Special Issue "Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy"

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biomacromolecules, Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: closed (31 December 2020).

Special Issue Editors

Dr. José Alejandro Heredia-Guerrero
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Guest Editor
Departamento de Biología Molecular y Bioquímica, Universidad de Málaga, 29071 Málaga, Spain
Interests: bio-based polymers; bioplastics; plant cuticle; agro-wastes; sustainability; food packaging
Special Issues and Collections in MDPI journals
Dr. Susana Guzman-Puyol
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Guest Editor
Departamento de Biología Molecular y Bioquímica, Universidad de Málaga, 29071 Málaga, Spain
Interests: cellulose; bioplastics; circular economy; composites; biodegradability
Special Issues and Collections in MDPI journals
Dr. José Jesús Benítez
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Guest Editor
Instituto de Ciencia de Materiales de Sevilla, Centro Mixto CSIC-Universidad de Sevilla, Americo Vespucio 49, Isla de la Cartuja, E-41092 Sevilla, Spain
Interests: polyesters; cutin; self-assembly; atomic force microscopy; polymers; food packaging
Special Issues and Collections in MDPI journals

Special Issue Information

Dear Colleagues,

The ubiquity of non-biodegradable petroleum-based plastics in the massive production of commodities in a linear economy context (i.e., the “take, make, and dispose” model) is one of the most important sources of global pollution. Moreover, the imminent dwindling of fossil resources, the contamination derived from monomer synthesis and large-scale production, as well as important concerns about the safety of these plastics in specific applications are increasing social alarm regarding their common use. Such social concern is driving greener and stricter market policies and legal regulations concerning sustainability. Among them, the idea of a circular bioeconomy is presented as a viable and desirable solution. In particular, the use of by-products and wastes from agriculture, food, forestry, fishery, etc., to produce functional polymers is of special interest.

In this Special Issue, we aim to publish original works and reviews about processes and technologies for the fabrication and synthesis of sustainable bio-based polymers and their industrial applications such as food packaging, biomedical devices, textiles, membranes, etc., in terms of a circular bioeconomy. Investigations about the life-cycle analysis of bio-based polymers are also included.

Dr. José Alejandro Heredia-Guerrero
Dr. Susana Guzman-Puyol
Dr. José Jesús Benitez
Guest Editors

Keywords

  • bio-based polymers
  • sustainability
  • circular bioeconomy
  • polymeric materials
  • life cycle analysis

Published Papers (12 papers)

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Research

Jump to: Review

Article
Anthocyanin Hybrid Nanopigments from Pomegranate Waste: Colour, Thermomechanical Stability and Environmental Impact of Polyester-Based Bionanocomposites
Polymers 2021, 13(12), 1966; https://doi.org/10.3390/polym13121966 - 14 Jun 2021
Viewed by 674
Abstract
In the present work, anthocyanin (ACN) hybrid nanopigments were synthetized by using a natural pomegranate dye (PD) and calcined hydrotalcite (HT) and montmorillonite (MMT) nanoclays. A wide colour gamut was obtained with MMT-based nanopigments ranging from reddish to bluish hues caused by structural [...] Read more.
In the present work, anthocyanin (ACN) hybrid nanopigments were synthetized by using a natural pomegranate dye (PD) and calcined hydrotalcite (HT) and montmorillonite (MMT) nanoclays. A wide colour gamut was obtained with MMT-based nanopigments ranging from reddish to bluish hues caused by structural transformations of ACNs at different pH values. However, a buffer effect was observed with HT obtaining samples a similar final colour regardless of the synthesis conditions. Nanopigments added with a biomordant extracted from pomegranate peels showed a different colour compared to the incorporation of a commercial mordant due to the intrinsic colouring properties of the pomegranate bioadditive. The developed nanopigments were incorporated at 7 wt% loading to produce novel polyester-based bionanocomposites which were characterized in terms of thermal, mechanical and colour properties. The encapsulation of PD into the nanoclays improved its thermal stability, in particular for MMT-based nanopigments. The pH changes observed during the nanofillers synthesis affected the final colour of the MMT-based nanocomposites, inducing a general increase in ∆E* and a decrease in gloss values. Slight improvements were obtained in terms of elastic modulus for MMT-based polymer samples confirming the applicability of the developed bionanocomposites as colouring and reinforcement materials. A very similar environmental profile was obtained for MMT and HT-based nanofillers showing MMT-based nanopigments a slightly better general behaviour. The results of the LCA study evidenced the suitability of the processes used in this work to the circular bioeconomy approach through sustainable food waste management and the production of bioplastics using waste substrates. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
Morphological, Structural, Thermal, Permeability, and Antimicrobial Activity of PBS and PBS/TPS Films Incorporated with Biomaster-Silver for Food Packaging Application
Polymers 2021, 13(3), 391; https://doi.org/10.3390/polym13030391 - 27 Jan 2021
Viewed by 646
Abstract
The development of antimicrobial film for food packaging application had become the focus for researchers and scientists. This research aims to study the characteristics and antimicrobial activity of novel biofilms made of poly (butylene succinate) (PBS) and tapioca starch (TPS) added with 1.5% [...] Read more.
The development of antimicrobial film for food packaging application had become the focus for researchers and scientists. This research aims to study the characteristics and antimicrobial activity of novel biofilms made of poly (butylene succinate) (PBS) and tapioca starch (TPS) added with 1.5% or 3% of Biomaster-silver (BM) particle. In morphological examination, the incorporation of 3% BM particle was considerably good in forming well-structured PBS film. Meanwhile, the functional groups analysis revealed the 3% BM particle was effectively interacted with PBS molecular chains. The flame retard behavior of BM metal particle also helped in enhancing the thermal stability for pure PBS and PBS/TPS films. The nucleating effect of BM particles had improved the films crystallinity. Small pore size features with high barrier property for gas permeability was obtained for BM filled PBS/TPS films. From antimicrobial analysis, the BM particles possessed antimicrobial activity against three bacteria Staphylococcus aureus, Escherichia coli, and Salmonella Typhimurium in which PBS/TPS 3% BM film exhibited strong antimicrobial activity against all tested bacteria, however, PBS/TPS 1.5% BM film exhibited strong antimicrobial activity against E. coli only. Hence, the incorporation of BM into PBS/TPS film could be a sustainable way for developing packaging films to preserve food products. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
Linking Expansion Behaviour of Extruded Potato Starch/Rapeseed Press Cake Blends to Rheological and Technofunctional Properties
Polymers 2021, 13(2), 215; https://doi.org/10.3390/polym13020215 - 09 Jan 2021
Cited by 2 | Viewed by 527
Abstract
In order to valorise food by-products into healthy and sustainable products, extrusion technology can be used. Thereby, a high expansion rate is often a targeted product property. Rapeseed press cake (RPC) is a protein- and fibre-rich side product of oil pressing. Although there [...] Read more.
In order to valorise food by-products into healthy and sustainable products, extrusion technology can be used. Thereby, a high expansion rate is often a targeted product property. Rapeseed press cake (RPC) is a protein- and fibre-rich side product of oil pressing. Although there is detailed knowledge about the expansion mechanism of starch, only a few studies describe the influence of press cake addition on the expansion and the physical quality of the extruded products. This study assessed the effect of RPC inclusion on the physical and technofunctional properties of starch-containing directly expanded products. The effect of starch type (native and waxy), RPC level (10, 40, 70 g/100 g), extrusion moisture content (24, 29 g/100 g) and barrel temperature (20–140 °C) on expansion, hardness, water absorption, and solubility of the extrudates and extruder response was evaluated. At temperatures above 120 °C, 70 g/100 g of RPC increased the sectional and volumetric expansion of extrudates, irrespective of starch type. Since expansion correlates with the rheological properties of the melt, RPC and RPC/starch blends were investigated pre- and postextrusion in a closed cavity rheometer at extrusion-like conditions. It was shown that with increasing RPC level the complex viscosity |ƞ*| of extruded starch/RPC blends increased, which could be linked to expansion behaviour. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
Color Fixation Strategies on Sustainable Poly-Butylene Succinate Using Biobased Itaconic Acid
Polymers 2021, 13(1), 79; https://doi.org/10.3390/polym13010079 - 28 Dec 2020
Viewed by 565
Abstract
Biopo-lybutylene succinate (bioPBS) is gaining attention in the biodegradable polymer market due to its promising properties, such as high biodegradability and processing versatility, representing a potential sustainable replacement for fossil-based commodities. However, there is still a need to enhance its properties for certain [...] Read more.
Biopo-lybutylene succinate (bioPBS) is gaining attention in the biodegradable polymer market due to its promising properties, such as high biodegradability and processing versatility, representing a potential sustainable replacement for fossil-based commodities. However, there is still a need to enhance its properties for certain applications, with aesthetical and mechanical properties being a challenge. The aim of the present work is to improve these properties by adding selected additives that will confer bioPBS with comparable properties to that of current counterparts such as polypropylene (PP) for specific applications in the automotive and household appliances sectors. A total of thirteen materials have been studied and compared, being twelve biocomposites containing combinations of three different additives: a commercial red colorant, itaconic acid (IA) to enhance color fixation and zirconia (ZrO2) nanoparticles to maintain at least native PBS mechanical properties. The results show that the combination of IA and the coloring agent tends to slightly yellowish the blend due to the absorbance spectra of IA and also to modify the gloss due to the formation of IA nanocrystals that affects light scattering. In addition, for low amounts of IA (4 wt %), Young’s Modulus seems to be kept while elongation at break is even raised. Unexpectedly, a strong aging affect was found after four weeks. IA increases the hydrophilic behavior of the samples and thus seems to accelerate the hydrolization of the matrix, which is accompanied by an accused disaggregation of phases and an overall softening and rigidization effect. The addition of low amounts of ZrO2 (2 wt %) seems to provide the desired effect for hardening the surface while almost not affecting the other properties; however, higher amounts tends to form aggregates saturating the compounds. As a conclusion, IA might be a good candidate for color fixing in biobased polymers. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
A Facile Fabrication of Biodegradable and Biocompatible Cross-Linked Gelatin as Screen Printing Substrates
Polymers 2020, 12(5), 1186; https://doi.org/10.3390/polym12051186 - 22 May 2020
Cited by 1 | Viewed by 1019
Abstract
This study focuses on preparation and valuation of the biodegradable, native, and modified gelatin film as screen-printing substrates. Modified gelatin film was prepared by crosslinking with various crosslinking agents and the electrode array was designed by screen-printing. It was observed that the swelling [...] Read more.
This study focuses on preparation and valuation of the biodegradable, native, and modified gelatin film as screen-printing substrates. Modified gelatin film was prepared by crosslinking with various crosslinking agents and the electrode array was designed by screen-printing. It was observed that the swelling ratio of C-2, crosslinked with glutaraldehyde and EDC/NHS (1-ethyl-3-(3-dimethylaminopropyl) carbodiimide/N-hydroxysuccinimide) was found to be lower (3.98%) than that of C-1 (crosslinked with only glutaraldehyde) (8.77%) and C-0 (without crosslinking) (28.15%). The obtained results indicate that the swelling ratios of both C-1 and C-2 were found to be lower than that of C-0 (control one without crosslinking). The Young’s modulus for C-1 and C-2 was found to be 8.55 ± 0.57 and 23.72 ± 2.04 kPa, respectively. Hence, it was conveyed that the mechanical strength of C-2 was found to be two times higher than that of C-l, suggesting that the mechanical strength was enhanced upon dual crosslinking in this study also. The adhesion study indicates that silver ink adhesion on the gelation surface is better than that of carbon ink. In addition, the electrical response of C-2 with a screen-printed electrode (SPE) was found to be the same as the commercial polycarbonate (PC) substrate. The result of MTT (3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl tetrazolium bromide) assay suggested that the silver SPE on C-2 was non-cytotoxic toward L929 fibroblast cells proliferation. The results indicated that C-2 gelatin is a promising material to act as a screen-printing substrate with excellent biodegradable and biocompatible properties. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
Bio-Based Coatings for Food Metal Packaging Inspired in Biopolyester Plant Cutin
Polymers 2020, 12(4), 942; https://doi.org/10.3390/polym12040942 - 18 Apr 2020
Cited by 4 | Viewed by 1800
Abstract
Metals used for food canning such as aluminum (Al), chromium-coated tin-free steel (TFS) and electrochemically tin-plated steel (ETP) were coated with a 2–3-µm-thick layer of polyaleuritate, the polyester resulting from the self-esterification of naturally-occurring 9,10,16-trihydroxyhexadecanoic (aleuritic) acid. The kinetic of the esterification was [...] Read more.
Metals used for food canning such as aluminum (Al), chromium-coated tin-free steel (TFS) and electrochemically tin-plated steel (ETP) were coated with a 2–3-µm-thick layer of polyaleuritate, the polyester resulting from the self-esterification of naturally-occurring 9,10,16-trihydroxyhexadecanoic (aleuritic) acid. The kinetic of the esterification was studied by FTIR spectroscopy; additionally, the catalytic activity of the surface layer of chromium oxide on TFS and, in particular, of tin oxide on ETP, was established. The texture, gloss and wettability of coatings were characterized by AFM, UV-Vis total reflectance and static water contact angle (WCA) measurements. The resistance of the coatings to solvents was also determined and related to the fraction of unreacted polyhydroxyacid. The occurrence of an oxidative diol cleavage reaction upon preparation in air induced a structural modification of the polyaleuritate layer and conferred upon it thermal stability and resistance to solvents. The promoting effect of the tin oxide layer in such an oxidative cleavage process fosters the potential of this methodology for the design of effective long-chain polyhydroxyester coatings on ETP. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
A Deeper Microscopic Study of the Interaction between Gum Rosin Derivatives and a Mater-Bi Type Bioplastic
Polymers 2020, 12(1), 226; https://doi.org/10.3390/polym12010226 - 16 Jan 2020
Cited by 11 | Viewed by 1439
Abstract
The interaction between gum rosin and gum rosin derivatives with Mater-Bi type bioplastic, a biodegradable and compostable commercial bioplastic, were studied. Gum rosin and two pentaerythritol esters of gum rosin (Lurefor 125 resin and Unik Tack P100 resin) were assessed as sustainable compatibilizers [...] Read more.
The interaction between gum rosin and gum rosin derivatives with Mater-Bi type bioplastic, a biodegradable and compostable commercial bioplastic, were studied. Gum rosin and two pentaerythritol esters of gum rosin (Lurefor 125 resin and Unik Tack P100 resin) were assessed as sustainable compatibilizers for the components of Mater-Bi® NF 866 polymeric matrix. To study the influence of each additive in the polymeric matrix, each gum rosin-based additive was compounded in 15 wt % by melt-extrusion and further injection molding process. Then, the mechanical properties were assessed, and the tensile properties and impact resistance were determined. Microscopic analyses were carried out by field emission scanning electron microscopy (FE-SEM), atomic force microscopy (AFM) and atomic force microscopy with nanomechanical assessment (AFM-QNM). The oxygen barrier and wettability properties were also assayed. The study revealed that the commercial thermoplastic starch is mainly composed of three phases: A polybutylene adipate-co-terephthalate (PBAT) phase, an amorphous phase of thermoplastic starch (TPSa), and a semi-crystalline phase of thermoplastic starch (TPSc). The poor miscibility among the components of the Mater-Bi type bioplastic was confirmed. Finally, the formulations with the gum rosin and its derivatives showed an improvement of the miscibility and the solubility of the components depending on the additive used. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
Preparation and Characterization of Bio-Based PLA/PBAT and Cinnamon Essential Oil Polymer Fibers and Life-Cycle Assessment from Hydrolytic Degradation
Polymers 2020, 12(1), 38; https://doi.org/10.3390/polym12010038 - 25 Dec 2019
Cited by 12 | Viewed by 2284
Abstract
Nowadays, the need to reduce the dependence on fuel products and to achieve a sustainable development is of special importance due to environmental concerns. Therefore, new alternatives must be sought. In this work, extruded fibers from poly (lactic acid) (PLA) and poly (butylene [...] Read more.
Nowadays, the need to reduce the dependence on fuel products and to achieve a sustainable development is of special importance due to environmental concerns. Therefore, new alternatives must be sought. In this work, extruded fibers from poly (lactic acid) (PLA) and poly (butylene adipate-co-terephthalate) (PBAT) added with cinnamon essential oil (CEO) were prepared and characterized, and the hydrolytic degradation was assessed. A two-phase system was observed with spherical particles of PBAT embedded in the PLA matrix. The thermal analysis showed partial miscibility between PLA and PBAT. Mechanically, Young’s modulus decreased and the elongation at break increased with the incorporation of PBAT and CEO into the blends. The variation in weight loss for the fibers was below 5% during the period of hydrolytic degradation studied with the most important changes at 37 °C and pH 8.50. From microscopy, the formation of cracks in the fiber surface was evidenced, especially for PLA fibers in alkaline medium at 37 °C. This study shows the importance of the variables that influence the performance of polyester-cinnamon essential oil-based fibers in agro-industrial applications for horticultural product preservation. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
Kinetics and Chemorheological Analysis of Cross-Linking Reactions in Humins
Polymers 2019, 11(11), 1804; https://doi.org/10.3390/polym11111804 - 02 Nov 2019
Cited by 5 | Viewed by 1010
Abstract
Humins is a biomass-derived material, co-product of the acid-catalyzed conversion of cellulose and hemicellulose to platform chemicals. This work presents a thorough study concerning the crosslinking kinetics of humins by chemorheological analysis and model-free kinetics under isothermal and non-isothermal curing. Humins can auto-crosslink [...] Read more.
Humins is a biomass-derived material, co-product of the acid-catalyzed conversion of cellulose and hemicellulose to platform chemicals. This work presents a thorough study concerning the crosslinking kinetics of humins by chemorheological analysis and model-free kinetics under isothermal and non-isothermal curing. Humins can auto-crosslink under the effect of temperature, and the reaction can be fastener when adding an acidic initiator. Thus, the effect of P-Toluenesulfonic acid monohydrate (pTSA) on the crosslinking kinetics was also studied. The dependencies of the effective activation energy (Eα-dependencies) were determined by an advanced isoconversional method and correlated with the variation of complex viscosity during curing. It is shown that humins curing involves multi-step complex reactions and that the use of an acidic initiator allows faster crosslinking at lower temperatures, involving lower Eα. The shift from chemical to diffusion control was also estimated. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Article
Determination of Mean Intrinsic Flexural Strength and Coupling Factor of Natural Fiber Reinforcement in Polylactic Acid Biocomposites
Polymers 2019, 11(11), 1736; https://doi.org/10.3390/polym11111736 - 23 Oct 2019
Cited by 10 | Viewed by 742
Abstract
This paper is focused on the flexural properties of bleached kraft softwood fibers, bio-based, biodegradable, and a globally available reinforcement commonly used in papermaking, of reinforced polylactic acid (PLA) composites. The matrix, polylactic acid, is also a bio-based and biodegradable polymer. Flexural properties [...] Read more.
This paper is focused on the flexural properties of bleached kraft softwood fibers, bio-based, biodegradable, and a globally available reinforcement commonly used in papermaking, of reinforced polylactic acid (PLA) composites. The matrix, polylactic acid, is also a bio-based and biodegradable polymer. Flexural properties of composites incorporating percentages of reinforcement ranging from 15 to 30 wt % were measured and discussed. Another objective was to evaluate the strength of the interface between the matrix and the reinforcements, using the rule of mixtures to determine the coupling factor. Nonetheless, this rule of mixtures presents two unknowns, the coupling factor and the intrinsic flexural strength of the reinforcement. Hence, applying a ratio between the tensile and flexural intrinsic strengths and a defined fiber tensile and flexural strength factors, derived from the rule of mixtures is proposed. The literature lacks a precise evaluation of the intrinsic tensile strength of the reinforcements. In order to obtain such intrinsic tensile strength, we used the Kelly and Tyson modified equation as well as the solution provided by Bowyer and Bader. Finally, we were able to characterize the intrinsic flexural strengths of the fibers when used as reinforcement of polylactic acid. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Review

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Review
Bio-Based Alternatives to Phenol and Formaldehyde for the Production of Resins
Polymers 2020, 12(10), 2237; https://doi.org/10.3390/polym12102237 - 28 Sep 2020
Cited by 14 | Viewed by 1859
Abstract
Phenol–formaldehyde (PF) resin continues to dominate the resin industry more than 100 years after its first synthesis. Its versatile properties such as thermal stability, chemical resistance, fire resistance, and dimensional stability make it a suitable material for a wide range of applications. PF [...] Read more.
Phenol–formaldehyde (PF) resin continues to dominate the resin industry more than 100 years after its first synthesis. Its versatile properties such as thermal stability, chemical resistance, fire resistance, and dimensional stability make it a suitable material for a wide range of applications. PF resins have been used in the wood industry as adhesives, in paints and coatings, and in the aerospace, construction, and building industries as composites and foams. Currently, petroleum is the key source of raw materials used in manufacturing PF resin. However, increasing environmental pollution and fossil fuel depletion have driven industries to seek sustainable alternatives to petroleum based raw materials. Over the past decade, researchers have replaced phenol and formaldehyde with sustainable materials such as lignin, tannin, cardanol, hydroxymethylfurfural, and glyoxal to produce bio-based PF resin. Several synthesis modifications are currently under investigation towards improving the properties of bio-based phenolic resin. This review discusses recent developments in the synthesis of PF resins, particularly those created from sustainable raw material substitutes, and modifications applied to the synthetic route in order to improve the mechanical properties. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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Review
Bio-Based Packaging: Materials, Modifications, Industrial Applications and Sustainability
Polymers 2020, 12(7), 1558; https://doi.org/10.3390/polym12071558 - 14 Jul 2020
Cited by 34 | Viewed by 5489
Abstract
Environmental impacts and consumer concerns have necessitated the study of bio-based materials as alternatives to petrochemicals for packaging applications. The purpose of this review is to summarize synthetic and non-synthetic materials feasible for packaging and textile applications, routes of upscaling, (industrial) applications, evaluation [...] Read more.
Environmental impacts and consumer concerns have necessitated the study of bio-based materials as alternatives to petrochemicals for packaging applications. The purpose of this review is to summarize synthetic and non-synthetic materials feasible for packaging and textile applications, routes of upscaling, (industrial) applications, evaluation of sustainability, and end-of-life options. The outlined bio-based materials include polylactic acid, polyethylene furanoate, polybutylene succinate, and non-synthetically produced polymers such as polyhydrodyalkanoate, cellulose, starch, proteins, lipids, and waxes. Further emphasis is placed on modification techniques (coating and surface modification), biocomposites, multilayers, and additives used to adjust properties especially for barriers to gas and moisture and to tune their biodegradability. Overall, this review provides a holistic view of bio-based packaging material including processing, and an evaluation of the sustainability of and options for recycling. Thus, this review contributes to increasing the knowledge of available sustainable bio-based packaging material and enhancing the transfer of scientific results into applications. Full article
(This article belongs to the Special Issue Sustainable Bio-Based Polymers: Towards a Circular Bioeconomy)
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