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Biobased Polymers for Packaging Applications
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Biobased Polymers for Packaging Applications

A special issue of Materials (ISSN 1996-1944).

Deadline for manuscript submissions: closed (30 June 2017) | Viewed by 106785

Special Issue Editor

Dr. Valentina Siracusa

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Guest Editor
Department of Chemical Sciences, Università degli Studi di Catania, 95125 Catania, Italy
Interests: polyesters; synthesis; chemical modification; thermal properties; mechanical properties; barrier properties; biodegradability; food packaging; active packaging; diffusion; permeability; bio-based and biodegradable polymers; polymers from waste; nanocomposites; biocomposites; life cycle assessment
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Special Issue Information

Dear Colleagues,

In recent years, both academic and industrial research in the field of plastic packaging has been strongly oriented towards green routes. The growing concerns of consumers regarding global warming and environmental legislation and regulation are even more propelling for the development of environmentally-friendly materials with a low carbon footprint, are increasingly encouraging research in green chemistry. In this case, it becomes imperative to decrease the demands for resources and energy, control waste, minimize gas emissions, reduce environmental pollution, optimize product processes, and, finally, make waste recycling effective. One interesting route is to utilize renewable monomers, coming from renewable feedstocks, which are polymerized with conventional melt or gas phase processes. Obtained bio-based polymers have advantages with respect to low carbon footprint materials, with recycling possibilities, obtained using energy-effective solvent free polymerization processes. In order to avoid conflict with food production, feedstock monomers, coming from agricultural and forestry wastes, are preferred. For example, lignocelluloses and starch could be used to produce a large variety of bio-based monomers, such as aliphatic hydrocarbons (ethylene, propylene, butylene, etc.), diols (ethylene glycol, 1,3-propanediol, 1,4-butanediol, etc.), diacids (succinic acid, sebacic acid, terephthalic acid, etc.), hydroxyalkanoic acids (lactic acid, hydroxybutyric acid, etc.), and furans (2,5-furandicarboxylic acid, etc.), which can be readily used in a polymerization process to produce bio-based polymers. Between them, furanoates polyesters have attracted a great deal of attention. When 2,5-furandicarboxylic acid was included in the ten bio-based chemicals list, this monomer was taken into consideration as a potential replacement for terephthalic acid, a widely monomer used for the production of polyethylene terephthalate (PET) and polybutylene terephthalate (PBT) polymers.

The progress achieved during the last few years could help researchers to work on fully bio-based polymers, in order to obtain new materials with real competitive properties relative to their oil-based counterparts. Some challenges could be the production of raw bio-based monomers in bulk quantities, the production of high quality bio-based polymers while controlling the cost–property ratio. Furthermore, the synthesis of bio-based polymers and copolymers with biodegradable features is also an interesting field of study to be addressed by the scientific community.

Prof. Valentina Siracusa
Guest Editor

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Keywords

  • Food packaging
  • Bio-based monomers
  • Bio-based polymers
  • Biopolymers
  • renewable sourcing
  • renewable plastics
  • gas barrier properties
  • bio-based polyesters
  • bio-based polyolefins
  • sustainable features
  • Furanoate polymers
  • Furanoate copolymers
  • 2,5-furandicarboxylic acid
  • Poly(ethylene 2,5-furandicarboxylate)
  • Poly(propylene 2,5-furandicarboxylate)
  • Poly(alkylene 2,5-furandicarboxylate)

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Published Papers (11 papers)

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Research

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15 pages, 1669 KiB  
Article
Poly(Neopentyl Glycol Furanoate): A Member of the Furan-Based Polyester Family with Smart Barrier Performances for Sustainable Food Packaging Applications
by Laura Genovese, Nadia Lotti, Valentina Siracusa and Andrea Munari
Materials 2017, 10(9), 1028; https://doi.org/10.3390/ma10091028 - 4 Sep 2017
Cited by 66 | Viewed by 7151
Abstract
In the last decade, there has been an increased interest from the food packaging industry toward the development and application of bioplastics, to contribute to the sustainable economy and to reduce the huge environmental problem afflicting the planet. In the present work, we [...] Read more.
In the last decade, there has been an increased interest from the food packaging industry toward the development and application of bioplastics, to contribute to the sustainable economy and to reduce the huge environmental problem afflicting the planet. In the present work, we focus on a new furan-based polyester, poly(neopentyl glycol 2,5-furanoate) (PNF) to be used for sustainable food packaging applications. The aromatic polyester was successfully synthesized with high molecular weight, through a solvent-free process, starting directly from 2,5-furandicarboxylic acid. PNF was revealed to be a material with good thermal stability, characterized by a higher Tg and Tm and a lower RAF fraction compared to poly(propylene 2,5-furanoate) (PPF), ascribable to the two methyl side groups present in PNF glycol-sub-unit. PNF’s mechanical characteristics, i.e., very high elastic modulus and brittle fracture, were found to be similar to those of PPF and PEF. Barrier properties to different gases, temperatures and relative humidity were evaluated. From the results obtained, PNF was showed to be a material with very smart barrier performances, significantly superior with respect to PEF’s ones. Lastly, PNF’s permeability behavior did not appreciably change after contact with food simulants, whereas it got worse with increasing RH, due to the polar nature of furan ring. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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18 pages, 1379 KiB  
Article
How Stress Treatments Influence the Performance of Biodegradable Poly(Butylene Succinate)-Based Copolymers with Thioether Linkages for Food Packaging Applications
by Valentina Siracusa, Laura Genovese, Andrea Munari and Nadia Lotti
Materials 2017, 10(9), 1009; https://doi.org/10.3390/ma10091009 - 30 Aug 2017
Cited by 8 | Viewed by 5067
Abstract
Biodegradable poly(butylene succinate) (PBS)-based random copolymers containing thioether linkages (P(BSxTDGSy)) of various compositions have been investigated and characterized from the gas barrier, thermal, and mechanical point of view, after food contact simulants or thermal and photoaging processes. Each stress treatment was performed on [...] Read more.
Biodegradable poly(butylene succinate) (PBS)-based random copolymers containing thioether linkages (P(BSxTDGSy)) of various compositions have been investigated and characterized from the gas barrier, thermal, and mechanical point of view, after food contact simulants or thermal and photoaging processes. Each stress treatment was performed on thin films and the results obtained have been compared to the same untreated film, used as a standard. Barrier properties with different gases (O2 and CO2) were evaluated, showing that the polymer chemical composition strongly influenced the permeability behavior. The relationships between the diffusion coefficients (D) and solubility (S) with polymer composition were also investigated. The results highlighted a correlation between polymer chemical structure and treatment. Gas transmission rate (GTR) mainly depending on the performed treatment, as GTR increased with the increase of TDGS co-unit amount. Thermal and mechanical tests allowed for the recording of variations in the degree of crystallinity and in the tensile properties. An increase in the crystallinity degree was recorded after contact with simulant liquids and aging treatments, together with a molecular weight decrease, a slight enhancement of the elastic modulus and a decrement of the elongation at break, proportional to the TDGS co-unit content. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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17 pages, 1941 KiB  
Article
Effect of Pullulan Coating on Postharvest Quality and Shelf-Life of Highbush Blueberry (Vaccinium corymbosum L.)
by Karolina Kraśniewska, Iwona Ścibisz, Małgorzata Gniewosz, Marta Mitek, Katarzyna Pobiega and Andrzej Cendrowski
Materials 2017, 10(8), 965; https://doi.org/10.3390/ma10080965 - 18 Aug 2017
Cited by 48 | Viewed by 7289
Abstract
Fruits form an important part of a healthy human diet as they contain many ingredients with proven pro-health effects such as vitamins, phenolic compounds, organic acids, fiber, and minerals. The purpose of this work was to evaluate the effect of pullulan coating on [...] Read more.
Fruits form an important part of a healthy human diet as they contain many ingredients with proven pro-health effects such as vitamins, phenolic compounds, organic acids, fiber, and minerals. The purpose of this work was to evaluate the effect of pullulan coating on the quality and shelf life of highbush blueberry during storage. General appearance, weight loss, dry matter, soluble solid content, reducing sugars, content of L-ascorbic acid, phenolic compounds (total phenolics, phenolics acids and anthocyanins) were determined in uncoated and coated blueberries fruits. The microbiological efficiency of pullulan coating was also evaluated. All parameters were monitored during storage at 4 °C and 16 °C by 28 and 14 days, respectively. The study showed that pullulan coating protects perishable food products especially susceptible to mechanical injury including fruits such as blueberries. Pullulan acts as a barrier that minimizes respiration rate, delaying deterioration and controlling microbial growth. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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22 pages, 2003 KiB  
Article
Performance of Poly(lactic acid) Surface Modified Films for Food Packaging Application
by Valentina Siracusa, Marco Dalla Rosa and Alexey L. Iordanskii
Materials 2017, 10(8), 850; https://doi.org/10.3390/ma10080850 - 25 Jul 2017
Cited by 17 | Viewed by 5767
Abstract
Five Poly(lactic acid) (PLA) film samples were analyzed to study the gas barrier behavior, thermal stability and mechanical performance for food packaging application. O2, CO2, N2, N2O, and C2H4 pure gases; Air; [...] Read more.
Five Poly(lactic acid) (PLA) film samples were analyzed to study the gas barrier behavior, thermal stability and mechanical performance for food packaging application. O2, CO2, N2, N2O, and C2H4 pure gases; Air; and Modified Atmosphere (MA, 79% N2O/21% O2) were used to analyze the influence of the chemical structure, storage temperature and crystalline phase on the gas barrier behavior. The kinetic of the permeation process was investigated at different temperatures, ranging from 5 °C to 40 °C. Annealing thermal treatment on the samples led to the crystalline percentage, influencing especially the gas solubility process. Thermal properties such as Tg and χc, and mechanical properties such as tensile strength and modulus were remarkably improved with surface PLA modification. A more pronounced reinforcing effect was noted in the case of metallization, as well as improved gas barrier performance. Tensile testing and tensile cycling tests confirmed the rigidity of the films, with about a 20% loss of elasticity after 25 cycles loading. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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16 pages, 4092 KiB  
Article
Processing Conditions, Thermal and Mechanical Responses of Stretchable Poly (Lactic Acid)/Poly (Butylene Succinate) Films
by Elena Fortunati, Debora Puglia, Antonio Iannoni, Andrea Terenzi, José Maria Kenny and Luigi Torre
Materials 2017, 10(7), 809; https://doi.org/10.3390/ma10070809 - 16 Jul 2017
Cited by 62 | Viewed by 6671
Abstract
Poly (lactic acid) (PLA) and poly (butylene succinate) (PBS) based films containing two different plasticizers [Acetyl Tributyl Citrate (ATBC) and isosorbide diester (ISE)] at three different contents (15 wt %, 20 wt % and 30 wt %) were produced by extrusion method. Thermal, [...] Read more.
Poly (lactic acid) (PLA) and poly (butylene succinate) (PBS) based films containing two different plasticizers [Acetyl Tributyl Citrate (ATBC) and isosorbide diester (ISE)] at three different contents (15 wt %, 20 wt % and 30 wt %) were produced by extrusion method. Thermal, morphological, mechanical and wettability behavior of produced materials was investigated as a function of plasticizer content. Filmature parameters were also adjusted and optimized for different formulations, in order to obtain similar thickness for different systems. Differential scanning calorimeter (DSC) results and evaluation of solubility parameter confirmed that similar miscibility was obtained for ATBC and ISE in PLA, while the two selected plasticizers resulted as not efficient for plasticization of PBS, to the limit that the PBS–30ATBC resulted as not processable. On the basis of these results, isosorbide-based plasticizer was considered a suitable agent for modification of a selected blend (PLA/PBS 80:20) and two mixing approaches were used to identify the role of ISE in the plasticization process: results from mechanical analysis confirmed that both produced PLA–PBS blends (PLA85–ISE15)–PBS20 and (PLA80–PBS20)–ISE15 could guarantee advantages in terms of deformability, with respect to the PLA80–PBS20 reference film, suggesting that the promising use of these stretchable PLA–PBS based films plasticized with isosorbide can provide novel solutions for food packaging applications. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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19 pages, 9457 KiB  
Article
Synthesis and Characterization of Bio-Based Polyesters: Poly(2-methyl-1,3-propylene-2,5-furanoate), Poly(isosorbide-2,5-furanoate), Poly(1,4-cyclohexanedimethylene-2,5-furanoate)
by Zoi Terzopoulou, Nejib Kasmi, Vasilios Tsanaktsis, Nikolaos Doulakas, Dimitrios N. Bikiaris, Dimitris S. Achilias and George Z. Papageorgiou
Materials 2017, 10(7), 801; https://doi.org/10.3390/ma10070801 - 14 Jul 2017
Cited by 60 | Viewed by 6493
Abstract
In the present study, three new biobased furanoate polyesters with potential use in food packaging applications, named poly(isosorbide furanoate) (PIsF), poly(methyl-propylene furanoate) (PMePF) and poly(1,4-cyclohexane-dimethylene 2,5-furanoate) (PCHDMF) were synthesized. As monomers for the preparation of the polyesters, 2,5-furandicarboxylic acid (FDCA) and diols with [...] Read more.
In the present study, three new biobased furanoate polyesters with potential use in food packaging applications, named poly(isosorbide furanoate) (PIsF), poly(methyl-propylene furanoate) (PMePF) and poly(1,4-cyclohexane-dimethylene 2,5-furanoate) (PCHDMF) were synthesized. As monomers for the preparation of the polyesters, 2,5-furandicarboxylic acid (FDCA) and diols with irregular or complicated structure were used, including isosorbide (IS), 2-methyl-1,3-propanediol (MPD) and 1,4-cyclohexane-dimethanol (CHDM). The polymerization process was carried out via melt polycondensation method. The structural characteristics and thermal behavior of the polymers were studied. The kinetic fragility of the amorphous phase of the polymers was evaluated. The thermal degradation was studied by means of thermogravimetry and a pyrolysis Py-GC/MS (Pyrolysis-Gas Chromatography/Mass Spectroscopy) system to estimate the degradation mechanism. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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14 pages, 6411 KiB  
Article
Effect of Starch Loading on the Thermo-Mechanical and Morphological Properties of Polyurethane Composites
by Tayser Sumer Gaaz, Abu Bakar Sulong, M. N. M. Ansari, Abdul Amir H. Kadhum, Ahmed A. Al-Amiery and Mohamed H. Nassir
Materials 2017, 10(7), 777; https://doi.org/10.3390/ma10070777 - 10 Jul 2017
Cited by 18 | Viewed by 4698
Abstract
The advancements in material science and technology have made polyurethane (PU) one of the most important renewable polymers. Enhancing the physio-chemical and mechanical properties of PU has become the theme of this and many other studies. One of these enhancements was carried out [...] Read more.
The advancements in material science and technology have made polyurethane (PU) one of the most important renewable polymers. Enhancing the physio-chemical and mechanical properties of PU has become the theme of this and many other studies. One of these enhancements was carried out by adding starch to PU to form new renewable materials called polyurethane-starch composites (PUS). In this study, PUS composites are prepared by adding starch at 0.5, 1.0, 1.5, and 2.0 wt.% to a PU matrix. The mechanical, thermal, and morphological properties of PU and PUS composites were investigated. Scanning electron microscope (SEM) images of PU and PUS fractured surfaces show cracks and agglomeration in PUS at 1.5 wt.% starch. The thermo-mechanical properties of the PUS composites were improved as starch content increased to 1.5 wt.% and declined by more starch loading. Despite this reduction, the mechanical properties were still better than that of neat PU. The mechanical strength increased as starch content increased to 1.5 wt.%. The tensile, flexural, and impact strengths of the PUS composites were found to be 9.62 MPa, 126.04 MPa, and 12.87 × 10−3 J/mm2, respectively, at 1.5 wt.% starch. Thermal studies showed that the thermal stability and crystallization temperature of the PUS composites increased compared to that of PU. The loss modulus curves showed that neat PU crystallizes at 124 °C and at 127 °C for PUS-0.5 wt.% and rises with increasing loading from 0.5 to 2 wt.%. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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11 pages, 1439 KiB  
Article
Gallic Acid as an Oxygen Scavenger in Bio-Based Multilayer Packaging Films
by Astrid F. Pant, Sven Sängerlaub and Kajetan Müller
Materials 2017, 10(5), 489; https://doi.org/10.3390/ma10050489 - 3 May 2017
Cited by 57 | Viewed by 9507
Abstract
Oxygen scavengers are used in food packaging to protect oxygen-sensitive food products. A mixture of gallic acid (GA) and sodium carbonate was used as an oxygen scavenger (OSc) in bio-based multilayer packaging films produced in a three-step process: compounding, flat film extrusion, and [...] Read more.
Oxygen scavengers are used in food packaging to protect oxygen-sensitive food products. A mixture of gallic acid (GA) and sodium carbonate was used as an oxygen scavenger (OSc) in bio-based multilayer packaging films produced in a three-step process: compounding, flat film extrusion, and lamination. We investigated the film surface color as well as oxygen absorption at different relative humidities (RHs) and temperatures, and compared the oxygen absorption of OSc powder, monolayer films, and multilayer films. The films were initially brownish-red in color but changed to greenish-black during oxygen absorption under humid conditions. We observed a maximum absorption capacity of 447 mg O2/g GA at 21 °C and 100% RH. The incorporation of GA into a polymer matrix reduced the rate of oxygen absorption compared to the GA powder because the polymer acted as a barrier to oxygen and water vapor diffusion. As expected, the temperature had a significant effect on the initial absorption rate of the multilayer films; the corresponding activation energy was 75.4 kJ/mol. Higher RH significantly increased the oxygen absorption rate. These results demonstrate for the first time the production and the properties of a bio-based multilayer packaging film with GA as the oxygen scavenger. Potential applications include the packaging of food products with high water activity (aw > 0.86). Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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11 pages, 2560 KiB  
Article
A Facile Pathway to Modify Cellulose Composite Film by Reducing Wettability and Improving Barrier towards Moisture
by Xiaorong Hu, Lin Chen, Dandan Tao, Zhaocheng Ma and Shilin Liu
Materials 2017, 10(1), 39; https://doi.org/10.3390/ma10010039 - 5 Jan 2017
Cited by 16 | Viewed by 5298
Abstract
The hydrophilic property of cellulose is a key limiting factor for its wide application. Here, a novel solution impregnation pathway was developed to increase the hydrophobic properties of cellulose. When compared with the regenerated cellulose (RC), the composite films showed a decrease in [...] Read more.
The hydrophilic property of cellulose is a key limiting factor for its wide application. Here, a novel solution impregnation pathway was developed to increase the hydrophobic properties of cellulose. When compared with the regenerated cellulose (RC), the composite films showed a decrease in water uptake ability towards water vapor, and an increase of the water contact angle from 29° to 65° with increasing resin content in the composites, with only a slight change in the transmittance. Furthermore, the Young’s modulus value increased from 3.2 GPa (RC film) to 5.1 GPa (RCBEA50 film). The results indicated that the composites had combined the advantages of cellulose and biphenyl A epoxy acrylate prepolymer (BEA) resin. The presented method has great potential for the preparation of biocomposites with improved properties. The overall results suggest that composite films can be used as high-performance packaging materials. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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Review

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26 pages, 1866 KiB  
Review
On the Use of PLA-PHB Blends for Sustainable Food Packaging Applications
by Marina Patricia Arrieta, María Dolores Samper, Miguel Aldas and Juan López
Materials 2017, 10(9), 1008; https://doi.org/10.3390/ma10091008 - 29 Aug 2017
Cited by 326 | Viewed by 21922
Abstract
Poly(lactic acid) (PLA) is the most used biopolymer for food packaging applications. Several strategies have been made to improve PLA properties for extending its applications in the packaging field. Melt blending approaches are gaining considerable interest since they are easy, cost-effective and readily [...] Read more.
Poly(lactic acid) (PLA) is the most used biopolymer for food packaging applications. Several strategies have been made to improve PLA properties for extending its applications in the packaging field. Melt blending approaches are gaining considerable interest since they are easy, cost-effective and readily available processing technologies at the industrial level. With a similar melting temperature and high crystallinity, poly(hydroxybutyrate) (PHB) represents a good candidate to blend with PLA. The ability of PHB to act as a nucleating agent for PLA improves its mechanical resistance and barrier performance. With the dual objective to improve PLAPHB processing performance and to obtain stretchable materials, plasticizers are frequently added. Current trends to enhance PLA-PHB miscibility are focused on the development of composite and nanocomposites. PLA-PHB blends are also interesting for the controlled release of active compounds in the development of active packaging systems. This review explains the most relevant processing aspects of PLA-PHB based blends such as the influence of polymers molecular weight, the PLA-PHB composition as well as the thermal stability. It also summarizes the recent developments in PLA-PHB formulations with an emphasis on their performance with interest in the sustainable food packaging field. PLA-PHB blends shows highly promising perspectives for the replacement of traditional petrochemical based polymers currently used for food packaging. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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22 pages, 2084 KiB  
Review
Combination of Poly(lactic) Acid and Starch for Biodegradable Food Packaging
by Justine Muller, Chelo González-Martínez and Amparo Chiralt
Materials 2017, 10(8), 952; https://doi.org/10.3390/ma10080952 - 15 Aug 2017
Cited by 356 | Viewed by 24910
Abstract
The massive use of synthetic plastics, in particular in the food packaging area, has a great environmental impact, and alternative more ecologic materials are being required. Poly(lactic) acid (PLA) and starch have been extensively studied as potential replacements for non-degradable petrochemical polymers on [...] Read more.
The massive use of synthetic plastics, in particular in the food packaging area, has a great environmental impact, and alternative more ecologic materials are being required. Poly(lactic) acid (PLA) and starch have been extensively studied as potential replacements for non-degradable petrochemical polymers on the basis of their availability, adequate food contact properties and competitive cost. Nevertheless, both polymers exhibit some drawbacks for packaging uses and need to be adapted to the food packaging requirements. Starch, in particular, is very water sensitive and its film properties are heavily dependent on the moisture content, exhibiting relatively low mechanical resistance. PLA films are very brittle and offer low resistance to oxygen permeation. Their combination as blend or multilayer films could provide properties that are more adequate for packaging purposes on the basis of their complementary characteristics. The main characteristics of PLA and starch in terms of not only the barrier and mechanical properties of their films but also of their combinations, by using blending or multilayer strategies, have been analyzed, identifying components or processes that favor the polymer compatibility and the good performance of the combined materials. The properties of some blends/combinations have been discussed in comparison with those of pure polymer films. Full article
(This article belongs to the Special Issue Biobased Polymers for Packaging Applications)
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