Search Results (277)

The development of fully biodegradable poly(3-hydroxybutyrate) (PHB)-based materials with improved mechanical performance remains a major challenge due to the limited ductility and processability of this highly crystalline polymer. Blending and plasticisation are viable strategies to enhance PHB toughness; however, the interactions governing polymer–plasticiser compatibility and their impact on structure–property relationships remain not fully understood. In this work, the compatibility and plasticisation mechanisms of two citrate-based plasticisers, tributyl citrate (TBC) and acetyl tributyl citrate (ATBC), were systematically investigated in biodegradable blends based on PHB, polylactic acid (PLA), and poly(butylene adipate-co-terephthalate) (PBAT). Polymer–plasticiser affinity was evaluated through Hansen Solubility Parameters and interaction radius, which indicated good compatibility of PHB with both plasticisers and a stronger affinity for ATBC. Differential scanning calorimetry showed that citrate plasticisers reduced the glass transition temperature, modified crystallisation kinetics, and altered the crystalline morphology of the blends. Dynamic mechanical analysis confirmed the reduction in the glass transition temperature of PHB–PLA systems, which is in agreement with the DSC results. Migration experiments showed equilibrium after approximately 72 h, with PHB–PLA blends exhibiting better plasticiser retention than PHB–PBAT systems. TBC consistently showed higher migration than ATBC, in line with its lower molecular weight and higher volatility. Mechanical testing demonstrated that plasticisation efficiency strongly depended on blend composition: TBC was more effective in enhancing ductility in PHB–PLA blends, whereas ATBC performed better in PHB–PBAT systems. It was also highlighted that the plasticisers had a remarkable ability to substantially increase the ductility of the blends compared with their unplasticised counterparts, as reflected by the pronounced decrease in stiffness and the marked increase in elongation at break. SEM analysis of tensile fracture surfaces evidenced a brittle failure mode for PHB–PLA blends, whereas PHB–PBAT systems exhibited a ductile fracture mode with fibrillar features and clear signs of phase separation. Finally, thermogravimetric analysis showed no appreciable thermal degradation within the processing temperature window used for mixing and hot pressing, confirming the thermal stability of the materials under the selected conditions. These findings establish clear correlations between thermodynamic compatibility, migration behaviour, thermal properties, fracture mechanisms, and mechanical performance, providing useful guidelines for the design of citrate-plasticised PHB-based biodegradable materials. Full article

Microplastics (MPs) and pesticides increasingly co-occur in agricultural ecosystems, where they may jointly affect plant physiology and plant–microorganism interactions. This study investigated the individual and combined effects of biodegradable poly(butylene adipate-co-terephthalate) (PBAT), the herbicide metolachlor (MET), and the beneficial fungus Trichoderma harzianum KKP 534 on wheat (Triticum aestivum). Plant growth, physiological responses, chlorophyll content, cell membrane damage, antioxidant enzyme activities and selected metabolomic and lipidomic biomarkers were evaluated. High PBAT concentrations negatively affected wheat growth by reducing root and shoot length and increasing oxidative stress, as evidenced by elevated TBARS levels, increased antioxidant enzyme activities (POD, GST, CAT, and SOD), and enhanced membrane damage. Metabolomic and lipidomic analyses further revealed stress-associated changes in amino acid metabolism and membrane lipid remodelling. PBAT also adsorbed MET and 2,4-di-tert-butylphenol (DTBP), potentially altering their bioavailability and environmental behaviour. Although T. harzianum KKP 534 promoted plant growth and enhanced antioxidant responses under control conditions, these beneficial effects were attenuated in the presence of PBAT MP. The results suggest that biodegradable microplastics may influence plant–microbe interactions and modify pesticide dynamics under controlled conditions, highlighting the need for further studies in soil-based systems. Full article

Acute or chronic rotator cuff tears are major causes of shoulder dysfunction, motivating the development of scaffolds with tailored thickness and mechanics for supraspinatus tendon regeneration. This study aimed to investigate the effect of bilayer poly(butylene adipate-co-terephthalate) (PBAT) scaffold thickness on the tenogenic differentiation of rat adipose mesenchymal stem cells (r-AdMSCs) and supraspinatus tendon regeneration. Aligned fibers with a diameter of approximately 476 nm were deposited onto randomly oriented layers at different times (4 h; 4S, 6 h; 6S, 8 h; 8S), and scaffolds with increasing thicknesses from 441 µm (4S) to 1132 µm (8S) were produced. Mechanical testing showed comparable tensile strength for 4S and 6S (≈1.9–2.0 MPa) and modulus (5.5–7.3 MPa), while 8S exhibited markedly reduced stiffness (0.5 MPa) and hyper elastic deformation. Mechanical performance across degradation conditions remained strongly thickness-dependent: thinner scaffolds retained integrity and strengthened, with modulus increases during hydrolytic and enzymatic degradation, whereas thicker matrices showed limited remodeling and instability. Rat-AdMSCs’ were cultured on the scaffolds for 21 days. Cell-free and cell-laden mechanical responses further reflected thickness effects: cell-free samples stiffened due to media-induced passive matrix tightening, whereas cell-laden scaffolds showed extracellular matrix (ECM)-driven reinforcement, most prominently in 4S, which reached 2.1 MPa tensile strength with improved elasticity and balanced deformation. The 4S scaffold exhibited the highest tensile strength and significantly increased collagen-1 (col1), tenomodulin (tnmd) and scleraxis (scx) expression compared with the other groups. In conclusion, among all groups, 4S scaffolds demonstrated the most favorable mechanical and biological performance, suggesting that scaffold thickness plays a critical role in regulating tendon regeneration and will become even more suitable when matured in bioreactors. Full article

Biopolymers (BPs), obtained from urban and agricultural wastes, are known as active principles to manufacture ready-for-use finished products in several sectors of the agriculture and chemical industries. These findings prospect a biowaste-based refinery producing chemical specialities to replace products derived from fossil feedstock. The present paper reports new materials containing BPs. Composite granules containing Poly(Butylene Adipate-Co-Terephthalate (PBAT) as a matrix and BPs as fillers are manufactured by twin-screw extrusion. The granules are used to make single-layer PBAT-BP mulch films by single-screw extrusion and three-layer Starch-PBAT-BP films by blown co-extrusion. The films are tested for mechanical properties, and for structural stability and effects in the in vitro cress germination and the in-field horticulture. The results show that both the films’ effects on plant performance and the films’ structural degradation are regulated by the BP and polymeric matrix release kinetics in the operational germination medium or the field soil, and in turn, that the kinetics depend on the mulch film structural features. The horticulture trials prove that the three-layer mulch films have adequate mechanical strength (25 MPa maximum tensile strength and 520% elongation at break) and about 6 months lifespan to maintain and/or improve the soil protection and crop production (17 t/ha) over the plant seasonal cycle. These findings widen the range of renewable chemical specialities potentially producible by the envisioned biowaste-based refinery. Full article

Multilayer packaging—engineered by integrating complementary materials such as plastics, paper, and aluminum—has become a cornerstone technology for enhancing shelf life, minimizing spoilage, and reinforcing the mechanical integrity of packaging formats including films, pouches, and bottles. In this study, a laminate was developed by thermally bonding polylactic acid (PLA) with a poly(butylene adipate-co-terephthalate) (PBAT)/thermoplastic starch (TPS) matrix embedded with silver nanoparticles (Ag-NPs) at 0–3 wt.%. The resulting structures were systematically evaluated for their barrier performance, physicochemical characteristics, and antimicrobial functionality. Fourier-transform infrared (FTIR) spectroscopy confirmed the absence of chemical interactions between Ag-NPs and the polymer matrix, indicating physical dispersion rather than chemical bonding. However, at higher loading (3 wt.%), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDX) revealed notable nanoparticle aggregation. Functionally, the multilayer films demonstrated markedly improved water vapor barrier properties compared to single-layer PBAT/TPS films. Migration studies showed that silver release increased with nanoparticle concentration and was significantly enhanced under acidic conditions relative to distilled water. Importantly, Ag-NP-incorporated laminates exhibited pronounced antibacterial activity against Staphylococcus aureus. Collectively, these findings highlight the potential of Ag-NP-enriched, starch-based multilayer laminates as next-generation active packaging systems that combine with effective microbial control. Full article

The growing demand for sustainable food packaging has intensified interest in biodegradable materials that can reduce environmental impact while preserving food quality. Among these materials, biodegradable polyester–starch composite films functionalized with phenolic compounds have gained attention as promising active packaging systems. They combine the melt processability and structural stability of polyesters, such as poly(lactic acid) (PLA), poly(butylene adipate-co-terephthalate) (PBAT), poly(butylene succinate) (PBS), and poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) with the renewability and biodegradability of starch and the antioxidant, antimicrobial, and UV-protective functions of phenolics, such as ferulic acid, quercetin, tea polyphenols, and anthocyanins. This review discusses recent advances in the selection of biodegradable polyesters, starch and thermoplastic starch blending, phenolic incorporation strategies, and their effects on compatibility, morphology, mechanical strength, barrier properties, optical behavior, release, and active packaging functionality. The characteristics and functionality of these films are governed not only by the individual components but also by phase morphology, interfacial interactions, phenolic location, processing conditions, and release control. Key challenges include polyester–starch incompatibility, TPS moisture sensitivity, phenolic stability during melt processing, migration safety, controlled release, and industrial scale-up. Collectively, biodegradable polyester–starch films functionalized with phenolic compounds represent a promising route for developing next-generation sustainable active packaging and may contribute to circular economy approaches. Full article

Improving the interfacial compatibility between cellulose and poly(butylene adipate-co-terephthalate) (PBAT) is critical for enhancing the performance of PBAT-based composites. Here, microcrystalline cellulose (MCC) was homogeneously silanized at the molecular chain level using t-hexyldimethylchlorosilane (TDMS-Cl) as the modifier, yielding t-hexyldimethylsilylated cellulose (TDMS-Cell). TDMS-Cell/PBAT composite films were then prepared by solution blending and casting in tetrahydrofuran (THF). Structural characterizations confirmed the successful grafting of TDMS-Cl onto cellulose chains, resulting in TDMS-Cell with a degree of substitution of approximately 2. Microstructural observations combined with thermal analysis revealed that TDMS-Cell exerted a dual effect on the crystallization behavior of PBAT: it acted as a heterogeneous nucleating agent that increased the crystallization temperature, while the pronounced steric hindrance simultaneously suppressed crystal growth. Mechanical testing showed that simultaneous strengthening and toughening were achieved at an optimal TDMS-Cell loading of 3–5 wt%. Specifically, the tensile strength increased from ~16 MPa for neat PBAT to 21 MPa (31.25% improvement), and the elongation at break increased from ~700% to 964% (37.7% improvement). In addition, the incorporation of an appropriate amount of TDMS-Cell effectively enhanced the surface hydrophobicity of the composite films. At higher filler loading, however, solvent evaporation-induced phase separation led to self-aggregation of TDMS-Cell, which in turn deteriorated both the mechanical properties and surface hydrophobicity of the composites. Overall, this work systematically elucidates the structure–property relationships of silanized cellulose/PBAT composites in a homogeneous solution system, providing a rational basis for interfacial design and property optimization of PBAT/biomass-based composite materials. The prepared TDMS-Cell/PBAT composite films with balanced mechanical strength, tunable crystallization behavior, and improved surface hydrophobicity exhibit great potential for practical applications in high-performance flexible packaging materials, functional film substrates, lightweight composite structural components, and tunable hydrophobicity coating substrates. Full article

Plastic pollution from packaging waste is driving the development of biodegradable composites for sustainable packaging. In this work, poly(butylene adipate-co-terephthalate)/poly(3-hydroxybutyrate) (PBAT/PHBH) blends (50/50 wt.%) were reinforced with agro-industrial waste fillers—spent coffee grounds (SCG), brewer’s spent grain (BSG), and cellulose powder (CP)—at 1–15 wt.% loading. The effects of these fillers on tensile properties, impact strength, and thermal stability were examined and supported by scanning electron microscopy (SEM) of fracture surfaces and thermogravimetric analysis (TGA). The neat PBAT/PHBH blend exhibited balanced stiffness and ductility. Low BSG loadings (≤5 wt.%) produced the greatest toughening, with impact strength increasing by ~92% and elongation at break significantly improving over the neat blend. SEM analysis indicated crack deflection and particle pull-out as dominant energy-dissipation mechanisms at low BSG loading. At higher BSG loading (15 wt.%), particle clustering and larger voids acted as stress concentrators, reducing impact performance. SCG improved ductility at low loading (1 wt.%), whereas increasing SCG content led to progressive reductions in tensile strength and elongation due to increased debonding and microvoid formation. In contrast, CP exhibited minimal reinforcement efficiency within the investigated range (1–5 wt.%). Overall, filler addition generally reduced tensile strength and, in several cases, tensile modulus, reflecting limited interfacial compatibility between the hydrophilic lignocellulosic fillers and the hydrophobic polyester matrix. TGA indicated a modest improvement in thermal stability at higher BSG loadings, reflected by shifts in T_5% and T_max1 (PHBH) toward higher temperatures. Overall, this study demonstrates that upcycled coffee and beer waste fillers can impart specific toughness benefits to biodegradable PBAT/PHBH blends, but interfacial incompatibility currently limits their reinforcement efficiency. The findings highlight the potential and challenges of these biocomposites for sustainable packaging applications and suggest that interface engineering (e.g., compatibilizers) will be key to unlocking optimal performance. Full article

This study investigates the effects of organic salts, including sodium citrate (SC), calcium citrate (CC), and calcium lactate (CL), on the structure–property–function relationships of thermoplastic starch/poly(butylene adipate-co-terephthalate) (TPS/PBAT) films for active packaging applications. TPS incorporated with organic salts was prepared via twin-screw extrusion, blended with PBAT, and further processed into blown films. The films were systematically characterized using ¹H NMR, FTIR, and SEM, together with optical, mechanical, water vapor permeability, and antimicrobial evaluations against Staphylococcus aureus. The results revealed that SC primarily modulated hydrogen-bonding interactions within the starch matrix, resulting in improved structural homogeneity, balanced mechanical properties, and the highest antimicrobial activity among all formulations. In contrast, CL and CC promoted ionic crosslinking through Ca²⁺–starch interactions, leading to increased stiffness and Young’s modulus but reduced polymer chain mobility and limited release of active species, particularly in CC-containing systems. These differences in molecular interactions were consistent with variations in film microstructure, where SC-containing films exhibited more uniform morphologies, while calcium-based systems showed denser but less permeable structures. Furthermore, films containing SC and CL at appropriate concentrations achieved a favorable balance between transparency, water vapor barrier properties, and antimicrobial performance. Overall, this study provides new mechanistic insights into how monovalent and divalent organic salts govern intermolecular interactions, microstructure, and functional performance in TPS/PBAT systems. The findings highlight the critical role of additive type and concentration in designing biodegradable active packaging materials with tunable mechanical, barrier, and antimicrobial properties. Full article

We investigated the synthesis and characterization of biodegradable films composed of poly (lactic acid) (PLA) and poly(butylene adipate-co-terephthalate) (PBAT), with lignin as a natural additive and dicumyl peroxide (DCP) as a compatibilizer. The PLA/PBAT ratio of 70:30 was optimized and the DCP was incorporated at different concentrations to enhance interfacial adhesion. The effects of lignin addition (0.005–0.02%) on the mechanical, thermal, and biodegradation properties were evaluated using SEM, FTIR, XRD, and TGA analyses. The optimal formulation had improved tensile strength, elongation at break, and thermal stability, with the highest degradation rate of 44.22% after 90 days of soil burial. Life cycle assessment using SimaPro software (SimaPro 9.1.1.1) and ReCiPe 2016 Midpoint indicated that the film containing 0.005% lignin had the lowest environmental impact. The primary environmental concerns were marine and freshwater ecotoxicity, associated with solvent use. Based on the results, incorporating small amounts of lignin enhanced the biodegradability and reduced the environmental footprint of the PLA/PBAT films, highlighting their potential for sustainable packaging applications. Full article

Corn starch (CS)/poly (butylene adipate-co-terephthalate) (PBAT) blends were prepared by extrusion and injection molding processes. The CS content in the blends changed between 0 and 50 wt.% in 10 wt.% steps. Melt flow rates, mechanical properties, thermal stability, melting and crystallization behavior, as well as hydrophilicity of the blends were investigated. Based on these, the degradation properties of PBAT and the blend containing 50 wt.% CS (50%CS/PBAT) in water and open-air storage were comparatively studied via visual appearance observation, Shore hardness testing, and water absorption measurement. The results showed that the melt flow rates and the mechanical properties of the blends, including the tensile strength, tensile modulus, impact strength, and elongation at break, initially increased before decreasing as CS content in the blends increased, while the flexural strength and flexural modulus of the samples increased monotonously. The sample would become more thermal unstable when more CS was used. Besides these, the crystallinity and water contact angle became smaller. Immersion in water would blacken the visual appearances of PBAT and 50%CS/PBAT samples, but cracks could be found much more obviously in the blend than in neat PBAT; both the hardness and the mass of PBAT rose slightly while those of 50%CS/PBAT dropped significantly. An open-air storage would also blacken the visual appearances of PBAT and 50%CS/PBAT, and the hardness of the two samples would be decreased to almost the same extent. The results showed that the incorporation of CS in PBAT had much greater effects on the flow ability, mechanical properties, thermal stability, melt and crystallization behavior, as well as hydrophilicity of the blends. Immersion in water or being placed in air could accelerate the degradation of 50%CS/PBAT much more seriously than PBAT. Compared with PBAT, 50%CS/PBAT was of much lower cost and easier to be degraded, especially in water; it should be an ideal degradable blend for applications in packaging, agricultural mulch, and some other areas. Full article

The commercialization of poly(butylene succinate-co-adipate) (PBSA), a biodegradable and potentially fully biobased random copolyester, is still ongoing. Due to its high relevance as mono material or as blend component in flexible film applications, a sound understanding of compounding, further processing and film properties is necessary. In this work, PBSA, poly (lactic acid) (PLA) and blends at three different compositions thereof were processed into flat films and blown films, respectively. Investigating the films with X-ray diffraction (XRD), multivariate confocal Raman microscopy (CRM) and scanning electron microscopy (SEM) revealed the semicrystalline order as well as the blend morphology. While PBSA is semicrystalline, PLA remains amorphous after the processing step. As imaged by CRM, flat films exhibit lamellar-like domains formed during uniaxial stretching and rapid cooling, whereas blown films show no pronounced preferential orientation. Tensile tests in both the machine and transverse directions demonstrate the versatility of PBSA and its blends in spanning a wide range of mechanical strength and flexibility, covering and partly exceeding the stiffness and strength ranges typically reported for commodity polyolefins while exhibiting reduced ductility. Differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA) provide further insights into the thermal properties of the pure and blend materials. Full article

This study presents the effect of gamma rays of up to 2000 kGy on the chemical structure and the physical properties of a poly(butylene adipate-co-terephthalate) (PBAT) with 48% mol of terephthalic units. PBAT is a polymer with properties similar to polyethylene (PE) but it is biodegradable and not toxic to the environment, and it can be prepared with a renewable content of up to 68.6% weight, with uses in biomedicine and packaging. Previous studies found in the literature have been conducted using low doses and the results were contradictory. The results for gel content and crosslinking efficiency were in agreement with the results found in the literature. Molecular weight decreased and widened with the increase in dose. Proton NMR analysis was used for the first time in PBAT to determine the changes in chemical species, the formation of new chemical species, and the bonds more susceptible to be broken by gamma rays. Both thermal and mechanical properties were explained by the scission of the chains in the amorphous phase and at the boundaries of the crystallites. The thermal parameters most affected by irradiation were the crystallization temperature and temperature of melting after cooling from the melt. Stress and strain at break suffered a continuous decrease with dose until PBAT became fragile at high dose. Full article

In this work, compatibilized poly(lactic acid)/poly(butylene adipate-co-terephthalate) (PLA/PBAT) blends were developed and characterized, to be potentially utilized as biodegradable self-healing matrices for composite laminates. Blends containing 10, 20 and 30%wt of PBAT and 0.5 phr of an epoxy-based compatibilizer were prepared by melt compounding and hot pressing. Rheological measurements showed that moduli and complex viscosity generally increased with PBAT content, while maintaining viscosity levels suitable for conventional melt-processing operations. FT-IR and FESEM analyses confirmed the formation of an immiscible but well-compatibilized morphology, characterized by a homogeneous dispersion of PBAT domains within the PLA phase. Mechanical tests revealed a decrease in tensile modulus (up to 44%), strength (up to 45%) and fracture toughness (up to 40%) with a PBAT content up to 30%wt. Self-healing was evaluated by measuring the fracture toughness (K_IC) recovery after thermal treatment at 140 °C. After healing, the blend containing 20%wt of PBAT exhibited a self-healing efficiency of 64% under impact conditions, which was attributed to the smoother fracture surface generated at an elevated strain rate that facilitated a more effective flow of the molten PBAT phase across the crack interface during healing. The formulation containing 20%wt of PBAT featured the best balance between mechanical performance and self-healing efficiency. Full article

Cellulose nanocrystals (CNCs) possess outstanding mechanical properties and sustainability; however, their hydrophilic nature makes their dispersion challenging in hydrophobic bioplastic matrices. Surface modification of CNC is therefore inevitable for effective nanocomposite fabrication. In this study, CNC surface was modified using a green, water-based grafting-from method, enabling the growth of poly(2-hydroxyethyl methacrylate) (PHEMA) chains directly from its surface. This modification decreases intermolecular hydrogen bonding among CNCs and enhances their compatibility with poly(butylene adipate-co-terephthalate) (PBAT), a commercially available biodegradable aliphatic–aromatic copolyester widely used in sustainable packaging applications. The enhanced interfacial interaction arises from both the improved dispersion of CNCs within the PBAT matrix and the ability of PHEMA’s hydroxyl groups to form secondary interactions with PBAT. To examine how grafted polymer chain length influences CNC dispersion, PHEMA was grown from CNC surfaces at different grafting degrees. Additionally, PHEMA homopolymers were synthesized and melt-mixed with PBAT to evaluate the role of PHEMA in the absence of CNC. Neat and modified CNCs (mCNCs) were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, water contact angle measurements, wettability tests, and thermogravimetric analysis. Nanocomposites containing 3 wt% neat CNCs, mCNCs, or PHEMA homopolymers were subsequently prepared using an internal melt mixer. Melt rheology, differential scanning calorimetry, and dynamic mechanical analysis were then used to characterize the final viscoelastic and thermomechanical behavior of the resulting nanocomposites. The increased storage modulus and complex viscosity of the nanocomposites confirmed that the CNCs grafted with an intermediate PHEMA chain length exhibited improved network formation and enhanced interfacial interaction with PBAT. Full article