Advances in Biodegradable Polymeric Materials with Applications in the Food Industry

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

Deadline for manuscript submissions: closed (25 February 2024) | Viewed by 22758

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Institute of Multidisciplinary Research for Science Technology, Valahia University of Targoviste, 13 Sinaia Alley, 130004 Targoviste, Romania
Interests: applied chemistry; analytical instrumental analysis; food analysis; advanced materials with ecological footprint; circular economy
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Guest Editor
Sciences and Advanced Technologies Department, Faculty of Sciences and Arts, Valahia University of Targoviste, 13 Sinaia Alley, 130004 Targoviste, Romania
Interests: chemistry; analytical chemistry; nanomaterials; bio based materials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Plastics used in the manufacture of packaging materials have become an important segment for the food industry due to their characteristics and low production costs. In the last several decades, companies in the food chain (producers, retailers, etc.) oriented towards a longer shelf life, and this generated a significant increase of the demand for food packaging. In addition, the use of petroleum-based plastics has led to environmental problems because of low rates of the recycling and reuse processes on one hand, and the high half-life of these polymeric materials on the other. 

Alternatives to oil-based polymers which are currently being explored include biopolymer materials and bio-based composites that can degrade easily after use. According to their composition, biopolymers may be classified into three categories: i. polymers incorporating biomass; ii. polymers synthesized from bio-derived monomers; and iii. biopolymers produced by living organisms. The global efforts put into creating new polymeric materials for the highly consuming food industry are closely combined with the attempts to maintain and improve the quality in the field. In this respect, the restrictive regulations translate into the need of desired physical, thermal, mechanical and chemical properties, which need to be characterized through advanced instrumental techniques. 

Dr. Cristina Mihaela Nicolescu
Dr. Marius Bumbac
Guest Editors

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Keywords

  • biopolymers
  • food packaging
  • bio-based composites
  • biodegradability
  • advanced techniques for polymeric materials characterization

Published Papers (11 papers)

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Research

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12 pages, 1246 KiB  
Article
Stability Qualification of Resins/Metallic Oxide Composites for Surface Oxidative Protection
by Traian Zaharescu, Radu Mirea, Tunde Borbath and Istvan Borbath
Polymers 2024, 16(3), 333; https://doi.org/10.3390/polym16030333 - 25 Jan 2024
Viewed by 731
Abstract
The accelerated degradation of alkyd resins via γ-irradiation is investigated using non-isothermal chemiluminescence. The stability qualification is possible through the comparison of emission intensities on a temperature range starting from 100 °C up to 250 °C under accelerated degradation caused by radiolysis scission. [...] Read more.
The accelerated degradation of alkyd resins via γ-irradiation is investigated using non-isothermal chemiluminescence. The stability qualification is possible through the comparison of emission intensities on a temperature range starting from 100 °C up to 250 °C under accelerated degradation caused by radiolysis scission. The measurements achieved in the samples of cured state resin modified by various inorganic oxides reveal the influence of metallic traces on the aging amplitude, when the thermal resistance increases as the irradiation dose is augmented. Even though the unirradiated samples present a prominent chemiluminescence intensity peak at 80 °C, the γ-processed specimens show less intense spectra under the pristine materials and the oxidation starts smoothly after 75 °C. The values of activation energies required for oxidative degradation of the sample subjected to 100 kGy are significantly higher in the composite states than in the neat resin. The degradation mechanism of polymerized resins is discussed taking into account the effects of fillers on the stability of studied epoxy resin at various temperatures when the degradation and crosslinking are in competition for the decay of free radical. Full article
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14 pages, 1093 KiB  
Article
Characterization of Moringa oleifera Seed Oil for the Development of a Biopackage Applied to Maintain the Quality of Turkey Ham
by Lesly Adamari Cueto Covarrubias, Mónica Andrea Valdez Solana, Claudia Avitia Domínguez, Alfredo Téllez Valencia, Jorge Armando Meza Velázquez and Erick Sierra Campos
Polymers 2024, 16(1), 132; https://doi.org/10.3390/polym16010132 - 30 Dec 2023
Viewed by 880
Abstract
Moringa oleifera has a high level of active chemicals that are useful in the food industry, and they have antibacterial and food preservation properties. The characterization of M. oleifera seed oil (MOS) may vary due to agronomic and environmental factors. Therefore, it was [...] Read more.
Moringa oleifera has a high level of active chemicals that are useful in the food industry, and they have antibacterial and food preservation properties. The characterization of M. oleifera seed oil (MOS) may vary due to agronomic and environmental factors. Therefore, it was necessary to know the composition of lipids present in our oil extracted under pressing at 180 °C and thus determine if it is suitable to produce a biopackaging. Within the characterization of the oil, it was obtained that MOS presented high-quality fatty acids (71% oleic acid) with low values of acidity (0.71 mg KOH/g) and peroxide (1.74 meq O2/kg). Furthermore, MOS was not very sensitive to lipoperoxidation by tert-butyl hydroperoxide (tBuOOH) and its phenolic components, oleic acid and tocopherols, allowed MOS to present a recovery of 70% after 30 min of treatment. Subsequently, a biopackaging was developed using a multiple emulsion containing corn starch/carboxymethylcellulose/glycerol/MOS, which presented good mechanical properties (strength and flexibility), transparency, and a barrier that prevents the transfer of UV light by 30% and UV-C by 98%, as well as a flux with the atmosphere of 5.12 × 10−8 g/ m.s. Pa that prevents moisture loss and protects the turkey ham from O2. Hence, the turkey ham suffered less weight loss and less hardness due to its preservation in the biopackaging. Full article
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18 pages, 4578 KiB  
Article
Polyhydroxybutyrate-co-hydroxyvalerate (PHBV) with Phenolic Acids for Active Food Packaging
by Eva Moll and Amparo Chiralt
Polymers 2023, 15(21), 4222; https://doi.org/10.3390/polym15214222 - 25 Oct 2023
Cited by 2 | Viewed by 1574
Abstract
PHBV films incorporating 3, 6 and 9% ferulic acid (FA) or p-coumaric acid (PCA) were obtained by melt blending and compression moulding. The films’ microstructures and thermal behaviours were analysed as well as their mechanical, optical and barrier properties. The overall and specific [...] Read more.
PHBV films incorporating 3, 6 and 9% ferulic acid (FA) or p-coumaric acid (PCA) were obtained by melt blending and compression moulding. The films’ microstructures and thermal behaviours were analysed as well as their mechanical, optical and barrier properties. The overall and specific migration of the materials in different food simulants was also characterised. FA was homogeneously mixed with the polymer, whereas PCA was mainly dispersed as fine particles in the PHBV matrices due to its higher melting point. These structural features promoted differences in the physical properties of the films depending on the compound concentration. As the concentration of both compounds rose, the barrier capacity of the films to oxygen, and to a lesser extent water vapour, was enhanced. While FA promoted the extensibility of the films, 9% PCA enhanced their brittleness. Both compounds affected the crystallisation pattern of the polymer, promoting smaller crystalline formations and a slight decrease in crystallinity. Although the overall migration of every film formulation was lower than the overall migration limit (OML), the release of active compounds was dependent on the food simulant; almost total release was noted in ethanol containing simulants but was more limited in aqueous systems. Therefore, these films could be used as food contact materials, contributing to extending the food’s shelf life. Full article
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21 pages, 3402 KiB  
Article
Nanocellulose from Cocoa Shell in Pickering Emulsions of Cocoa Butter in Water: Effect of Isolation and Concentration on Its Stability and Rheological Properties
by Catalina Gómez Hoyos, Luis David Botero, Andrea Flórez-Caro, Jorge Andrés Velásquez-Cock and Robin Zuluaga
Polymers 2023, 15(20), 4157; https://doi.org/10.3390/polym15204157 - 19 Oct 2023
Viewed by 1368
Abstract
There is a growing interest in developing new strategies to completely or partially replace cocoa butter in food and cosmetic products due to its cost and health effects. One of these alternatives is to develop stable emulsions of cocoa butter in water. However, [...] Read more.
There is a growing interest in developing new strategies to completely or partially replace cocoa butter in food and cosmetic products due to its cost and health effects. One of these alternatives is to develop stable emulsions of cocoa butter in water. However, incorporating cocoa butter is challenging as it solidifies and forms crystals, destabilizing the emulsion through arrested coalescence. Prevention against this destabilization mechanism is significantly lower than against coalescence. In this research, the rheological properties of nanocellulose from cocoa shell, a by-product of the chocolate industry, were controlled through isolation treatments to produce nanocellulose with a higher degree of polymerization (DP) and a stronger three-dimensional network. This nanocellulose was used at concentrations of 0.7 and 1.0 wt %, to develop cocoa butter in-water Pickering emulsion using a high shear mixing technique. The emulsions remained stable for more than 15 days. Nanocellulose was characterized using attenuated total reflection–Fourier transform infrared spectroscopy (ATR–FTIR), hot water and organic extractives, atomic force microscopy (AFM), degree of polymerization (DP), and rheological analysis. Subsequently, the emulsions were characterized on days 1 and 15 after their preparation through photographs to assess their physical stability. Fluorescent and electronic microscopy, as well as rheological analysis, were used to understand the physical properties of emulsions. Full article
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17 pages, 7138 KiB  
Article
TEMPO-Oxidized Cellulose Nanofibril Films Incorporating Graphene Oxide Nanofillers
by Yoojin Kim, Young-Teck Kim, Xiyu Wang, Byungjin Min and Su-il Park
Polymers 2023, 15(12), 2646; https://doi.org/10.3390/polym15122646 - 11 Jun 2023
Viewed by 1731
Abstract
To design a new system of novel TEMPO-oxidized cellulose nanofibrils (TOCNs)/graphene oxide (GO) composite, 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-mediated oxidation was utilized. For the better dispersion of GO into the matrix of nanofibrillated cellulose (NFC), a unique process combining high-intensity homogenization and ultrasonication was adopted [...] Read more.
To design a new system of novel TEMPO-oxidized cellulose nanofibrils (TOCNs)/graphene oxide (GO) composite, 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-mediated oxidation was utilized. For the better dispersion of GO into the matrix of nanofibrillated cellulose (NFC), a unique process combining high-intensity homogenization and ultrasonication was adopted with varying degrees of oxidation and GO percent loadings (0.4 to 2.0 wt%). Despite the presence of carboxylate groups and GO, the X-ray diffraction test showed that the crystallinity of the bio-nanocomposite was not altered. In contrast, scanning electron microscopy showed a significant morphological difference in their layers. The thermal stability of the TOCN/GO composite shifted to a lower temperature upon oxidation, and dynamic mechanical analysis signified strong intermolecular interactions with the improvement in Young’s storage modulus and tensile strength. Fourier transform infrared spectroscopy was employed to observe the hydrogen bonds between GO and the cellulosic polymer matrix. The oxygen permeability of the TOCN/GO composite decreased, while the water vapor permeability was not significantly affected by the reinforcement with GO. Still, oxidation enhanced the barrier properties. Ultimately, the newly fabricated TOCN/GO composite through high-intensity homogenization and ultrasonification can be utilized in a wide range of life science applications, such as the biomaterial, food, packaging, and medical industries. Full article
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18 pages, 6813 KiB  
Article
Preparation and Characterization of Microalgae Styrene-Butadiene Composites Using Chlorella vulgaris and Arthrospira platensis Biomass
by Marius Bumbac, Cristina Mihaela Nicolescu, Radu Lucian Olteanu, Stefan Cosmin Gherghinoiu, Costel Bumbac, Olga Tiron, Elena Elisabeta Manea, Cristiana Radulescu, Laura Monica Gorghiu, Sorina Geanina Stanescu, Bogdan Catalin Serban and Octavian Buiu
Polymers 2023, 15(6), 1357; https://doi.org/10.3390/polym15061357 - 8 Mar 2023
Cited by 4 | Viewed by 1794
Abstract
The food industry is a high consumer of polymer packing materials, sealing materials, and engineering components used in production equipment. Biobased polymer composites used in the food industry are obtained by incorporating different biogenic materials into the structure of a base polymer matrix. [...] Read more.
The food industry is a high consumer of polymer packing materials, sealing materials, and engineering components used in production equipment. Biobased polymer composites used in the food industry are obtained by incorporating different biogenic materials into the structure of a base polymer matrix. Renewable resources such as microalgae, bacteria, and plants may be used as biogenic materials for this purpose. Photoautotrophic microalgae are valuable microorganisms that are able to harvest sunlight energy and capture CO2 into biomass. They are characterized by their metabolic adaptability to environmental conditions, higher photosynthetic efficiency than terrestrial plants, and natural macromolecules and pigments. The flexibility of microalgae to grow in either low-nutrient or nutrient-rich environments (including wastewater) has led to the attention for their use in various biotechnological applications. Carbohydrates, proteins, and lipids are the main three classes of macromolecular compounds contained in microalgal biomass. The content in each of these components depends on their growth conditions. In general, proteins represent 40–70% of microalgae dry biomass, followed by carbohydrates (10–30%) and lipids (5–20%). A distinctive feature of microalgae cells is the presence of light-harvesting compounds such as photosynthetic pigments carotenoids, chlorophylls, and phycobilins, which are also receiving growing interest for applications in various industrial fields. The study comparatively reports on polymer composites obtained with biomass made of two species of green microalgae: Chlorella vulgaris and filamentous, gram-negative cyanobacterium Arthrospira. Experiments were conducted to reach an incorporation ratio of the biogenic material into the matrix in the 5–30% range, and the resulting materials were characterized by their mechanical and physicochemical properties. Full article
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14 pages, 2093 KiB  
Article
Physicochemical Characterization and Antioxidant Properties of Chitosan and Sodium Alginate Based Films Incorporated with Ficus Extract
by Saurabh Bhatia, Ahmed Al-Harrasi, Yasir Abbas Shah, Muhammad Jawad, Mohammed Said Al-Azri, Sana Ullah, Md Khalid Anwer, Mohammed F. Aldawsari, Esra Koca and Levent Yurdaer Aydemir
Polymers 2023, 15(5), 1215; https://doi.org/10.3390/polym15051215 - 28 Feb 2023
Cited by 8 | Viewed by 2202
Abstract
Aqueous extract of fruit obtained from Ficus racemosa enriched with phenolic components was used for the first time to fabricate chitosan (CS) and sodium alginate (SA)-based edible films. The edible films supplemented with Ficus fruit aqueous extract (FFE) were characterized physiochemically (using Fourier [...] Read more.
Aqueous extract of fruit obtained from Ficus racemosa enriched with phenolic components was used for the first time to fabricate chitosan (CS) and sodium alginate (SA)-based edible films. The edible films supplemented with Ficus fruit aqueous extract (FFE) were characterized physiochemically (using Fourier transform infrared spectroscopy (FT-IR), Texture analyser (TA), Thermogravimetric analysis (TGA), scanning electron microscopy (SEM), X-ray diffraction (XRD), and colourimeter) and biologically (using antioxidant assays). CS–SA–FFA films showed high thermal stability and high antioxidant properties. The addition of FFA into CS–SA film decreased transparency, crystallinity, tensile strength (TS), and water vapour permeability (WVP) but ameliorate moisture content (MC), elongation at break (EAB) and film thickness. The overall increase in thermal stability and antioxidant property of CS–SA–FFA films demonstrated that FFA could be alternatively used as a potent natural plant-based extract for the development of food packaging material with improved physicochemical and antioxidant properties. Full article
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15 pages, 6606 KiB  
Article
Preparation and Characterization of New Bioplastics Based on Polybutylene Succinate (PBS)
by Federico Barrino, Harrison De La Rosa-Ramírez, Chiara Schiraldi, Juan López-Martínez and María Dolores Samper
Polymers 2023, 15(5), 1212; https://doi.org/10.3390/polym15051212 - 28 Feb 2023
Cited by 11 | Viewed by 3145
Abstract
Sea and environmental pollution due to microplastics are global problems that in recent years have attracted particular interest in the scientific community. The increase in the world population and the consequent consumerism of non-reusable materials are amplifying these problems. In this manuscript, we [...] Read more.
Sea and environmental pollution due to microplastics are global problems that in recent years have attracted particular interest in the scientific community. The increase in the world population and the consequent consumerism of non-reusable materials are amplifying these problems. In this manuscript, we present novel bioplastics, which are completely biodegradable, for their potential use in food packaging, to replace fossil-fuel-derived plastic films and slow food degradation due to oxidative processes or microbial contamination. In this study, thin films based on polybutylene succinate (PBS) were prepared to reduce pollution, and different percentages by weight (1, 2 and 3 wt%) of extra virgin olive oil (EVO) and coconut oil (CO) were included to improve the chemico-physical properties of the polymer and possibly improve the functionality of the films in terms of prolonged food preservation. Attenuated total reflectance Fourier transform infrared (ATR/FTIR) spectroscopy was used to evaluate the interactions between the polymer and the oil. Furthermore, the mechanical properties and thermal behavior of the films were evaluated as a function of the oil content. A scanning electron microscopy (SEM) micrograph showed the surface morphology and the thickness of the materials. Finally, apple and kiwi were selected for a food-contact test, and the wrapped sliced fruit was monitored and evaluated for 12 days to macroscopically evaluate the oxidative process and/or eventually occurring contamination. The films were shown to reduce the browning of sliced fruit due to oxidation, and no molds were evidenced up to 10/12 days of observation with the addition of PBS, with 3 wt% of EVO achieving the best outcomes. Full article
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14 pages, 2970 KiB  
Article
Stabilization Activity of Kelp Extract in Ethylene–Propylene Rubber as Safe Packaging Material
by Traian Zaharescu
Polymers 2023, 15(4), 977; https://doi.org/10.3390/polym15040977 - 16 Feb 2023
Viewed by 1384
Abstract
This paper presents the stabilization effects of the solid extract of kelp (Ascophyllum nodosum) on an engineering elastomer, ethylene–propylene copolymer (EPR), which may be used as packaging material. Progressive increase in additive loadings (0.5, 1, and 2 phr) increases the oxidation [...] Read more.
This paper presents the stabilization effects of the solid extract of kelp (Ascophyllum nodosum) on an engineering elastomer, ethylene–propylene copolymer (EPR), which may be used as packaging material. Progressive increase in additive loadings (0.5, 1, and 2 phr) increases the oxidation induction time for thermally aged rubber at 190 °C from 10 min to 30 min for pristine material and modified polymer by adding 2 phr protection powder. When the studied polymer is γ-irradiated at 50 and 100 kGy, the onset oxidation temperatures increase as a result of blocking the oxidation reactivity of free radicals. The stabilization effect occurs through the activity of alginic acid, which is one of the main active components associated with alginates. The accelerated degradation caused by γ-exposure advances more slowly when the kelp extract is present. The OOT value for the oxidation of EPR samples increases from 130 °C to 165 °C after the γ-irradiation of pristine and modified (2 phr of kelp powder) EPR, respectively. The altered oxidation state of EPR samples by the action of γ-rays in saline serum is faster in neat polymer than in stabilized material. When the probes are placed in physiological serum and irradiated at 25 kGy, the OOT value for neat EPR (145 °C) is much lower than the homologous value for the polymer samples protected by kelp extract (153 °C for the concentration of 0.5 phr, 166 °C for the concentration of 1 phr, and 185 °C for the concentration of 2 phr). Full article
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14 pages, 1563 KiB  
Article
Development of Novel Blown Shrink Films from Poly(Lactide)/Poly(Butylene-Adipate-co-Terephthalate) Blends for Sustainable Food Packaging Applications
by Arianna Pietrosanto, Annalisa Apicella, Paola Scarfato, Loredana Incarnato and Luciano Di Maio
Polymers 2022, 14(14), 2759; https://doi.org/10.3390/polym14142759 - 6 Jul 2022
Cited by 6 | Viewed by 2024
Abstract
Heat-shrinkable films, largely made of polyolefins and widely employed in the packaging sector as collation or barrier films, due to their short service life, are held responsible for high environmental impact. One possible strategy for reduction in their carbon footprint can be the [...] Read more.
Heat-shrinkable films, largely made of polyolefins and widely employed in the packaging sector as collation or barrier films, due to their short service life, are held responsible for high environmental impact. One possible strategy for reduction in their carbon footprint can be the use of biodegradable polymers. Thus, this work aimed to develop novel, heat-shrinkable, fully biodegradable films for green packaging applications and to analyze their functional performance. Films were obtained from blends of amorphous polylactic acid (PLA) and poly(butylene-adipate-co-terephthalate) (PBAT) at different mass ratios and compatibilized with a chain extender. They were produced by means of a lab-scale film blowing extrusion apparatus and characterized in terms of physical–mechanical properties and shrinkability. The influence of the processing parameters during the extrusion blowing process on the films’ behavior was investigated, highlighting the effects of blend composition and stretching drawing conditions. Shrinkage tests demonstrated that the produced films have shrinkability values in the typical range of mono-oriented films (ca. 60–80% in machine direction and ca. 10–20% in transverse direction). Moreover, the shrinkage in machine direction increases both with the mass flow rate, the take-up ratio to blow-up ratio and the bubble cooling of the film blowing process, and with the PLA content into the blend. In particular, films at higher PLA content also exhibit higher transparency and stiffness. Full article
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Review

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48 pages, 3852 KiB  
Review
Biopolymers Produced by Lactic Acid Bacteria: Characterization and Food Application
by Cristina Mihaela Nicolescu, Marius Bumbac, Claudia Lavinia Buruleanu, Elena Corina Popescu, Sorina Geanina Stanescu, Andreea Antonia Georgescu and Siramona Maria Toma
Polymers 2023, 15(6), 1539; https://doi.org/10.3390/polym15061539 - 20 Mar 2023
Cited by 11 | Viewed by 4511
Abstract
Plants, animals, bacteria, and food waste are subjects of intensive research, as they are biological sources for the production of biopolymers. The topic links to global challenges related to the extended life cycle of products, and circular economy objectives. A severe and well-known [...] Read more.
Plants, animals, bacteria, and food waste are subjects of intensive research, as they are biological sources for the production of biopolymers. The topic links to global challenges related to the extended life cycle of products, and circular economy objectives. A severe and well-known threat to the environment, the non-biodegradability of plastics obliges different stakeholders to find legislative and technical solutions for producing valuable polymers which are biodegradable and also exhibit better characteristics for packaging products. Microorganisms are recognized nowadays as exciting sources for the production of biopolymers with applications in the food industry, package production, and several other fields. Ubiquitous organisms, lactic acid bacteria (LAB) are well studied for the production of exopolysaccharides (EPS), but much less as producers of polylactic acid (PLA) and polyhydroxyalkanoates (PHAs). Based on their good biodegradability feature, as well as the possibility to be obtained from cheap biomass, PLA and PHAs polymers currently receive increased attention from both research and industry. The present review aims to provide an overview of LAB strains’ characteristics that render them candidates for the biosynthesis of EPS, PLA, and PHAs, respectively. Further, the biopolymers’ features are described in correlation with their application in different food industry fields and for food packaging. Having in view that the production costs of the polymers constitute their major drawback, alternative solutions of biosynthesis in economic terms are discussed. Full article
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