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Article

Substitution of Fossil Layers with Biobased Ones in Sustainable Cellulosic Packaging for Dairy Products

by
Maria-Beatrice Coltelli
1,*,
Simone Giangrandi
2,
Vincenzo Tricoli
1,
Luca Panariello
1 and
Andrea Lazzeri
1
1
Department of Civil and Industrial Engineering, University of Pisa, 56122 Pisa, Italy
2
Lucense Scarl, 55100 Lucca, Italy
*
Author to whom correspondence should be addressed.
Appl. Sci. 2025, 15(17), 9615; https://doi.org/10.3390/app15179615 (registering DOI)
Submission received: 14 July 2025 / Revised: 12 August 2025 / Accepted: 27 August 2025 / Published: 31 August 2025
(This article belongs to the Special Issue Innovation in Dairy Products)
Browse Figures
Versions Notes

Abstract

Featured Application

These results hold relevance to the search for biobased and biocircular materials for dairy product packaging.

Abstract

Home-compostable, biobased films were developed by blending poly(lactic acid) (PLA) with poly(butylene succinate-co-adipate) (PBSA). Among the formulations, the PLA/PBSA 60/40 blend demonstrated strong potential for industrial film production due to its enhanced flexibility and tear resistance. Thanks to their thermoplastic nature, these films can be applied to various substrates—such as paper or paperboard—and are easily recyclable within industrial processing environments. In this study, nanostructured clay and talc were incorporated into PLA/PBSA 60/40-based films to produce composites, which were evaluated for their effectiveness in limiting the diffusion of moisture from high-humidity soft cheeses. The materials’ melt fluidity and tensile properties were also characterized, and the composite morphology was examined using electron microscopy. The results revealed that the filler type significantly affected both the morphological structure and barrier performance, highlighting the critical role of material composition in the development of effective and environmentally sustainable packaging solutions. The biobased PLA/PBSA (60/40) films, particularly those filled with talc, exhibited high processability, flexibility, and effectiveness as a moisture barrier for dairy packaging. Although not yet feasible as a direct LDPE substitute without increasing their thickness, their low mass loss points to their strong potential for sustainable applications—especially when paired with paperboard in rigid packaging.

1. Introduction

In recent decades, the need for innovative and sustainable packaging solutions for dairy products has become increasingly urgent [1,2,3]. Among the materials explored, cellulose has emerged as a promising candidate due to its recyclability, biodegradability, and renewability [4,5,6]. Several researchers and food industries have investigated and implemented cellulose-based packaging, particularly for dry or semi-moist dairy products [4,7,8] However, a significant limitation of cellulose is its poor resistance to moisture, which makes it unsuitable for packing high-moisture foods such as fresh tomatoes or soft cheeses [9,10]. To address this, recent advancements have focused on enhancing cellulose’s water resistance [11,12] and functionality [13,14,15]. Researchers developed an edible, biodegradable film by combining milk protein (casein) with plant-derived cellulose, offering a sustainable solution for moisture-sensitive dairy items [16]. Another research group created a multilayered composite film using bacterial cellulose, chitosan, and waterborne polyurethane, achieving both antimicrobial properties and improved water resistance, making it viable for wet foods [17]. Additionally, cellulose-based hydrogels are being explored for active packaging applications [18], such as moisture control and the gradual release of preservatives.
These innovations are paving the way for more versatile and eco-friendly packaging options, potentially expanding the use of cellulose even for challenging food categories.
Nowadays, the use of multilayer packaging for dairy products [19,20] is widespread on the market [21,22]. The paper or paperboard component represents the main weight of the packaging and provides essential mechanical properties—such as the flexibility of paper [23]-based packaging and the rigidity of board-based packaging. Moreover, the high cellulosic content contributes significantly to recyclability [24,25,26] since paper is typically recycled through repulping the shredded packaging in paper mills. However, the water barrier layers are generally provided by fossil-based polymers, such as polyethylene [27]. The current research is aiming to protect perishable foods by focusing on the development of novel multilayer systems composed of biobased and compostable polymers [28,29], along with paper or paperboard layers.
The use of renewable resources for all layers ensures that all of the packaging materials are carbon-neutral, thereby reducing their impact on climate change [30,31]. In addition, compostable packaging materials can be processed through suitable recycling steps prior to industrial composting, promoting a fully biocircular system and enhancing soil health [32].
However, the barrier properties of many biobased and biodegradable formulations still fall short of those offered by conventional fossil-based films, such as low-density polyethylene (LDPE). In this regard, systematic investigations of blending various biobased polyesters to produce films for use in multilayer cellulosic packaging to enhance its functional performance remain largely unexplored [33].
Recently, biobased and home-compostable films [34,35] have been developed by blending poly(lactic acid) (PLA) with poly(butylene succinate-co-adipate) (PBSA) [36]. In particular, the PLA/PBSA 60/40 blend demonstrated strong potential for industrial film production, offering improved flexibility [37], home compostability [34], and tearing resistance [38]. Thanks to their thermoplastic nature, these films can be applied to a variety of substrates and were found to be readily recyclable in industrial processing environments [39]. However, their barrier properties for packaging perishable liquid or semi-liquid foods have not yet been thoroughly investigated [40,41]. Due to its lamellar structure, talc has often been investigated as an additive for enhancing the barrier properties of bioplastic films [42,43], as has clay [44,45]. Both fillers possess a lamellar structure; however, talc is electrically neutral between its layers, while clay features negatively charged lamellae separated by interlayer cations. These contrasting characteristics highlight a fundamental difference in polarity between these two materials. In both cases, the dispersion of nanostructured inorganics into the polymeric matrix is an obstacle to the diffusion of small molecules [46,47].
In this study, aiming to develop and design packaging for dairy products with a short shelf life (2–10 days), composites containing clay and talc were prepared by dispersing these nanostructured fillers into PLA/PBSA (60/40) films. The effectiveness of these composites in limiting the diffusion of perishable dairy food components was evaluated. Additionally, the composites were analyzed for their melt fluidity. The results demonstrated that the selected composition significantly influenced the barrier properties of the films. These findings underscore the critical role of material composition in creating effective and environmentally sustainable packaging solutions.

2. Materials and Methods

2.1. The Production of the Materials

The PLA used in this paper was Total Corbion Luminy LX175 (Rayong, Thailand). The PBSA used in this paper was Mitsubishi BioPBS FD92PM (Tokyo, Japan). The talc used was ULTRA5c from Imifabi (Singapore), featuring an average particle diameter of 0.5 μm, with 75% of the particles measuring less than 1 μm. This product contains 99–100% talc by weight. Talc is made up of hydrous magnesium silicate, with its chemical composition represented by the formula Mg3Si4O10(OH)2. The clay was Cloisite 20A from BYK, comprising particles of which 50% had dimensions smaller than 10 microns. This product is an organically modified montmorillonite (MMT) clay, specifically a type of Cloisite Na+ modified with a quaternary ammonium salt, dimethyl dihydrogenated tallow ammonium cations. The blends and composites (Table 1) were prepared using a Haake Minilab II micro-compounder (Thermo Scientific Haake GmbH, Karlsruhe, Germany) (Figure 1a). After the introduction of the material, the melt, pushed by screws, ran through a closed circuit (with the valve closed) for 1 min. In the tests, the rotating speed was 100 rpm, and the processing temperature was 190 °C. T = 190 °C.

2.2. Characterization of the Materials

Investigation of the flow behavior was carried out using a CEAST Melt Flow Tester M20 (Instron, Canton, MA, USA) equipped with an encoder. The ISO1133D custom TTT was followed at 190 °C with a weight of 2.160 kg. Using the encoder, the melt volume rate (MVR) was recorded, and the melt flow rate (MFR) was determined by weighing the material. The standard deviation values for the MFR data were estimated from the standard deviation values of the MVR data multiplied for the melt density (MFR/MVR).
Two films were fabricated using a Noselab compression molding press at a pressure of 10 tons (about 9.5 bar) for 60 s. A total of 0.8 g of polymeric material was used for each film. After melt compression, the films were cooled using a compressed air flow (Figure 1b). With the same procedure, films made of low-density polyethylene of the same thickness were also produced. All of the films were characterized in terms of their average thickness, resulting in a narrow range of 72–77 μm.
The films were characterized through tensile tests. These tests were performed on rectangular 10 × 80 mm specimens cut from the films, avoiding the inclusion of bubbles or any defects. The useful length used was 40 mm (so of the initial 80 mm, 20 was blocked into the upper clamp and 20 mm into the lower clamp). The universal testing machine used was the INSTRON 5500R, equipped with a 100 N load cell and compressed air clamps. The test speed was 10 mm/min. The specimens were conditioned for at least 2 days in a climatic chamber at room temperature and 50% RH before testing. The tests were performed on 8 specimens for each sample.
The films were cryo-fractured in liquid nitrogen, and the fractured surfaces were coated with platinum via sputtering. A Scanning Electron Microscopy (SEM) analysis was then carried out using a FEI Quanta 450 FEG instrument (Graz, Austria). To carry out the barrier property tests, aiming to study their moisture retention, two films were produced for each formulation. The diameter of the films obtained was 13–14 cm. For each formulation, two films were sealed along three edges using a Cocoon sealing machine for packaging (Lissone, Italy). A predetermined quantity of fresh whey (kindly provided by Fruzzetti Dairy, Cascina, Pisa, Italy) was then introduced into the partially sealed container, after which point final sealing was performed (Figure 1c,d). The weight of the sealed samples (maintained at 4 °C) was measured using an analytical balance as a function of time for more than 30 days and compared to their initial weights. Each test was replicated, and the differences observed between the replicated results resulted in less than 0.3% (as an estimation of uncertainty).

3. Results and Discussion

The melt fluidity results indicated that the addition of clay led to a marked increase in melt fluidity, attributed to chain scission induced by hydrolysis of the polyester macromolecules—an effect previously reported by several authors [39,48] and attributed to the action of the transesterification catalyst of the Al alkoxide groups present in clay [49].
The inclusion of talc similarly resulted in increased fluidity (Table 2), although the measured values were lower, suggesting a less pronounced extent of degradation. Talc consists of stacked layers of silica tetrahedra and magnesium-containing octahedra, held together by weak van der Waals forces [50]. In contrast, clay is composed of negatively charged aluminosilicate layers that host exchangeable positive cations [51]. Due to these distinct structural features—particularly the presence of localized surface charges—the catalytic activity of clay in promoting chain scission in polyesters [52] can be more pronounced than that of talc.
When both fillers were used, the values observed were intermediate. These results can be explained by considering that while the fillers promote chain scission, they also reinforce the melt, thereby increasing the viscosity through interactions with the polymer matrix. In the composite containing both clay and talc, the higher filler content may counterbalance the increase in fluidity caused by degradation.
Since a reduction in molecular weight can influence the mechanical properties of polymeric materials, the tensile behavior of the films was evaluated. The mean values and standard deviations for breaking stress and breaking strain are reported in Table 3. In blends with a higher PLA content, talc was observed to increase the stress at break, indicating improved tensile strength of the film. However, a corresponding decrease in the strain at break suggested reduced ductility. Overall, talc demonstrated a reinforcing effect on the mechanical performance of the films, attributable to the better interaction with the polymeric matrix than that of clay.
The morphological analysis of the composites, conducted on cryo-fractured films (Figure 2), indicated that the talc particles were clearly distinguishable within the complex biphasic matrix of the blend—both in the formulation containing only talc and in that incorporating both talc and clay (as suggested by yellow circles). The talc lamellae appear well embedded into the matrix, suggesting good compatibility, consistent with the results of the tensile tests. In contrast, clay particles were more challenging to discern within the polymeric matrix, and no lamellae were observed. This likely points to greater difficulty in achieving exfoliation of the clay within the blend.
Table 4 reports the percentage of whey-related weight loss after 30 days, highlighting the barrier performance of the different packaging formulations. Certainly, the migrating molecule through the film is water in this system, and hence, the results depend on the intrinsic hydro repellence of the material constituting the film. The best behavior in terms of the barrier properties was shown by PLA/PBSA 60/40. The addition of fillers induced an increase in mass loss. This result can be attributed to the increased polarity of the film material, which, especially when clay is used, can favor the diffusion of water into the film.
It can be observed that the increase in the mass loss due to whey leakage is quite limited with the addition of talc or when both talc and clay are added. On the contrary, this increase is more significant when only clay is used. These results can be correlated with the data on the melt flow rate and melt volume rate and with the mechanical results too. The better interactions typical of talc with the biopolyester-based matrix result in greater inhibition of water diffusion through the film.
In Figure 3, the mass loss curves of the different samples as a function of time are compared. It is noticed that for up to two weeks, the behavior of PBSA/PLA 60/40 and the packaging containing talc almost entirely overlaps. On the contrary, the peculiarity of the curve obtained for the sample containing only clay is observed, which showed the highest mass loss.
Low-density polyethylene (LDPE) was considered a reference material for films adopted in packaging because of its high hydrorepellence and good flexibility. So, its behavior as packaging for whey was compared with that of the best-performing blend (Figure 4). After 30 days, the LDPE films showed a better performance in terms of their barrier properties. On the other hand, polyethylene is more hydrorepellent than a polyester blend.
Linear fitting of the experimental data considering the PLA/PBSA 60/40 film and the commercial LDPE film allowed equations correlating the time and the weight percentage to be obtained (Table 5), from which it was possible to calculate the mass loss at one week or 10 days. This is the current typical shelf life of this perishable product.
Although the PLA/PBSA composite exhibited lower humidity barrier properties compared to those of the commercial alternative, the mass loss observed after 7–10 days was considered acceptable for “primo sale” or “mozzarella” cheese. In fact, these are fresh cheeses characterized by a delicate flavor and soft texture. They are typically distributed through small, local shops, often located in the same regions as the farms and dairies where they are produced. This localized distribution reflects the strong connection between the product and its territory of origin, preserving traditional production methods and supporting short supply chains.
With the aim of exploiting the results obtained in the dairy sector, a packaging solution was designed and prototyped at the Centro Qualità Carta laboratory in LUCENSE (Figure 5). The prototype consisted of a rigid tray. This type of rigid packaging utilizes a commercially available cardboard approved for food contact. The prototype was created by applying a PLA/PBSA 60/40 biopolymer film to the inner surface of the tray and heat-sealing it to the substrate using pressure and temperature. Based on initial experimental tests, the optimal parameters ensuring good adhesion between the two materials were identified as 160 °C with 5 min of pressure application.

4. Conclusions

Different biobased film formulations were compared in terms of their processability, mechanical properties, and ability to limit the diffusion of the water-based liquids present in perishable dairy foods. A home-compostable and biobased PLA/PBSA (60/40) blend was used to prepare films and composites containing nanostructured clay and talc. The PLA/PBSA (60/40) blend demonstrated the best performance in terms of its melt fluidity, flexibility, and barrier properties against the leakage of whey.
However, the blend filled with talc—a layered, electrically neutral filler—exhibited even better processability, mechanical performance, and barrier properties than those of the neat biopolyester matrix. This unusual behavior suggests that the interaction between talc and biopolyesters (which are considered hydrophobic) is stronger compared to that for other fillers.
Overall, given that the best-performing material (the PLA/PBSA 60/40 blend) displayed inferior barrier properties compared to those of low-density polyethylene (LDPE), substituting LDPE with this biobased layer in multilayer packaging is currently not feasible—unless a greater film thickness is employed. This would, however, result in an increase in packaging weight.
Despite this notable limitation, the mass loss over one week remained very low, indicating potential for future applications in the packaging of fresh dairy products (such as mozzarella or primo sale), pending further testing. This would support the development of innovative materials aligned with environmentally friendly solutions.

Author Contributions

Conceptualization: M.-B.C. and L.P.; methodology: L.P.; investigation: M.-B.C. and S.G.; resources: S.G.; data curation: L.P. and M.-B.C.; writing—original draft preparation: M.-B.C. and V.T.; writing—review and editing: A.L. and S.G.; visualization: M.-B.C.; supervision: A.L.; project administration: S.G.; funding acquisition: S.G. All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by Regione Toscana, which supported the ProCaEcoPack project (Sotto-misura 16.2—Rural Development Programme 2014–2020 of GAL F.A.R. Maremma).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

The raw data supporting the conclusions of this article can be made available by the authors on request.

Acknowledgments

The Tuscany region is thanked for its support to the Pro CaEcoPack project (Call Sotto-misura 16.2 Rural Development Programme 2014–2020 of GAL F.A.R. Maremma).

Conflicts of Interest

The authors declare no conflicts of interest.

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Applsci 15 09615 g001
Figure 1. Preparation of the materials and examples of prepared samples: (a) recovery of the material by the mini extruder; (b) two films produced using the PLA/PBSA 60/40 blend through compression molding; (c) whey sealed into films made of PLA/PBSA 60/40; (d) whey sealed into films made by PLA7PBSA 60/40 + talc.
Figure 1. Preparation of the materials and examples of prepared samples: (a) recovery of the material by the mini extruder; (b) two films produced using the PLA/PBSA 60/40 blend through compression molding; (c) whey sealed into films made of PLA/PBSA 60/40; (d) whey sealed into films made by PLA7PBSA 60/40 + talc.
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Figure 2. SEM micrographs recorded of cryo-fractured surfaces of composite films.
Figure 2. SEM micrographs recorded of cryo-fractured surfaces of composite films.
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Figure 3. The percentage weight loss as a function of time for the different film packaging solutions tested.
Figure 3. The percentage weight loss as a function of time for the different film packaging solutions tested.
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Figure 4. A comparison between the percentage weight loss as a function of time for the best biobased film packaging solution tested and a low-density polyethylene film of the same thickness.
Figure 4. A comparison between the percentage weight loss as a function of time for the best biobased film packaging solution tested and a low-density polyethylene film of the same thickness.
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Figure 5. The prototype made with paperboard and PLA/PBSA 60/40 film.
Figure 5. The prototype made with paperboard and PLA/PBSA 60/40 film.
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Table 1. Composition of blends and composites prepared through mini extrusion.
Table 1. Composition of blends and composites prepared through mini extrusion.
SamplesPBSA (% by Weight)PLA (% by Weight)Talc (% by Weight)Clay (% by Weight)
PLA/PBSA 60/404060--
PLA/PBSA 60/40 + clay38.157.1-4.8
PLA/PBSA 60/40 + talc38.157.14.8-
PLA/PBSA 60/40 + talc + clay36.454.54.64.6
Table 2. Melt volume rate and melt flow rate results. The significance of the standard deviation was investigated using Student’s t test (p < 0.05). Means that were identified as not significantly different are grouped under the same letter.
Table 2. Melt volume rate and melt flow rate results. The significance of the standard deviation was investigated using Student’s t test (p < 0.05). Means that were identified as not significantly different are grouped under the same letter.
SamplesMVR (cm3/10 min)MFR (g/10 min)
PLA/PBSA 60/404.4 ± 0.1 a5.0 ± 0.2
PLA/PBSA 60/40 + clay37.9 ± 1.9 b42.1 ± 2.1
PLA/PBSA 60/40 + talc23.6 ± 2.1 c26.7 ± 2.3
PLA/PBSA 60/40 + talc + clay33.4 ± 1.1 d37.1 ± 1.2
Table 3. Results of tensile tests performed on films. The significance of the standard deviation was investigated using Student’s t test (p < 0.05). Means that were identified as not significantly different are grouped under the same letter.
Table 3. Results of tensile tests performed on films. The significance of the standard deviation was investigated using Student’s t test (p < 0.05). Means that were identified as not significantly different are grouped under the same letter.
SamplesTensile Strength (MPa)Strain at Break (%)
PLA/PBSA 60/4019.4 ± 4.5 a45.8 ± 10.3 a
PLA/PBSA 60/40 + clay18.6 ± 4.0 a5.8 ± 0.5 b
PLA/PBSA 60/40 + talc24.3 ± 2.1 b7.0 ± 0.4 c
PLA/PBSA 60/40 + talc + clay16.9 ± 4.6 a5.4 ± 0.5 b
Table 4. The average mass loss due to whey leakage after 30 days for the different films. The significance of standard deviation was investigated using Student’s t test (p < 0.05). Means that were identified as not significantly different are grouped under the same letter.
Table 4. The average mass loss due to whey leakage after 30 days for the different films. The significance of standard deviation was investigated using Student’s t test (p < 0.05). Means that were identified as not significantly different are grouped under the same letter.
PackagingMass Loss in 30 Days (%)
PLA/PBSA 60/409.7 a
PLA/PBSA 60/40 + clay16.4 c
PLA/PBSA 60/40 + talc10.9 b
PLA/PBSA 60/4 + talc + clay10.7 b
Table 5. Equations for the mass loss percentage as a function of time of whey packed in PLA/PBSA 60/40 and LDPE films, with the mass loss percentages calculated at 7 and 10 days.
Table 5. Equations for the mass loss percentage as a function of time of whey packed in PLA/PBSA 60/40 and LDPE films, with the mass loss percentages calculated at 7 and 10 days.
Packaging MaterialFitting EquationR2Loss at One WeekLoss at 10 Days
PLA/PBSA 60/40Y = −0.35679 X + 99.768240.999−2.73%−3.80%
LDPE (Commercial)Y = −0.04171 X + 100.03760.962−0.25%−0.38%
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MDPI and ACS Style

Coltelli, M.-B.; Giangrandi, S.; Tricoli, V.; Panariello, L.; Lazzeri, A. Substitution of Fossil Layers with Biobased Ones in Sustainable Cellulosic Packaging for Dairy Products. Appl. Sci. 2025, 15, 9615. https://doi.org/10.3390/app15179615

AMA Style

Coltelli M-B, Giangrandi S, Tricoli V, Panariello L, Lazzeri A. Substitution of Fossil Layers with Biobased Ones in Sustainable Cellulosic Packaging for Dairy Products. Applied Sciences. 2025; 15(17):9615. https://doi.org/10.3390/app15179615

Chicago/Turabian Style

Coltelli, Maria-Beatrice, Simone Giangrandi, Vincenzo Tricoli, Luca Panariello, and Andrea Lazzeri. 2025. "Substitution of Fossil Layers with Biobased Ones in Sustainable Cellulosic Packaging for Dairy Products" Applied Sciences 15, no. 17: 9615. https://doi.org/10.3390/app15179615

APA Style

Coltelli, M.-B., Giangrandi, S., Tricoli, V., Panariello, L., & Lazzeri, A. (2025). Substitution of Fossil Layers with Biobased Ones in Sustainable Cellulosic Packaging for Dairy Products. Applied Sciences, 15(17), 9615. https://doi.org/10.3390/app15179615

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