstrate a transition from brittle fracture in 100% TPS batches to increased ductility in PBS-containing blends. For the 100% PBS samples, a slight ductile fracture was observed, particularly in the 0-100-oil batch, where several flake-like structures formed. This phenomenon is likely due to the folding of crystalline planes under tensile loading.
In the TPS/PBS blends, distinct TPS and PBS phase separations are evident, as shown in Figure 10c–j, with TPS being the dispersed phase, which is particularly noticeable in Figure 10c,d. This phenomenon is in line with that observed in other studies and is attributed to the enthalpy of mixing being positive, which may lead to phase separation. Also, when chemical interactions (such as hydrogen bonding) are weak or absent, the materials become immiscible, while high molecular weights tend to lower the entropy of mixing, thereby contributing to immiscibility [61]. Notably, phase separation appears less pronounced in the 80-20-4468 batch compared to the 80-20-oil batch, underscoring the role of compatibilizers in the TPS/PBS compounding process [62] and highlighting the greater effectiveness of Joncryl® ADR 4468 over ELO. Furthermore, comparisons between Figure 10e–j reveal improved miscibility between TPS and PBS in the Joncryl® ADR 4468 batches due to the smaller amount of droplets, aligning with the previously observed mechanical and thermal performance results.
This difference in miscibility may be attributed to the distinct mechanisms of Joncryl® ADR 4468 and ELO. While Joncryl® ADR 4468 enhances compatibility through crosslinking via chain extension, ELO functions as both a chain extender and a lubricant, forming a gel-like structure [46]. ELO facilitates compatibilization by interacting with the chain ends of PBS and hydroxyl groups in TPS. However, its lubricating effect increases chain mobility, leading to greater polymer chain distances and weaker polymer–polymer interactions [46,63]. According to gel theory, ELO acts as a plasticizer, further reducing polymer–polymer interactions, which is particularly evident in Figure 10f,h,j. In contrast, Joncryl® ADR 4468 enhances compatibilization by interacting with the chain ends of PBS and hydroxyl groups in TPS without introducing lubricating or gel-forming effects.

4. Conclusions

This study examines the comparative effectiveness of the polymeric chain extender Joncryl® ADR 4468 and ELO as compatibilizers in improving the mechanical, thermal, and morphological properties of TPS/PBS blends. The results from tensile and impact testing indicate that incorporating PBS enhances the strength and ductility of the final materials, particularly in the presence of both compatibilizers. This improvement is attributed to the chemical structures of the compatibilizers, which facilitate interactions with the hydroxyl groups present in the PBS and TPS chains, leading to chain extension and enhanced compatibilization. However, the batches with Joncryl® ADR 4468 exhibited superior mechanical strength and Young’s moduli compared to the batches with ELO. This difference is primarily due to the plasticization effect of ELO, which increases chain mobility and reduces polymer–polymer interactions, leading to phase separation, as observed in morphological analyses. The plasticization effect is further confirmed by the lower glass transition temperatures (Tg) recorded for the ELO batches compared to those recorded for the Joncryl® ADR 4468 batches. Despite its relatively lower mechanical performance, ELO presents a promising alternative as a natural, eco-friendly compatibilizer with a low carbon footprint and reduced toxicity during processing. This study provides a basis for further optimization strategies, such as refining blending parameters and incorporating nanoclays, to enhance the properties of ELO-modified TPS/PBS blends.

Author Contributions

Conceptualization, K.G., Y.C. and M.N.C.; methodology, K.G., Y.L., A.P., D.L. and S.C.; software, K.G., Y.L. and A.P.; validation, K.G., Y.C. and M.N.C.; formal analysis, K.G., S.F.T., Y.C. and M.N.C.; investigation, K.G., Y.C. and M.N.C.; resources, K.G., Y.C. and M.N.C.; data curation, K.G., M.H., Y.C. and M.N.C.; writing—original draft preparation, K.G., M.H., Y.C. and M.N.C.; writing—review and editing, K.G., S.F.T., Y.C. and M.N.C.; visualization, K.G., Y.C. and M.N.C.; supervision, K.G., Y.C. and M.N.C.; project administration, K.G., Y.C. and M.N.C.; funding acquisition, Y.C. and M.N.C. All authors have read and agreed to the published version of the manuscript.

Funding

This research is supported by Research Ireland (SFI22/NCF/HE/1142) and MAGICBIOMAT (HE101181381).

Data Availability Statement

The data presented in this study are available on request from the corresponding author since the data are part of an ongoing research.

Acknowledgments

The authors would like to acknowledge the support they received from the staff in Applied Polymer Technology and Centre for Industrial Services and Design in Technological University of Shannon: Midlands and Midwest.

Conflicts of Interest

The authors declare no conflicts of interest.

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Figure 1. Dimensions of injection-molded tensile bars.
Figure 1. Dimensions of injection-molded tensile bars.
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Figure 2. Stress–strain curves as a function of (a) Joncryl® ADR 4468 batches and (b) ELO batches (n = 5).
Figure 2. Stress–strain curves as a function of (a) Joncryl® ADR 4468 batches and (b) ELO batches (n = 5).
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Figure 3. Tensile results of TPS/PBS blends as a function of varied compatibilizers: (a) Joncryl® ADR 4468 and (b) ELO (n = 5).
Figure 3. Tensile results of TPS/PBS blends as a function of varied compatibilizers: (a) Joncryl® ADR 4468 and (b) ELO (n = 5).
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Figure 4. Impact test results for the TPS/PBS blends as a function of compatibilizers, (n = 5).
Figure 4. Impact test results for the TPS/PBS blends as a function of compatibilizers, (n = 5).
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Figure 5. DSC results for batches of 100-0-4468, 100-0-oil, and 100-0-N/A.
Figure 5. DSC results for batches of 100-0-4468, 100-0-oil, and 100-0-N/A.
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Figure 6. DSC results in this study: (a) Tg for 80-20-4468 to 0-100-4468; (b) Tg for 80-20-oil to 0-100-oil; (c) Tcc for 80-20-4468 to 0-100-4468; (d) Tcc for 80-20-oil to 0-100-oil; (e) Tm for 80-20-4468 to 0-100-4468 and (f) Tm for 80-20-oil to 0-100-oil.
Figure 6. DSC results in this study: (a) Tg for 80-20-4468 to 0-100-4468; (b) Tg for 80-20-oil to 0-100-oil; (c) Tcc for 80-20-4468 to 0-100-4468; (d) Tcc for 80-20-oil to 0-100-oil; (e) Tm for 80-20-4468 to 0-100-4468 and (f) Tm for 80-20-oil to 0-100-oil.
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Figure 7. FTIR results for all blends in function of two compatibilizers: (a) Joncryl® ADR 4468 and (b) ELO.
Figure 7. FTIR results for all blends in function of two compatibilizers: (a) Joncryl® ADR 4468 and (b) ELO.
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Figure 8. Rheological result curves for Joncryl® ADR 4468 batches: (a) storage modulus, (b) loss modulus, and (c) complex viscosity.
Figure 8. Rheological result curves for Joncryl® ADR 4468 batches: (a) storage modulus, (b) loss modulus, and (c) complex viscosity.
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Figure 9. Rheology results for all linseed oil batches: (a) storage modulus, (b) loss modulus, and (c) complex viscosity.
Figure 9. Rheology results for all linseed oil batches: (a) storage modulus, (b) loss modulus, and (c) complex viscosity.
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Figure 10. SEM images for blended batches: (a) 100-0-4468; (b) 100-0-oil; (c) 80-20-4468; (d) 80-20-oil; (e) 60-40-4468; (f) 60-40-oil; (g) 40-60-4468; (h) 40-60-oil; (i) 20-80-4468; (j) 20-80-oil; (k) 0-100-4468; (l) 0-100-oil.
Figure 10. SEM images for blended batches: (a) 100-0-4468; (b) 100-0-oil; (c) 80-20-4468; (d) 80-20-oil; (e) 60-40-4468; (f) 60-40-oil; (g) 40-60-4468; (h) 40-60-oil; (i) 20-80-4468; (j) 20-80-oil; (k) 0-100-4468; (l) 0-100-oil.
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Table 1. Characteristics for the raw materials used in this study.
Table 1. Characteristics for the raw materials used in this study.
CharacteristicsTPSPBS
Test MethodUnitValueTest MethodUnitValue
DensityISO 1183g/cm31.24ISO 1183g/cm31.26
Melt Flow IndexISO 1133g/10 min15 under 170 °C, 2.16 kgISO 1133g/10 min5 under 170 °C, 2.16 kg
Melting TemperatureISO 11357°C150–155ISO 3146°C115
Tensile Yield StressISO 527MPa26ISO 527-2MPa40
Young’s ModulusISO 527GPa1.7N/A
ElongationISO 527%4ISO 527-2%210
Izod Impact StrengthISO 180KJ/m22.5ISO 180KJ/m27
Table 2. Blended TPS/PBS compositions.
Table 2. Blended TPS/PBS compositions.
Component CompositionCompatibilizer
TPS (%)PBS (%)Joncryl® ADR 4468Linseed Oil
1000100-0-4468100-0-oil
802080-20-446880-20-oil
604060-40-446860-40-oil
406040-60-446840-60-oil
208020-80-446820-80-oil
01000-100-44680-100-oil
Table 3. Temperature employed in the compounding process.
Table 3. Temperature employed in the compounding process.
TPS Percentage of BlendZone 1Zone 2Zone 3Zone 4Zone 5Zone 6Zone 7Zone 8
100%, 80%, 60%110 °C135 °C180 °C180 °C190 °C190 °C190 °C190 °C
40%, 20%, 0%110 °C130 °C150 °C150 °C160 °C160 °C160 °C160 °C
Table 4. Injection molding parameters employed in this study.
Table 4. Injection molding parameters employed in this study.
CompositesTPSTPS80/PBS20TPS60/PBS40TPS40/PBS60TPS20/PBS80PBS
Conditions
Injection Speed (mm/s)80
Injection Pressure (bar)5601000
Holding Pressure
Base Point 1 (bar)450500
Base Point 2 (bar)450500
Switch Over Point (mm)1514
Circumferential Screw Speed (mm/s)170
Back Pressure (bar)40
Shot Size (mm)60
Cooling Time (second)50
Barrel Temperature (°C)
Zone 1140
Zone 2150
Zone 3160
Zone 4165
Nozzle165
Mold30
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MDPI and ACS Style

Gong, K.; Lu, Y.; Portela, A.; Farshbaf Taghinezhad, S.; Lawlor, D.; Connolly, S.; Hu, M.; Chen, Y.; Collins, M.N. A Comparative Study on the Compatibilization of Thermoplastic Starch/Polybutylene Succinate Blends by Chain Extender and Epoxidized Linseed Oil. Macromol 2025, 5, 24. https://doi.org/10.3390/macromol5020024

AMA Style

Gong K, Lu Y, Portela A, Farshbaf Taghinezhad S, Lawlor D, Connolly S, Hu M, Chen Y, Collins MN. A Comparative Study on the Compatibilization of Thermoplastic Starch/Polybutylene Succinate Blends by Chain Extender and Epoxidized Linseed Oil. Macromol. 2025; 5(2):24. https://doi.org/10.3390/macromol5020024

Chicago/Turabian Style

Gong, Ke, Yinshi Lu, Alexandre Portela, Soheil Farshbaf Taghinezhad, David Lawlor, Shane Connolly, Mengli Hu, Yuanyuan Chen, and Maurice N. Collins. 2025. "A Comparative Study on the Compatibilization of Thermoplastic Starch/Polybutylene Succinate Blends by Chain Extender and Epoxidized Linseed Oil" Macromol 5, no. 2: 24. https://doi.org/10.3390/macromol5020024

APA Style

Gong, K., Lu, Y., Portela, A., Farshbaf Taghinezhad, S., Lawlor, D., Connolly, S., Hu, M., Chen, Y., & Collins, M. N. (2025). A Comparative Study on the Compatibilization of Thermoplastic Starch/Polybutylene Succinate Blends by Chain Extender and Epoxidized Linseed Oil. Macromol, 5(2), 24. https://doi.org/10.3390/macromol5020024

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