Special Issue "Novel Biodegradable and Renewable Polymer-Based Nanohybrids and Applications"

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Biomaterials".

Deadline for manuscript submissions: 15 November 2020.

Special Issue Editor

Dr. Erlantz Lizundia
Website
Guest Editor
1 Department of Graphic Design and Engineering Projects, Bilbao Faculty of Engineering, University of the Basque Country (UPV/EHU), Bilbao 48013, Spain
2 BCMaterials, Basque Center Centre for Materials, Applications and Nanostructures, UPV/EHU Science Park, 48940 Leioa, Spain.
Interests: renewable materials; polymers; nanomaterials; cellulose nanocrystals; cellulose derivatives; energy storage; environmental remediation; multifunctional properties

Special Issue Information

Dear Colleagues,

Thanks to their low cost, ease of processing, and immense possibilities in tailoring their chemical and physical properties, polymers represent a leading class of material worldwide. Unfortunately, improper waste disposal policies have led to tremendous negative impacts on the biosphere, making them one of the biggest threats that faces our society. Being aware of the environmental burden associated with the “scourge of plastic”, it is up to scientists and industries to provide innovative alternatives to tackle this threat to humanity.

Biodegradable and renewable polymer-based nanohybrids emerge as a viable alternative to high “carbon footprint” petroleum-derived plastics, as they combine the biodegradability/renewability of the hosting matrix with improved functional properties arising from the incorporation of nanoparticles. In this sense, flagship polymers include but are not limited to polyesters, polysaccharides such as cellulose and chitin, certain classes of polyurethanes and polycarbonates, and polyanhydrides. With a plethora of opportunities arising from the combination of biodegradable/renewable polymers and nanoparticles, these systems offer exciting opportunities to design and synthesize novel multifunctional materials and devices. These are aimed to be applied in the fields of medicine, packaging, energy storage, catalysis, water purification, sensors, and actuators. Thanks to such propitious characteristics, it is expected that polymeric nanohybrids may take the lead in the transition to a sustainable society.

This Special Issue seeks to address recent developments in novel nanohybrids based on biodegradable and renewable polymers in a comprehensive way. Manuscripts dealing with the synthesis of novel biodegradable/renewable polymers, nanoparticles/nanohybrids/nanocomposites, functionalization, processing, multifunctional properties, novel applications, life cycle assessment (LCA), and recycling will be considered. Full papers, communications, and reviews covering these subjects are welcome.

Dr.  Erlantz Lizundia
Guest Editor

Manuscript Submission Information

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Keywords

  • Biobased/biodegradable polymers
  • Nanocomposites
  • Sustainable and renewable materials
  • Interface modification
  • Processing
  • Smart and multifunctional properties
  • Energy storage
  • Catalysis
  • Recycling
  • Life cycle assessment (LCA)

Published Papers (5 papers)

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Research

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Open AccessArticle
Cellulose Nanocrystal and Water-Soluble Cellulose Derivative Based Electromechanical Bending Actuators
Materials 2020, 13(10), 2294; https://doi.org/10.3390/ma13102294 - 15 May 2020
Abstract
This study reports a versatile method for the development of cellulose nanocrystals (CNCs) and water-soluble cellulose derivatives (methyl cellulose (MC), hydroxypropyl cellulose (HPC), and sodium carboxymethyl cellulose (NaCMC)) films comprising the ionic liquid (IL) 2-hydroxy-ethyl-trimethylammonium dihydrogen phosphate ([Ch][DHP]) for actuator fabrication. The influence [...] Read more.
This study reports a versatile method for the development of cellulose nanocrystals (CNCs) and water-soluble cellulose derivatives (methyl cellulose (MC), hydroxypropyl cellulose (HPC), and sodium carboxymethyl cellulose (NaCMC)) films comprising the ionic liquid (IL) 2-hydroxy-ethyl-trimethylammonium dihydrogen phosphate ([Ch][DHP]) for actuator fabrication. The influence of the IL content on the morphology and physico–chemical properties of free-standing composite films was evaluated. Independently of the cellulose derivative, the ductility of the films increases upon [Ch][DHP] incorporation to yield elongation at break values of nearly 15%. An increase on the electrical conductivity as a result of the IL incorporation into cellulosic matrices is found. The actuator performance of composites was evaluated, NaCMC/[Ch][DHP] showing the maximum displacement along the x-axis of 9 mm at 8 Vpp. Based on the obtained high electromechanical actuation performance, together with their simple processability and renewable nature, the materials fabricated here represent a step forward in the development of sustainable soft actuators of high practical relevance. Full article
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Open AccessArticle
Electroactive γ-Phase, Enhanced Thermal and Mechanical Properties and High Ionic Conductivity Response of Poly (Vinylidene Fluoride)/Cellulose Nanocrystal Hybrid Nanocomposites
Materials 2020, 13(3), 743; https://doi.org/10.3390/ma13030743 - 06 Feb 2020
Abstract
Cellulose nanocrystals (CNCs) were incorporated into poly (vinylidene fluoride) (PVDF) to tailor the mechanical and dielectric properties of this electroactive polymer. PVDF/CNC nanocomposites with concentrations up to 15 wt.% were prepared by solvent-casting followed by quick vacuum drying in order to ensure the [...] Read more.
Cellulose nanocrystals (CNCs) were incorporated into poly (vinylidene fluoride) (PVDF) to tailor the mechanical and dielectric properties of this electroactive polymer. PVDF/CNC nanocomposites with concentrations up to 15 wt.% were prepared by solvent-casting followed by quick vacuum drying in order to ensure the formation of the electroactive γ-phase. The changes induced by the presence of CNCs on the morphology of PVDF and its crystalline structure, thermal properties, mechanical performance and dielectric behavior are explored. The results suggest a relevant role of the CNC surface −OH groups, which interact with PVDF fluorine atoms. The real dielectric constant ε’ of nanocomposites at 200 Hz was found to increase by 3.6 times up to 47 for the 15 wt.% CNC nanocomposite due to an enhanced ionic conductivity provided by CNCs. The approach reported here in order to boost the formation of the γ-phase of PVDF upon the incorporation of CNCs serves to further develop cellulose-based multifunctional materials. Full article
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Open AccessArticle
Enzymatic Degradation of Acrylic Acid-Grafted Poly(butylene succinate-co-terephthalate) Nanocomposites Fabricated Using Heat Pressing and Freeze-Drying Techniques
Materials 2020, 13(2), 376; https://doi.org/10.3390/ma13020376 - 14 Jan 2020
Abstract
Biodegradable acrylic acid-grafted poly(butylene succinate-co-terephthalate) (g-PBST)/organically modified layered zinc phenylphosphonate (m-PPZn) nanocomposites were effectively fabricated containing covalent bonds between the g-PBST and m-PPZn. The results of wide-angle X-ray diffraction and transmission electron microscopy revealed that the morphology of the g-PBST/m-PPZn nanocomposites contained a [...] Read more.
Biodegradable acrylic acid-grafted poly(butylene succinate-co-terephthalate) (g-PBST)/organically modified layered zinc phenylphosphonate (m-PPZn) nanocomposites were effectively fabricated containing covalent bonds between the g-PBST and m-PPZn. The results of wide-angle X-ray diffraction and transmission electron microscopy revealed that the morphology of the g-PBST/m-PPZn nanocomposites contained a mixture of partially exfoliated or intercalated conformations. The isothermal crystallization behavior of the nanocomposites showed that the half-time for crystallization of 5 wt % g-PBST/m-PPZn nanocomposites was less than 1 wt % g-PBST/m-PPZn nanocomposites. This finding reveals that increasing the loading of m-PPZn can increase the crystallization rate of nanocomposites. Degradation tests of g-PBST/m-PPZn nanocomposites fabricated using the heat pressing and the freeze-drying process were performed by lipase from Pseudomonas sp. The degradation rates of g-PBST-50/m-PPZn nanocomposites were significantly lower than those of g-PBST-70/m-PPZn nanocomposites. The g-PBST-50 degraded more slowly due to the higher quantity of aromatic group and increased stiffness of the polymer backbone. The degradation rate of the freeze-drying specimens contained a more extremely porous conformation compared to those fabricated using the heat pressing process. Full article
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Open AccessArticle
Effects of Citric Acid on Structures and Properties of Thermoplastic Hydroxypropyl Amylomaize Starch Films
Materials 2019, 12(9), 1565; https://doi.org/10.3390/ma12091565 - 13 May 2019
Cited by 1
Abstract
Hydroxypropyl amylomaize starch (HPAS) films were prepared by hot press. The effects of initial pH of HPAS on the mechanical properties, molecular interaction, structure, and cross-linking degree of the resultant films were investigated. A weak acidic condition was suitable for cross-linking of citric [...] Read more.
Hydroxypropyl amylomaize starch (HPAS) films were prepared by hot press. The effects of initial pH of HPAS on the mechanical properties, molecular interaction, structure, and cross-linking degree of the resultant films were investigated. A weak acidic condition was suitable for cross-linking of citric acid and HPAS by reactive extrusion. The film of HPAS with an initial pH of 5.66 had the maximum tensile strength of 7.20 MPa and elongation-at-break of 94.53%, and the weight average molecular weight of HPAS increased to 4.17 × 105 g/mol. An appropriate initial pH facilitated the formation of diester bonds between HPAS and citric acid during extrusion, but too low initial pH levels resulted in hydrolysis of starch molecules and reduced the mechanical properties. Full article
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Review

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Open AccessReview
α-Cyclodextrin-Based Polypseudorotaxane Hydrogels
Materials 2020, 13(1), 133; https://doi.org/10.3390/ma13010133 - 28 Dec 2019
Abstract
Supramolecular hydrogels that are based on inclusion complexes between α-cyclodextrin and (co)polymers have gained significant attention over the last decade. They are formed via dynamic noncovalent bonds, such as host–guest interactions and hydrogen bonds, between various building blocks. In contrast to typical chemical [...] Read more.
Supramolecular hydrogels that are based on inclusion complexes between α-cyclodextrin and (co)polymers have gained significant attention over the last decade. They are formed via dynamic noncovalent bonds, such as host–guest interactions and hydrogen bonds, between various building blocks. In contrast to typical chemical crosslinking (covalent linkages), supramolecular crosslinking is a type of physical interaction that is characterized by great flexibility and it can be used with ease to create a variety of “smart” hydrogels. Supramolecular hydrogels based on the self-assembly of polypseudorotaxanes formed by a polymer chain “guest” and α-cyclodextrin “host” are promising materials for a wide range of applications. α-cyclodextrin-based polypseudorotaxane hydrogels are an attractive platform for engineering novel functional materials due to their excellent biocompatibility, thixotropic nature, and reversible and stimuli-responsiveness properties. The aim of this review is to provide an overview of the current progress in the chemistry and methods of designing and creating α-cyclodextrin-based supramolecular polypseudorotaxane hydrogels. In the described systems, the guests are (co)polymer chains with various architectures or polymeric nanoparticles. The potential applications of such supramolecular hydrogels are also described. Full article
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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

1. Supramolecular hydrogels based on inclusion complexes of α-cyclodextrin and polymeric nanoparticles

Adrian Domiński, Tomasz Konieczny, Piotr Kurcok*

Centre of Polymer and Carbon Materials of the Polish Academy of Sciences, 34, M. Curie-Sklodowskiej St., 41-819 Zabrze, Poland; [email protected]

Abstract: Supramolecular hydrogels, due to rheological properties and biocompatibility, have gained considerable attention over the last decade in tissue engineering and controlled drug delivery systems. They are formed as a result of dynamic non-covalent bonds between various building blocks (host-guest interactions, hydrogen bonds etc.). Comparing with typical chemical crosslinking (covalent linkages), supramolecular crosslinking as a type of physical interaction is characterized by facility and flexibility when creating a variety of "intelligent" hydrogels. Hydrophilic chains of polymeric nanoparticles can penetrate into the cavity of α-cyclodextrin and form polypseudorotaxanes, which subsequently undergoes self-assembly and supramolecular gels are formed. The supramolecular gels based on the self-assembly incorporation between α-cyclodextrin „host” and polymeric nanoparticle „guest” are promising biocompatible and biodegradable materials in the wide range of applications.

Aim of this work, is a comprehensive presentation of mechanism and kinetics of formation as well as  microstructure of such polypseudorotaxanes. The advances in development of supramolecular hydrogels based on host-guest interaction between α-CD and self-assembled amphiphilic polymeric nanoparticles has also been described.

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