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Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior

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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Applications".

Deadline for manuscript submissions: closed (30 April 2020) | Viewed by 45755

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Prof. Dr. Alexey L. Iordanskii

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N. N. Semenov Federal Research Center for Chemical Physics Academy of Science, 119991 Moscow, Russia
Interests: biodegradable polymers; transport phenomena; electrospun fibers; controlled release; polymer blends; composites; water in macromolecular systems; sorption; gas permeability
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Prof. Dr. Nadia Lotti

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Department of Civil, Chemical, Environmental and Materials Engineering, University of Bologna, 40126 Bologna, Italy
Interests: polymer design; polymer synthesis and characterization; polymer modification; copolymerization; solid state properties; thermal properties and crystallization kinetics; mechanical characterization; bio-based monomers; bio-based polymers; nano-polymer; nanocomposites; gas barrier behaviour; polymer compostability; biopolymers for engineering tissue; polymeric for controlled drug delivery; biodegradation
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Dr. Michelina Soccio

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Department of Civil, Chemical, Environmental and Materials Engineering, University of Bologna, Via Terracini 28, 40131 Bologna, Italy
Interests: polymer synthesis; polymer modification; copolymerization; polymer characterization; solid state properties in polymers; polymer thermal properties; polymer crystallization kinetics; mechanical characterization; bio-based monomers; biopolymers; biomaterials; polymer nanostructuring; nanocomposites; gas barrier properties; polymer compostability; biopolymers for tissue engineering; polymeric devices for controlled drug delivery; biodegradation
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Special Issue Information

Dear Colleagues,

Over the few coming decades, bio-based and biodegradable plastics produced from sustainable bioresources should essentially substitute the prevalent synthetic plastics produced from exhaustible hydrocarbon fossils. To the greatest extent, this revolutionary trend has to be applied to the packaging manufacturing area, and especially to food packaging implementation.

Currently, polymer packaging wastes that cannot be decomposed in an eco-friendly manner at landfill sites generate a series of severe environmental challenges. In spite of the urgent need to use bioplastics, their global production capacity is in fact rather limited and in 2018 amounted to 2.1 million tons, i.e., less than 1% of total polymer production. Biodegradable plastics are produced in even smaller quantities, about 0.9 MT, but in accordance with the prognosis of European Bioplastics Nova Institute, in the next 5 years, their manufacturing will grow by ~45% and approach 1.3 MT annually. To supply rapid production, an increment of biodegradable plastics could provide the effective development of scientific–technical potential that promotes the comprehensive exploration of their structural, functional, and dynamic characteristics.

In this regard, the transition from passive barrier materials preventing water and oxygen transport as well as bacteria infiltration to active functional packaging that provides gas diffusion selectivity, antiseptics’ and other modifiers’ release, quality food indicators, temperature sensors, etc. should be based on thorough study of biopolymer crystallinity, morphology, diffusivity, active agent release, and controlled biodegradability. The last process includes biopolymer degradation prevention to enhance food packaging shelf-life and, in landfill sites, the acceleration of decomposition rate after end-of-life approaching.

In this Special Issue, we aspire to collect reasonable and comprehensive findings regarding structure and functionality of bio-based sustainable polymers performing as multifaceted barrier and active packaging in food, cosmetic, and other areas. The content of the collection will cover diverse fields of knowledge embracing polymer chemistry, microbiology, biotechnology, chemical engineering, materials science, physical–chemical characterizations, transport–diffusion phenomena, controlled release, biodegradation exploring, and others.

Prof. Dr. Alexey Iordanskii
Guest Editor

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Keywords

barrier polymers
active packaging
diffusion
permeability
bio-based and biodegradable polymers
biocomposites
electrospinning
food and cosmetic applications

Published Papers (11 papers)

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Editorial

Jump to: Research

4 pages, 170 KiB

Open AccessEditorial

Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior

by Alexey Iordanskii

Polymers 2020, 12(7), 1537; https://doi.org/10.3390/polym12071537 - 12 Jul 2020

Cited by 10 | Viewed by 2824

Abstract

An overview of the articles has presented for the Special Issue “Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior”. This issue has objective of collecting comprehensive findings regarding structure and functionality of bio-based sustainable polymers performing as multifaceted barrier and packaging in food, cosmetic, and other areas. The content of the collection covers diverse fields of knowledge embracing polymer chemistry, materials science, transport–diffusion phenomena, biodegradation exploring, and others. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

Research

Jump to: Editorial

26 pages, 8828 KiB

Open AccessArticle

Managing the Uncertainty and Accuracy of Life Cycle Assessment Results for the Process of Beverage Bottle Moulding

by Patrycja Bałdowska-Witos, Katarzyna Piotrowska, Weronika Kruszelnicka, Marek Błaszczak, Andrzej Tomporowski, Marek Opielak, Robert Kasner and Józef Flizikowski

Polymers 2020, 12(6), 1320; https://doi.org/10.3390/polym12061320 - 10 Jun 2020

Cited by 20 | Viewed by 3238

Abstract

Using environmentally friendly materials in the technological process of bottle production fits perfectly into the idea of sustainable development. The use of natural raw materials as well as conscious energy consumption are strategic aspects that should be considered in order to improve the effectiveness of the bottle moulding process. This paper presents a new and structured approach to the analysis of uncertainty and sensitivity in life cycle assessment, one developed in order to support the design process of environmentally friendly food packaging materials. With regard to this “probabilistic” approach to life cycle assessment, results are expressed as ranges of environmental impacts, and alternative solutions are developed while offering the concept of input uncertainty and the effect thereof on the final result. This approach includes: (1) the evaluation of the quality of inputs (represented by the origin matrix); (2) the reliability of results and (3) the uncertainty of results (the Monte Carlo method). The use of the methodology is illustrated based on an experiment conducted with real data from the technological process of bottle production. The results provide insight into the uncertainty of life cycle assessment indicators regarding global warming, acidification and the use of arable fields and farmland. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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18 pages, 1983 KiB

Open AccessArticle

Biodegradable Polylactide–Poly(3-Hydroxybutyrate) Compositions Obtained via Blending under Shear Deformations and Electrospinning: Characterization and Environmental Application

by Svetlana Rogovina, Lubov Zhorina, Andrey Gatin, Eduard Prut, Olga Kuznetsova, Anastasia Yakhina, Anatoliy Olkhov, Naum Samoylov, Maxim Grishin, Alexey Iordanskii and Alexandr Berlin

Polymers 2020, 12(5), 1088; https://doi.org/10.3390/polym12051088 - 10 May 2020

Cited by 19 | Viewed by 3196

Abstract

Compositions of polylactide (PLA) and poly(3-hydroxybutyrate) (PHB) thermoplastic polyesters originated from the nature raw have been obtained by blending under shear deformations and electrospinning methods in the form of films and nanofibers as well as unwoven nanofibrous materials, respectively. The degrees of crystallinity calculated on the base of melting enthalpies and thermal transition temperatures for glassy state, cold crystallization, and melting point for individual biopolymers and ternary polymer blends PLA-PHB- poly(ethyleneglycol) (PEG) have been evaluated. It has been shown that the mechanical properties of compositions depend on the presence of plasticizers PEG with different molar masses in interval of 400–1000. The experiments on the action of mold fungi on the films have shown that PHB is a fully biodegradable polymer unlike PLA, whereas the biodegradability of the obtained composites is determined by their composition. The sorption activity of PLA–PHB nanofibers and unwoven nanofibrous PLA–PHB composites relative to water and oil has been studied and the possibility of their use as absorbents in wastewater treatment from petroleum products has been demonstrated. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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14 pages, 3699 KiB

Open AccessArticle

Influence of Genipin Crosslinking on the Properties of Chitosan-Based Films

by Nataliya Kildeeva, Anatoliy Chalykh, Mariya Belokon, Tatyana Petrova, Vladimir Matveev, Evgeniya Svidchenko, Nikolay Surin and Nikita Sazhnev

Polymers 2020, 12(5), 1086; https://doi.org/10.3390/polym12051086 - 10 May 2020

Cited by 38 | Viewed by 4493

Abstract

Chitosan is a promising environment friendly active polymer packaging material due to its biodegradability, exceptional film forming capacity, great mechanical strength, appropriate barrier property along with intrinsic antioxidant and antimicrobial features. Bifunctional reagent was used for producing water insoluble chitosan films. Biopolymeric films crosslinked by Genipin (Gp), which is a reagent of natural origin, should have high potential in food packaging. The influence of the ratio of functional groups in the chitosan-Gp system on film absorption in the visible and ultraviolet regions of the spectrum, sorption, physical, and mechanical properties of the films has been studied. The degree of chitosan crosslinking in the films obtained from solutions containing Gp was estimated using the experimental data on film swelling and water vapor sorption isotherms. It is demonstrated that crosslinking with genipin improves swelling, water resistance, and mechanical properties of the films. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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15 pages, 4550 KiB

Open AccessArticle

Comparative Structure-Property Characterization of Poly(3-Hydroxybutyrate-Co-3-Hydroxyvalerate)s Films under Hydrolytic and Enzymatic Degradation: Finding a Transition Point in 3-Hydroxyvalerate Content

by Vsevolod A. Zhuikov, Yuliya V. Zhuikova, Tatiana K. Makhina, Vera L. Myshkina, Alexey Rusakov, Alexey Useinov, Vera V. Voinova, Garina A. Bonartseva, Alexandr A. Berlin, Anton P. Bonartsev and Alexey L. Iordanskii

Polymers 2020, 12(3), 728; https://doi.org/10.3390/polym12030728 - 24 Mar 2020

Cited by 28 | Viewed by 4084

Abstract

The hydrolytic and enzymatic degradation of polymer films of poly(3-hydroxybutyrate) (PHB) of different molecular mass and its copolymers with 3-hydroxyvalerate (PHBV) of different 3-hydroxyvalerate (3-HV) content and molecular mass, 3-hydroxy-4-methylvalerate (PHB4MV), and polyethylene glycol (PHBV-PEG) produced by the Azotobacter chroococcum 7B by controlled biosynthesis technique were studied under in vitro model conditions. The changes in the physicochemical properties of the polymers during their in vitro degradation in the pancreatic lipase solution and in phosphate-buffered saline for a long time (183 days) were investigated using different analytical techniques. A mathematical model was used to analyze the kinetics of hydrolytic degradation of poly(3-hydroxyaklannoate)s by not autocatalytic and autocatalytic hydrolysis mechanisms. It was also shown that the degree of crystallinity of some polymers changes differently during degradation in vitro. The total mass of the films decreased slightly up to 8–9% (for the high-molecular weight PHBV with the 3-HV content 17.6% and 9%), in contrast to the copolymer molecular mass, the decrease of which reached 80%. The contact angle for all copolymers after the enzymatic degradation decreased by an average value of 23% compared to 17% after the hydrolytic degradation. Young’s modulus increased up to 2-fold. It was shown that the effect of autocatalysis was observed during enzymatic degradation, while autocatalysis was not available during hydrolytic degradation. During hydrolytic and enzymatic degradation in vitro, it was found that PHBV, containing 5.7–5.9 mol.% 3-HV and having about 50% crystallinity degree, presents critical content, beyond which the structural and mechanical properties of the copolymer have essentially changed. The obtained results could be applicable to biomedical polymer systems and food packaging materials. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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19 pages, 2034 KiB

Open AccessArticle

Gas Transport Phenomena and Polymer Dynamics in PHB/PLA Blend Films as Potential Packaging Materials

by Valentina Siracusa, Svetlana Karpova, Anatoliy Olkhov, Anna Zhulkina, Regina Kosenko and Alexey Iordanskii

Polymers 2020, 12(3), 647; https://doi.org/10.3390/polym12030647 - 12 Mar 2020

Cited by 33 | Viewed by 4265

Abstract

Actually, in order to replace traditional fossil-based polymers, many efforts are devoted to the design and development of new and high-performance bioplastics materials. Poly(hydroxy alkanoates) (PHA_S) as well as polylactides are the main candidates as naturally derived polymers. The intention of the present study is to manufacture fully bio-based blends based on two polyesters: poly (3-hydroxybutyrate) (PHB) and polylactic acid (PLA) as real competitors that could be used to replace petrol polymers in packaging industry. Blends in the shape of films have been prepared by chloroform solvent cast solution methodology, at different PHB/PLA ratios: 1/0, 1/9, 3/7, 5/5, 0/1. A series of dynamic explorations have been performed in order to characterize them from a different point of view. Gas permeability to N₂, O₂, and CO₂ gases and probe (TEMPO) electron spin resonance (ESR) analyses were performed. Blend surface morphology has been evaluated by Scanning Electron Microscopy (SEM) while their thermal behavior was analyzed by Differential Scanning Calorimetry (DSC) technique. Special attention was devoted to color and transparency estimation. Both probe rotation mobility and N₂, O₂, and CO₂ permeation have monotonically decreased during the transition from PLA to PHB, for all contents of bio-blends, namely because of transferring from PLA with lower crystallinity to PHB with a higher one. Consequently, the role of the crystallinity was elucidated. The temperature dependences for CO₂ permeability and diffusivity as well as for probe correlation time allowed the authors to evaluate the activation energy of both processes. The values of gas transport energy activation and TEMPO rotation mobility are substantially close to each other, which should testify that polymer segmental mobility determines the gas permeability modality. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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17 pages, 4215 KiB

Open AccessArticle

Effect of Natural Rubber in Polyethylene Composites on Morphology, Mechanical Properties and Biodegradability

by Elena Mastalygina, Ivetta Varyan, Natalya Kolesnikova, Maria Isabel Cabrera Gonzalez and Anatoly Popov

Polymers 2020, 12(2), 437; https://doi.org/10.3390/polym12020437 - 13 Feb 2020

Cited by 22 | Viewed by 5094

Abstract

Compounding natural additives with synthetic polymers allows developing more eco-friendly materials with enhanced biodegradability. The composite films based on low-density polyethylene (PE) with different content of natural rubber (NR) (10–30 wt%) were investigated. The influence of NR content on structural features, water absorption and mechanical properties of the composites were studied. The 70PE/30NR composite is characterized by the uniform distribution and the smallest size of NR domains (45 ± 5 μm). A tensile test was satisfied by the mechanical properties of the biocomposites, caused by elasticity of NR domains. The tensile strength of 70PE/30NR composite film is 5 ± 0.25 MPa. Higher water absorption of PE/NR composites (1.5–3.7 wt%) compared to neat PE facilitates penetrating vital activity products of microorganisms. Mycological test with mold fungi and full-scale soil test detected the composite with 30 wt% of NR as the most biodegradable (mass loss was 7.2 wt% for 90 days). According to infrared spectroscopy and differential scanning calorimetry analysis, NR consumption and PE structural changes in the biocomposites after exposure to soil occurred. The PE/NR composites with enhanced biodegradability as well as satisfied mechanical and technological properties have potential applications in packaging and agricultural films. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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20 pages, 4837 KiB

Open AccessArticle

Application of LCA Method for Assessment of Environmental Impacts of a Polylactide (PLA) Bottle Shaping

by Patrycja Bałdowska-Witos, Weronika Kruszelnicka, Robert Kasner, Andrzej Tomporowski, Józef Flizikowski, Zbigniew Kłos, Katarzyna Piotrowska and Katarzyna Markowska

Polymers 2020, 12(2), 388; https://doi.org/10.3390/polym12020388 - 09 Feb 2020

Cited by 29 | Viewed by 5258

Abstract

In recent years, there has been a significant increase in the consumption of single-use packaging. Their material diversity is a significant barrier to recycling, causing overloading of landfills. Increasing negative environmental aspects have highlighted the need to develop solutions to achieve a relatively high efficiency of the bottle shaping process with the lowest possible energy consumption. The aim of the project is to try to describe the impact of this process on the state, transformation and development of the natural environment. The work concerns current issues of the impact of packaging on the natural environment. The main goal was to conduct a life cycle analysis (LCA) of beverage bottles made of polylactide. The functional unit comprised a total of 1000 pieces of PLA bottles with a capacity of 1 L. The boundary of the adopted system included the steps from the delivery of the preforms to the production plant to their correct formation in the process of forming beverage bottles. Further stages of the production process were excluded from the system, such as beverage bottling, labeling, and storage and distribution. Processes related to transport and storage of raw material were also excluded. The LCA analysis was performed using the program of the Dutch company Pre Consultants called SimaPro 8.4.0. The ReCiPe 2016 method was chosen for the interpretation of the quantity of emitted substances into the natural environment. The test results were presented graphically on bar charts and subjected to verification and interpretation. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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10 pages, 1471 KiB

Open AccessEditor’s ChoiceArticle

Water Vapor Permeability through Porous Polymeric Membranes with Various Hydrophilicity as Synthetic and Natural Barriers

by Chalykh Anatoly, Zolotarev Pavel, Chalykh Tatiana, Rubtsov Alexei and Zolotova Svetlana

Polymers 2020, 12(2), 282; https://doi.org/10.3390/polym12020282 - 01 Feb 2020

Cited by 10 | Viewed by 4083

Abstract

The article is devoted to the analysis of sorption kinetics, permeability, and diffusion of water vapor in porous polymeric membranes of different hydrophilicities and through-porosities. The water transport measurement with a constant gradient of partial pressure allows the authors to obtain reliable characteristics for porous membranes, films, artificial leathers, and fabrics of various chemical natures (synthetic and bio-based) and phase structures. All the kinetic permeability curves were determined and effective diffusion coefficients, as well as their apparent activation energies, were calculated at the stationary and non-stationary stages of the mass transfer. The relationship between the sorption–diffusion characteristics of the polymer barriers and their vapor permeability is traced. Within the framework of a Zolotarev–Dubinin dual dispersive model, an analytical equation is obtained that relates permeability to diffusion coefficients of water vapor in the pore volume, polymer skeleton material using such characteristics as porosity and the solubility coefficient. It is proposed to use this equation to predict the sorption properties for barrier and porous materials of complex architecture specifically in food packaging. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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18 pages, 4139 KiB

Open AccessArticle

Research of the Influence of the Ultrasonic Treatment on the Melts of the Polymeric Compositions for the Creation of Packaging Materials with Antimicrobial Properties and Biodegrability

by Irina Kirsh, Yuliya Frolova, Olga Bannikova, Olga Beznaeva, Isabella Tveritnikova, Dmitry Myalenko, Valentina Romanova and Daria Zagrebina

Polymers 2020, 12(2), 275; https://doi.org/10.3390/polym12020275 - 30 Jan 2020

Cited by 12 | Viewed by 2719

Abstract

Ensuring the microbiological safety of food products is a problem of current interest. The use of antimicrobial packaging materials is a way of solving the problem. When developing packaging materials, it is advisable to use a modern approach based on the creation of biodegradable materials. The difficulty in the selection of the polymer compositions’ components lies in solving the dilemma of the joint introduction and processing of antimicrobial and biodegradable agents. The studies of the ultrasound treatment on the melts of polymer mixtures showed an increase in the dispersion process of the components of the mixture. In this regard, this work aimed to study the effect of the ultrasonic treatment on the melts of polymer compositions containing thermoplastic starch and birch bark extract (BBE). In the work, the properties of PE-based packaging materials with various BBE concentrations obtained with ultrasonic treatment of melts on a laboratory extruder were studied. Biodegradable polymer compositions containing thermoplastic starch and BBE, obtained with the use of the ultrasonic treatment during extrusion, were investigated. The methods for studying rheological, physic-mechanical, antimicrobial properties and sanitary chemical indicators of materials were used in the article. It was found that ultrasonic treatment increases the melt flow and contributes to the production of materials with the uniform distribution of additives. The BBE content from 1.0% and higher in the contents of the material provides antimicrobial properties. When studying the permeability of oxygen and water vapor of the polymer compositions based on PE and BBE, it was found that the introduction of a filler increases vapor permeability by about 8–12% compared with control samples. The optimal concentration of BBE in polyethylene compositions containing thermoplastic starch was determined. The extension of the shelf life of the food product during storage in the developed material was established. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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17 pages, 3009 KiB

Open AccessArticle

On the Use of Gallic Acid as a Potential Natural Antioxidant and Ultraviolet Light Stabilizer in Cast-Extruded Bio-Based High-Density Polyethylene Films

by Luis Quiles-Carrillo, Sergi Montava-Jordà, Teodomiro Boronat, Chris Sammon, Rafael Balart and Sergio Torres-Giner

Polymers 2020, 12(1), 31; https://doi.org/10.3390/polym12010031 - 23 Dec 2019

Cited by 35 | Viewed by 5517

Abstract

This study originally explores the use of gallic acid (GA) as a natural additive in bio-based high-density polyethylene (bio-HDPE) formulations. Thus, bio-HDPE was first melt-compounded with two different loadings of GA, namely 0.3 and 0.8 parts per hundred resin (phr) of biopolymer, by twin-screw extrusion and thereafter shaped into films using a cast-roll machine. The resultant bio-HDPE films containing GA were characterized in terms of their mechanical, morphological, and thermal performance as well as ultraviolet (UV) light stability to evaluate their potential application in food packaging. The incorporation of 0.3 and 0.8 phr of GA reduced the mechanical ductility and crystallinity of bio-HDPE, but it positively contributed to delaying the onset oxidation temperature (OOT) by 36.5 °C and nearly 44 °C, respectively. Moreover, the oxidation induction time (OIT) of bio-HDPE, measured at 210 °C, was delayed for up to approximately 56 and 240 min, respectively. Furthermore, the UV light stability of the bio-HDPE films was remarkably improved, remaining stable for an exposure time of 10 h even at the lowest GA content. The addition of the natural antioxidant slightly induced a yellow color in the bio-HDPE films and it also reduced their transparency, although a high contact transparency level was maintained. This property can be desirable in some packaging materials for light protection, especially UV radiation, which causes lipid oxidation in food products. Therefore, GA can successfully improve the thermal resistance and UV light stability of green polyolefins and will potentially promote the use of natural additives for sustainable food packaging applications. Full article

(This article belongs to the Special Issue Bio-Based and Biodegradable Plastics: From Passive Barrier to Active Packaging Behavior)

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