Polymers

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15 pages, 2013 KiB

Open AccessArticle

Migration and Degradation in Composting Environment of Active Polylactic Acid Bilayer Nanocomposites Films: Combined Role of Umbelliferone, Lignin and Cellulose Nanostructures

by Magdalena L. Iglesias-Montes, Francesca Luzi, Franco Dominici, Luigi Torre, Liliana B. Manfredi, Viviana P. Cyras and Debora Puglia

Polymers 2021, 13(2), 282; https://doi.org/10.3390/polym13020282 - 16 Jan 2021

Cited by 18 | Viewed by 2958

Abstract

This study was dedicated to the functional characterization of innovative poly(lactic acid) (PLA)-based bilayer films containing lignocellulosic nanostructures (cellulose nanocrystals (CNCs) or lignin nanoparticles (LNPs)) and umbelliferone (UMB) as active ingredients (AIs), prepared to be used as active food packaging. Materials proved to [...] Read more.

This study was dedicated to the functional characterization of innovative poly(lactic acid) (PLA)-based bilayer films containing lignocellulosic nanostructures (cellulose nanocrystals (CNCs) or lignin nanoparticles (LNPs)) and umbelliferone (UMB) as active ingredients (AIs), prepared to be used as active food packaging. Materials proved to have active properties associated with the antioxidant action of UMB and LNPs, as the combination of both ingredients in the bilayer formulations produced a positive synergic effect inducing the highest antioxidant capacity. The results of overall migration for the PLA bilayer systems combining CNCs or LNPs and UMB revealed that none of these samples exceeded the overall migration limit required by the current normative for food packaging materials in both non-polar and polar simulants. Finally, all the hydrophobic monolayer and bilayer films were completely disintegrated in composting conditions in less than 18 days of incubation, providing a good insight on the potential use of these materials for application as active and compostable food packaging. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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11 pages, 1662 KiB

Open AccessArticle

Microstructure, Thermal Conductivity, and Flame Retardancy of Konjac Glucomannan Based Aerogels

by Ying Kuang, Lijun Chen, Junjun Zhai, Si Zhao, Qinjian Xiao, Kao Wu, Dongling Qiao and Fatang Jiang

Polymers 2021, 13(2), 258; https://doi.org/10.3390/polym13020258 - 14 Jan 2021

Cited by 18 | Viewed by 3545

Abstract

With abundant renewable resources and good biodegradability, bio-based aerogels are considered as promising insulating materials for replacing the conventional petroleum-based foam. In this study, konjac glucomannan (KGM)-based aerogels were prepared as thermal insulation materials via a convenient sol–gel and freeze-drying progress with different [...] Read more.

With abundant renewable resources and good biodegradability, bio-based aerogels are considered as promising insulating materials for replacing the conventional petroleum-based foam. In this study, konjac glucomannan (KGM)-based aerogels were prepared as thermal insulation materials via a convenient sol–gel and freeze-drying progress with different content of plant polysaccharides, proteins, and wheat straw. The morphology, thermal conductivity, and flame retardancy of KGM-based aerogels were determined. The KGM-based aerogels showed a uniform three-dimensional porous microstructure. The addition of wheat straw could significantly reduce the pore size of aerogels due to its special multi-cavity structure. KGM-based aerogels showed low densities (0.0234–0.0559 g/cm⁻³), low thermal conductivities (0.04573–0.05127 W/mK), low peak heat release rate (PHRR, 46.7–165.5 W/g), and low total heat release (THR, 5.7–16.2 kJ/g). Compared to the conventional expanded polystyrene (EPS) and polyurethane (PU) foam, the maximum limiting oxygen index (LOI) of KGM-based aerogels increased by 24.09% and 47.59%, the lowest PHRR decreased by 79.37% and 94.26%, and the lowest THR decreased by 76.54% and 89.25%, respectively. The results demonstrated that the KGM-based aerogels had better performance on flame retardancy than PU and EPS, indicating high potential applications as heat insulation in the green advanced engineering field. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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20 pages, 6702 KiB

Open AccessArticle

Physico-Chemical, Thermal, and Electrochemical Analysis of Solid Polymer Electrolyte from Vegetable Oil-Based Polyurethane

by Siti Rosnah Mustapa, Min Min Aung and Marwah Rayung

Polymers 2021, 13(1), 132; https://doi.org/10.3390/polym13010132 - 30 Dec 2020

Cited by 17 | Viewed by 3680

Abstract

In this paper, we report the preparation of bio-based polyurethane (PU) from renewable vegetable oil. The PU was synthesized through the reaction between jatropha oil-based polyol and isocyanate in a one-shot method. Then, lithium perchlorate (LiClO₄) salt was added to the [...] Read more.

In this paper, we report the preparation of bio-based polyurethane (PU) from renewable vegetable oil. The PU was synthesized through the reaction between jatropha oil-based polyol and isocyanate in a one-shot method. Then, lithium perchlorate (LiClO₄) salt was added to the polyurethane system to form an electrolyte film via a solution casting technique. The solid polymer electrolyte was characterized through several techniques such as nuclear magnetic resonance (NMR), Fourier transforms infrared (FTIR), electrochemical studies, thermal studies by differential scanning calorimetry (DSC), and dynamic mechanical analysis (DMA). The NMR analysis confirmed that the polyurethane was successfully synthesized and the intermolecular reaction had occurred in the electrolytes system. The FTIR results show the shifting of the carbonyl group (C=O), ether and ester group (C–O–C), and amine functional groups (N–H) in PU–LiClO₄ electrolytes compared to the blank polyurethane, which suggests that interaction occurred between the oxygen and nitrogen atom and the Li+ ion as they acted as electron donors in the electrolytes system. DSC analysis shows a decreasing trend in glass transition temperature, T_g and melting point, T_m of the polymer electrolyte as the salt content increases. Further, DMA analysis shows similar behavior in terms of T_g. The ionic conductivity increased with increasing salt content until the optimum value. The dielectric analysis reveals that the highest conducting electrolyte has the lowest relaxation time. The electrochemical behavior of the PU electrolytes is in line with the T_g result from the thermal analysis. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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15 pages, 3800 KiB

Open AccessArticle

Preliminary Study of In Vitro Three-Dimensional Skin Model Using an Ovine Collagen Type I Sponge Seeded with Co-Culture Skin Cells: Submerged versus Air-Liquid Interface Conditions

by Mh Busra Fauzi, Zahra Rashidbenam, Aminuddin Bin Saim and Ruszymah Binti Hj Idrus

Polymers 2020, 12(12), 2784; https://doi.org/10.3390/polym12122784 - 25 Nov 2020

Cited by 17 | Viewed by 5028

Abstract

Three-dimensional (3D) in vitro skin models have been widely used for cosmeceutical and pharmaceutical applications aiming to reduce animal use in experiment. This study investigate capability of ovine tendon collagen type I (OTC-I) sponge suitable platform for a 3D in vitro skin model [...] Read more.

Three-dimensional (3D) in vitro skin models have been widely used for cosmeceutical and pharmaceutical applications aiming to reduce animal use in experiment. This study investigate capability of ovine tendon collagen type I (OTC-I) sponge suitable platform for a 3D in vitro skin model using co-cultured skin cells (CC) containing human epidermal keratinocytes (HEK) and human dermal fibroblasts (HDF) under submerged (SM) and air-liquid interface (ALI) conditions. Briefly, the extracted OTC-I was freeze-dried and crosslinked with genipin (OTC-I_GNP) and carbodiimide (OTC-I_EDC). The gross appearance, physico-chemical characteristics, biocompatibility and growth profile of seeded skin cells were assessed. The light brown and white appearance for the OTC-I_GNP scaffold and other groups were observed, respectively. The OTC-I_GNP scaffold demonstrated the highest swelling ratio (~1885%) and water uptake (94.96 ± 0.14%). The Fourier transformation infrared demonstrated amide A, B and I, II and III which represent collagen type I. The microstructure of all fabricated sponges presented a similar surface roughness with the presence of visible collagen fibers and a heterogenous porous structure. The OTC-I_EDC scaffold was more toxic and showed the lowest cell attachment and proliferation as compared to other groups. The micrographic evaluation revealed that CC potentially formed the epidermal- and dermal-like layers in both SM and ALI that prominently observed with OTC-I_GNP compared to others. In conclusion, these results suggest that OTC_GNP could be used as a 3D in vitro skin model under ALI microenvironment. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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22 pages, 6607 KiB

Open AccessArticle

Silane-Functionalized Sheep Wool Fibers from Dairy Industry Waste for the Development of Plasticized PLA Composites with Maleinized Linseed Oil for Injection-Molded Parts

by Franciszek Pawlak, Miguel Aldas, Francisco Parres, Juan López-Martínez and Marina Patricia Arrieta

Polymers 2020, 12(11), 2523; https://doi.org/10.3390/polym12112523 - 29 Oct 2020

Cited by 28 | Viewed by 4983

Abstract

Poly(lactic acid) (PLA) was plasticized with maleinized linseed oil (MLO) and further reinforced with sheep wool fibers recovered from the dairy industry. The wool fibers were firstly functionalized with 1 and 2.5 phr of tris(2-methoxyethoxy)(vinyl) (TVS) silane coupling agent and were further used [...] Read more.

Poly(lactic acid) (PLA) was plasticized with maleinized linseed oil (MLO) and further reinforced with sheep wool fibers recovered from the dairy industry. The wool fibers were firstly functionalized with 1 and 2.5 phr of tris(2-methoxyethoxy)(vinyl) (TVS) silane coupling agent and were further used in 1, 5, and 10 phr to reinforce the PLA/MLO matrix. Then, the composite materials were processed by extrusion, followed by injection-molding processes. The mechanical, thermal, microstructural, and surface properties were assessed. While the addition of untreated wool fibers to the plasticized PLA/MLO matrix caused a general decrease in the mechanical properties, the TVS treatment was able to slightly compensate for such mechanical losses. Additionally, a shift in cold crystallization and a decrease in the degree of crystallization were observed due to the fiber silane modification. The microstructural analysis confirmed enhanced interaction between silane-modified fibers and the polymeric matrix. The inclusion of the fiber into the PLA/MLO matrix made the obtained material more hydrophobic, while the yellowish color of the material increased with the fiber content. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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16 pages, 6581 KiB

Open AccessArticle

Synthesis of Bio-Based Poly(Butylene Adipate-co-Butylene Itaconate) Copolyesters with Pentaerythritol: A Thermal, Mechanical, Rheological, and Molecular Dynamics Simulation Study

by Chin-Wen Chen, Hsu-I Mao, Zhi-Yu Yang, Kuan-Wei Huang, Hao-Chen Yan and Syang-Peng Rwei

Polymers 2020, 12(9), 2006; https://doi.org/10.3390/polym12092006 - 3 Sep 2020

Cited by 6 | Viewed by 3659

Abstract

Bio-based unsaturated poly(butylene adipate-co-butylene itaconate) (PBABI) aliphatic copolyesters were synthesized with pentaerythritol (PE) as a modifier, observing the melting point, crystallization, and glass transition temperatures were decreased from 59.5 to 19.5 °C and 28.2 to −9.1 °C as an increase of itaconate concentration, [...] Read more.

Bio-based unsaturated poly(butylene adipate-co-butylene itaconate) (PBABI) aliphatic copolyesters were synthesized with pentaerythritol (PE) as a modifier, observing the melting point, crystallization, and glass transition temperatures were decreased from 59.5 to 19.5 °C and 28.2 to −9.1 °C as an increase of itaconate concentration, and T_g ranged from −54.6 to −48.1 °C. PBABI copolyesters tend to the amorphous state by the existence of the BI unit above 40 mol%. The yield strength, elongation, and Young’s modulus at different BA/BI ratios were valued in a range of 13.2–13.8 MPa, 575.2–838.5%, and 65.1–83.8 MPa, respectively. Shear-thinning behavior was obtained in all BA/BI ratios of PBABI copolyesters around an angular frequency range of 20–30 rad s⁻¹. Furthermore, the thermal and mechanical properties of PBABI copolyesters can be well regulated via controlling the itaconic acid contents and adding the modifier. PBABI copolyesters can be coated on a 3D air mesh polyester fabric to reinforce the mechanical property for replacing traditional plaster applications. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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14 pages, 1632 KiB

Open AccessArticle

Injection-Molded Parts of Partially Biobased Polyamide 610 and Biobased Halloysite Nanotubes

by David Marset, Celia Dolza, Teodomiro Boronat, Nestor Montanes, Rafael Balart, Lourdes Sanchez-Nacher and Luis Quiles-Carrillo

Polymers 2020, 12(7), 1503; https://doi.org/10.3390/polym12071503 - 6 Jul 2020

Cited by 23 | Viewed by 3774

Abstract

This works focuses on the development of environmentally friendly composites with a partially biobased polyamide 610 (PA610), containing 63% biobased content, and a natural inorganic filler at the nanoscale, namely, halloysite nanotubes (HNTs). PA610 composites containing 10, 20, and 30 wt% HNTs were [...] Read more.

This works focuses on the development of environmentally friendly composites with a partially biobased polyamide 610 (PA610), containing 63% biobased content, and a natural inorganic filler at the nanoscale, namely, halloysite nanotubes (HNTs). PA610 composites containing 10, 20, and 30 wt% HNTs were obtained by melt extrusion in a twin screw co-rotating extruder. The resulting composites were injection-molded for further characterization. The obtained materials were characterized to obtain reliable data about their mechanical, thermal, and morphological properties. The effect of the HNTs wt% on these properties was evaluated. From a mechanical standpoint, the addition of 30 wt% HNTs gave an increase in tensile modulus of twice the initial value, thus verifying how this type of natural load provides increased stiffness on injection molded parts. The materials prepared with HNTs slightly improved the thermal stability, while a noticeable improvement on thermomechanical resistance over a wide temperature range was observed with increasing HNTs content. The obtained results indicate that high biobased content composites can be obtained with an engineering thermoplastic, i.e., PA610, and a natural inorganic nanotube-shaped filler, i.e., HNTs, with balanced mechanical properties and attractive behavior against high temperature. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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22 pages, 5823 KiB

Open AccessArticle

Effect of Lemon Waste Natural Dye and Essential Oil Loaded into Laminar Nanoclays on Thermomechanical and Color Properties of Polyester Based Bionanocomposites

by Bàrbara Micó-Vicent, Valentin Viqueira, Marina Ramos, Francesca Luzi, Franco Dominici, Luigi Torre, Alfonso Jiménez, Debora Puglia and María Carmen Garrigós

Polymers 2020, 12(7), 1451; https://doi.org/10.3390/polym12071451 - 28 Jun 2020

Cited by 16 | Viewed by 3733

Abstract

In this work, polyester-based nanocomposites added with laminar nanoclays (calcined hydrotalcite, HT, and montmorillonite, MMT) loaded with lemon waste natural dye (LD) and essential oil (LEO) were prepared and characterized. The optimal conditions to synthetize the hybrid materials were obtained by using statistically [...] Read more.

In this work, polyester-based nanocomposites added with laminar nanoclays (calcined hydrotalcite, HT, and montmorillonite, MMT) loaded with lemon waste natural dye (LD) and essential oil (LEO) were prepared and characterized. The optimal conditions to synthetize the hybrid materials were obtained by using statistically designed experiments. The maximum LD adsorption with HT was found using 5 wt% of surfactant (sodium dodecyl sulfate), 5 wt% of mordant (aluminum potassium sulfate dodecahydrate) and 50% (v/v) ethanol. For MMT, 10 wt% of surfactant (cetylpyridinium bromide), 5 wt% of mordant, 1 wt% of (3-aminopropyl) triethoxysilane and 100% distilled water were used. LEO adsorption at 300 wt% was maximized with MMT, 10 wt% of surfactant and 50 °C following an evaporation/adsorption process. The obtained hybrid nanofillers were incorporated in a polyester-based matrix (INZEA) at different loadings (3, 5, and 7 wt%) and the obtained samples were characterized in terms of thermal stability, tensile behavior, and color properties. HT_LEM-based samples showed a bright yellow color compared to MMT_LEM ones. The presence of lemon hybrid pigments in INZEA-based systems produced a remarkable variation in CIELAB color space values, which was more visible with increasing the nanofillers ratio. A limited mechanical enhancement and reduced thermal stability was observed with the nanopigments addition, suggesting a limited extent of intercalation/exfoliation of MMT and HT in the polymer matrix. MMT_LEM pigments showed higher thermal stability than HT_LEM ones. A significant increase in Young’s modulus of nanocomposites loaded with hybrid LEO was observed compared to the biopolymer matrix. The LEO inclusion into the nanoclays efficiently improved its thermal stability, especially for MMT. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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20 pages, 3827 KiB

Open AccessArticle

Compatibilization and Characterization of Polylactide and Biopolyethylene Binary Blends by Non-Reactive and Reactive Compatibilization Approaches

by Jose M. Ferri, Daniel Garcia-Garcia, Emilio Rayón, Maria D. Samper and Rafael Balart

Polymers 2020, 12(6), 1344; https://doi.org/10.3390/polym12061344 - 14 Jun 2020

Cited by 40 | Viewed by 4931

Abstract

In this study, different compatibilizing agents were used to analyze their influence on immiscible blends of polylactide (PLA) and biobased high-density polyethylene (bioPE) 80/20 (wt/wt). The compatibilizing agents used were polyethylene vinyl acetate (EVA) with a content of 33% of vinyl acetate, polyvinyl [...] Read more.

In this study, different compatibilizing agents were used to analyze their influence on immiscible blends of polylactide (PLA) and biobased high-density polyethylene (bioPE) 80/20 (wt/wt). The compatibilizing agents used were polyethylene vinyl acetate (EVA) with a content of 33% of vinyl acetate, polyvinyl alcohol (PVA), and dicumyl peroxide (DPC). The influence of each compatibilizing agent on the mechanical, thermal, and microstructural properties of the PLA-bioPE blend was studied using different microscopic techniques (i.e., field emission electron microscopy (FESEM), transmission electron microscopy (TEM), and atomic force microscopy with PeakForce quantitative nanomechanical mapping (AFM-QNM)). Compatibilized PLA-bioPE blends showed an improvement in the ductile properties, with EVA being the compatibilizer that provided the highest elongation at break and the highest impact-absorbed energy (Charpy test). In addition, it was observed by means of the different microscopic techniques that the typical droplet-like structure is maintained, but the use of compatibilizers decreases the dimensions of the dispersed droplets, leading to improved interfacial adhesion, being more pronounced in the case of the EVA compatibilizer. Furthermore, the incorporation of the compatibilizers caused a very marked decrease in the crystallinity of the immiscible PLA-bioPE blend. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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29 pages, 6347 KiB

Open AccessArticle

Production and Characterization of Controlled Release Urea Using Biopolymer and Geopolymer as Coating Materials

by Babar Azeem, Kuzilati KuShaari, Muhammad Naqvi, Lau Kok Keong, Mohammed Khaloofah Almesfer, Zakaria Al-Qodah, Salman Raza Naqvi and Noureddine Elboughdiri

Polymers 2020, 12(2), 400; https://doi.org/10.3390/polym12020400 - 10 Feb 2020

Cited by 71 | Viewed by 7800

Abstract

Synthetic polymers-based controlled release urea (CRU) leaves non-biodegradable coating shells when applied in soil. Several alternative green materials are used to produce CRU, but most of these studies have issues pertaining to nitrogen release longevity, process viability, and the ease of application of [...] Read more.

Synthetic polymers-based controlled release urea (CRU) leaves non-biodegradable coating shells when applied in soil. Several alternative green materials are used to produce CRU, but most of these studies have issues pertaining to nitrogen release longevity, process viability, and the ease of application of the finished product. In this study, we utilized tapioca starch, modified by polyvinyl alcohol and citric acid, as coating material to produce controlled release coated urea granules in a rotary fluidized bed equipment. Response surface methodology is employed for studying the interactive effect of process parameters on urea release characteristics. Statistical analysis indicates that the fluidizing air temperature and spray rate are the most influential among all five process parameters studied. The optimum values of fluidizing air temperature (80 °C), spray rate (0.13 mL/s), atomizing pressure (3.98 bar), process time (110 min), and spray temperature (70 °C) were evaluated by multi-objective optimization while using genetic algorithms in MATLAB^®. Urea coated by modified-starch was double coated by a geopolymer to enhance the controlled release characteristics that produced promising results with respect to the longevity of nitrogen release from the final product. This study provides leads for the design of a fluidized bed for the scaled-up production of CRU. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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15 pages, 6076 KiB

Open AccessArticle

Fully Biobased Shape Memory Thermoplastic Vulcanizates from Poly(Lactic Acid) and Modified Natural Eucommia Ulmoides Gum with Co-Continuous Structure and Super Toughness

by Yan Wang, Jinhui Liu, Lin Xia, Mei Shen, Liping Wei, Zhenxiang Xin and Jinkuk Kim

Polymers 2019, 11(12), 2040; https://doi.org/10.3390/polym11122040 - 9 Dec 2019

Cited by 22 | Viewed by 4215

Abstract

Novel, fully biobased shape memory thermoplastic vulcanizates (TPVs) were prepared using two sustainable biopolymers, poly(lactic acid) (PLA), and modified natural Eucommia ulmoides gum (EUG-g-GMA), via a dynamic vulcanization technique. Simultaneously, in situ compatibilization was achieved in the TPVs to improve interfacial [...] Read more.

Novel, fully biobased shape memory thermoplastic vulcanizates (TPVs) were prepared using two sustainable biopolymers, poly(lactic acid) (PLA), and modified natural Eucommia ulmoides gum (EUG-g-GMA), via a dynamic vulcanization technique. Simultaneously, in situ compatibilization was achieved in the TPVs to improve interfacial adhesion and the crosslinked modified Eucommia ulmoides gum (EUG) was in “netlike” continuous state in the PLA matrix to form “sea-sea” phase structure. The promoted interface and co-continuous structure played critical roles in enhancing shape memory capacity and toughness of the TPVs. The TPV with 40 wt % modified EUG displayed the highest toughness with an impact strength of 54.8 kJ/m² and the most excellent shape memory performances with a shape fixity ratio (R_f) of 99.83% and a shape recovery ratio (R_r) of 93.74%. The prepared shape memory TPVs would open up great potential applications in biobased shape memory materials for smart medical devices. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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Review

Jump to: Research

16 pages, 3221 KiB

Open AccessReview

Cationic UV-Curing of Epoxidized Biobased Resins

by Camilla Noè, Minna Hakkarainen and Marco Sangermano

Polymers 2021, 13(1), 89; https://doi.org/10.3390/polym13010089 - 28 Dec 2020

Cited by 109 | Viewed by 9835

Abstract

Epoxy resins are among the most important building blocks for fabrication of thermosets for many different applications thanks to their superior thermo-mechanical properties and chemical resistance. The recent concerns on the environmental problems and the progressive depletion of petroleum feedstocks have drawn the [...] Read more.

Epoxy resins are among the most important building blocks for fabrication of thermosets for many different applications thanks to their superior thermo-mechanical properties and chemical resistance. The recent concerns on the environmental problems and the progressive depletion of petroleum feedstocks have drawn the research interest in finding biobased alternatives. Many curing techniques can be used to obtain the final crosslinked thermoset networks. The UV-curing technology can be considered the most environmentally friendly because of the absence of volatile organic compound (VOC) emissions and mild curing conditions. This review provides an overview of the state of the art of bio-based cationic UV-curable epoxy resins. Particular focus has been given to the sources of the bio-based epoxy monomers and the applications of the obtained products. Full article

(This article belongs to the Special Issue Applied Bio-Based Materials)

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