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Polymers
Special Issues
Design and Modification of Bio-Based Polymers, Blends and Composites
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Design and Modification of Bio-Based Polymers, Blends and Composites

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 (20 August 2021) | Viewed by 28104

Special Issue Editor

Dr. Balázs Imre

E-Mail Website
Guest Editor
School of Biotechnology, KTH Royal Institute of Technology, AlbaNova University Centre, 106 91 Stockholm, Sweden
Interests: sustainable materials; polymers from renewable resources; polymer blends; polymer composites; compatibilization; carbohydrate chemistry; reactive processing; thermal analysis
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Facing global challenges such as climate change, excessive plastic pollution, and the depletion of fossil resources, economies around the world have been slowly transforming themselves in recent decades, heading towards a more sustainable future. This process is driven by the increasing environmental awareness of our society that continues to affect legislation as well as the production, commercialization, and use of plastic materials. By utilizing natural building blocks and advanced polymerization techniques, a range of new, fully or partially bio-based polyolefins, polyesters, polyamides, and polyurethanes have been developed and marketed in the last few decades.

Polymers of natural origin are commonly applied in a range of areas, from food packaging and agriculture to pharmaceuticals. Nevertheless, despite the increasing role these materials play in our lives, their estimated share of the global plastics market remains stagnant, at around only 1%. Compared with conventional alternatives, bio-based polymers are expensive to extract or synthesize and difficult to process, while their property profiles often do not match the requirements of large-scale applications. Intense research and development efforts in this field continue to yield solutions to these challenges through technological innovations and the design of new materials, often by blending or the incorporation of fillers and reinforcements.

This Special Issue of Polymers aims to showcase the most recent developments in the synthesis, modification, processing, and characterization of renewable polymeric materials, with a particular focus on heterogeneous systems: polymer blends and composites, (nano)fillers and reinforcements, and hydrogels and aerogels. Besides original research papers, review articles are also warmly welcomed and will be considered for publication as part of the Special Issue.

Dr. Balázs Imre
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Polymers is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Natural building blocks
  • Bio-based polymers
  • Polymer blends
  • Polymer composites
  • Natural fibers
  • Polymer hydrogels
  • Polymer aerogels
  • Compatibilization
  • Reactive processing
  • Ring-opening polymerization

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Published Papers (8 papers)

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Research

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14 pages, 7722 KiB  
Article
Effects of an Electric Field on the Conformational Transition of the Protein: Pulsed and Oscillating Electric Fields with Different Frequencies
by Qun Zhang, Dongqing Shao, Peng Xu and Zhouting Jiang
Polymers 2022, 14(1), 123; https://doi.org/10.3390/polym14010123 - 30 Dec 2021
Cited by 14 | Viewed by 2272
Abstract
The effect of pulsed and oscillating electric fields with different frequencies on the conformational properties of all-α proteins was investigated by molecular dynamics simulations. The root mean square deviation, the root mean square fluctuation, the dipole moment distribution, and the secondary structure analysis [...] Read more.
The effect of pulsed and oscillating electric fields with different frequencies on the conformational properties of all-α proteins was investigated by molecular dynamics simulations. The root mean square deviation, the root mean square fluctuation, the dipole moment distribution, and the secondary structure analysis were used to assess the protein samples’ structural characteristics. In the simulation, we found that the higher frequency of the electric field influences the rapid response to the secondary structural transitions. However, the conformational changes measured by RMSD are diminished by applying the electrical field with a higher frequency. During the dipole moment analysis, we found that the magnitude and frequency of the dipole moment was directly related to the strength and frequency of the external electric field. In terms of the type of electric fields, we found that the average values of RMSD and RMSF of whole molecular protein are larger when the protein is exposed in the pulsed electric field. Concerning the typical sample 1BBL, the secondary structure analysis showed that two alpha-helix segments both transit to turns or random coils almost simultaneously when it is exposed in a pulsed electric field. Meanwhile, two segments present the different characteristic times when the transition occurs in the condition of an oscillating electric field. This study also demonstrated that the protein with fewer charged residues or more residues in forming α-helical structures display the higher conformational stability. These conclusions, achieved using MD simulations, provide a theoretical understanding of the effect of the frequency and expression form of external electric fields on the conformational changes of the all-α proteins with charged residues and the guidance for anticipative applications. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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19 pages, 33977 KiB  
Article
Poly(lactic acid)–Poly(butylene succinate)–Sugar Beet Pulp Composites; Part II: Water Absorption Characteristics with Fine and Coarse Sugar Beet Pulp Particles; A Phenomenological Investigation
by Rodion Kopitzky
Polymers 2021, 13(20), 3558; https://doi.org/10.3390/polym13203558 - 15 Oct 2021
Cited by 1 | Viewed by 1545
Abstract
Sugar beet pulp (SBP) is a residue available in large quantities from the sugar industry, and can serve as a cost-effective bio-based and biodegradable filler for fully bio-based compounds containing bio-based polyesters. The composition of SBP is characterized by an unusually high content [...] Read more.
Sugar beet pulp (SBP) is a residue available in large quantities from the sugar industry, and can serve as a cost-effective bio-based and biodegradable filler for fully bio-based compounds containing bio-based polyesters. The composition of SBP is characterized by an unusually high content of pectins, which are known as water-binding substances. Their molecular structure and the poor gelling properties, compared to other pectin sources, do not allow industrial use on a larger scale. However, good water absorption capacity can be advantageous for promoting plastics degradation or disintegration in the environment. In this study, we evaluated the water absorption capacity and processes of SBP-filled composites with bio-based polyesters on a longer time scale. We analyzed water absorption from a phenomenological point of view and tried to derive basic parameters for the general description of the composites behavior. We found that polar polyesters or polyester blends filled with higher amounts of especially coarse SBP suffer disintegration within a few weeks when supplied with sufficient water. On the other hand, less polar polyesters filled with fine SBP rather absorb water but do not show disintegration for several months. On a time scale of a few years, catalytic disintegration of the composites appears to be independent of the addition of SBP. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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14 pages, 3338 KiB  
Article
The Role of Structure and Interactions in Thermoplastic Starch–Nanocellulose Composites
by Emília Csiszár, Dávid Kun and Erika Fekete
Polymers 2021, 13(18), 3186; https://doi.org/10.3390/polym13183186 - 20 Sep 2021
Cited by 12 | Viewed by 3951
Abstract
Composite films were fabricated by using cellulose nanocrystals (CNCs) as reinforcement up to 50 wt% in thermoplastic starch (TPS). Structure and interactions were modified by using different types (glycerol and sorbitol) and different amounts (30 and 40%) of plasticizers. The structure of the [...] Read more.
Composite films were fabricated by using cellulose nanocrystals (CNCs) as reinforcement up to 50 wt% in thermoplastic starch (TPS). Structure and interactions were modified by using different types (glycerol and sorbitol) and different amounts (30 and 40%) of plasticizers. The structure of the composites was characterized by visible spectroscopy, Haze index measurements, and scanning electron microscopy. Tensile properties were determined by tensile testing, and the effect of CNC content on vapor permeability was investigated. Although all composite films are transparent and can hardly be distinguished by human eyes, the addition of CNCs somewhat decreases the transmittance of the films. This can be related to the increased light scattering of the films, which is caused by the aggregation of nanocrystals, leading to the formation of micron-sized particles. Nevertheless, strength is enhanced by CNCs, mostly in the composite series prepared with 30% sorbitol. Additionally, the relatively high water vapor permeability of TPS is considerably decreased by the incorporation of at least 20 wt% CNCs. Reinforcement is determined mostly by the competitive interactions among starch, nanocellulose, and plasticizer molecules. The aging of the films is caused by the additional water uptake from the atmosphere and the retrogradation of starch. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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16 pages, 9158 KiB  
Article
The Role of Interfacial Adhesion in Polymer Composites Engineered from Lignocellulosic Agricultural Waste
by Dávid Kun, Zoltán Kárpáti, Erika Fekete and János Móczó
Polymers 2021, 13(18), 3099; https://doi.org/10.3390/polym13183099 - 14 Sep 2021
Cited by 6 | Viewed by 2512
Abstract
This paper presents a comprehensive study about the application of a lignocellulosic agricultural waste, sunflower husk in different polymer composites. Two types of milled sunflower husk with different geometrical factors were incorporated into polypropylene, low-density and high-density polyethylene, polystyrene (PS), glycol-modified polyethylene terephthalate [...] Read more.
This paper presents a comprehensive study about the application of a lignocellulosic agricultural waste, sunflower husk in different polymer composites. Two types of milled sunflower husk with different geometrical factors were incorporated into polypropylene, low-density and high-density polyethylene, polystyrene (PS), glycol-modified polyethylene terephthalate (PETG) and polylactic acid (PLA). The filler content of the composites varied between 0 and 60 vol%. The components were homogenized in an internal mixer and plates were compression molded for testing. The Lewis–Nielsen model was fitted to the moduli of each composite series, and it was found that the physical contact of the filler particles is a limiting factor of composite modulus. Interfacial interactions were estimated from two independent approaches. Firstly, the extent of reinforcement was determined from the composition dependence of tensile strength. Secondly, the reversible work of adhesion was calculated from the surface energies of the components. As only weak van der Waals interactions develop in the interphase of polyolefins and sunflower husk particles, adhesion is weak in their composites resulting in poor reinforcement. Interfacial adhesion enhanced by specific interactions in the interphase, such as π electron interactions for PS, hydrogen bonds for PLA, and both for PETG based composites. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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21 pages, 26377 KiB  
Article
Poly(Lactic Acid)–Poly(Butylene Succinate)–Sugar Beet Pulp Composites; Part I: Mechanics of Composites with Fine and Coarse Sugar Beet Pulp Particles
by Rodion Kopitzky
Polymers 2021, 13(15), 2531; https://doi.org/10.3390/polym13152531 - 30 Jul 2021
Cited by 4 | Viewed by 2260
Abstract
Sugar beet pulp (SBP) is a residue available in large quantities from the sugar industry, and can serve as a cost-effective bio-based and biodegradable filler for fully bio-based compounds based on bio-based polyesters. The heterogeneous cell structure of sugar beet suggests that the [...] Read more.
Sugar beet pulp (SBP) is a residue available in large quantities from the sugar industry, and can serve as a cost-effective bio-based and biodegradable filler for fully bio-based compounds based on bio-based polyesters. The heterogeneous cell structure of sugar beet suggests that the processing of SBP can affect the properties of the composite. An “Ultra-Rotor” type air turbulence mill was used to produce SBP particles of different sizes. These particles were processed in a twin-screw extruder with poly(lactic acid) (PLA) and poly(butylene succinate) (PBS) and fillers to granules for possible marketable formulations. Different screw designs, compatibilizers and the use of glycerol as a thermoplasticization agent for SBP were also tested. The spherical, cubic, or ellipsoidal-like shaped particles of SBP are not suitable for usage as a fiber-like reinforcement. In addition, the fineness of ground SBP affects the mechanical properties because (i) a high proportion of polar surfaces leads to poor compatibility, and (ii) due to the inner structure of the particulate matter, the strength of the composite is limited to the cohesive strength of compressed sugar-cell compartments of the SBP. The compatibilization of the polymer–matrix–particle interface can be achieved by using compatibilizers of different types. Scanning electron microscopy (SEM) fracture patterns show that the compatibilization can lead to both well-bonded particles and cohesive fracture patterns in the matrix. Nevertheless, the mechanical properties are limited by the impact and elongation behavior. Therefore, the applications of SBP-based composites must be well considered. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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19 pages, 7640 KiB  
Article
Films Based on Mater-Bi® Compatibilized with Pine Resin Derivatives: Optical, Barrier, and Disintegration Properties
by Miguel Aldas, Cristina Pavon, José Miguel Ferri, Marina Patricia Arrieta and Juan López-Martínez
Polymers 2021, 13(9), 1506; https://doi.org/10.3390/polym13091506 - 7 May 2021
Cited by 17 | Viewed by 3419
Abstract
Mater-Bi® NF866 (MB) was blended with gum rosin and two pentaerythritol esters of gum rosin (labeled as LF and UT), as additives, to produce biobased and compostable films for food packaging or agricultural mulch films. The films were prepared by blending MB [...] Read more.
Mater-Bi® NF866 (MB) was blended with gum rosin and two pentaerythritol esters of gum rosin (labeled as LF and UT), as additives, to produce biobased and compostable films for food packaging or agricultural mulch films. The films were prepared by blending MB with 5, 10, and 15 wt.% of each additive. The obtained films were characterized by optical, colorimetric, wettability, and oxygen barrier properties. Moreover, the additives and the MB-based films were disintegrated under composting conditions and the effect of each additive on the biodegradation rate was studied. All films were homogeneous and optically transparent. The color of the films tended to yellow tones due to the addition of pine resin derivatives. All the formulated films presented a complete UV-transmittance blocking effect in the UVA and UVB region, and those with 5 wt.% of pine resin derivatives increased the MB hydrophobicity. Low amounts of resins tend to maintain the oxygen transmission rate (OTR) values of the neat MB, due to its good solubilizing and compatibilizing effects. The disintegration under composting conditions test revealed that gum rosin completely disintegrates in about 90 days, while UT degrades 80% and LF degrades 5%, over 180 days of incubation. As expected, the same tendency was obtained for the disintegration of the studied films, although Mater-Bi® reach 28% of disintegrability over the 180 days of the composting test. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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Review

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22 pages, 4479 KiB  
Review
Recent Advances in Biotechnological Itaconic Acid Production, and Application for a Sustainable Approach
by Bernadette-Emőke Teleky and Dan Cristian Vodnar
Polymers 2021, 13(20), 3574; https://doi.org/10.3390/polym13203574 - 16 Oct 2021
Cited by 43 | Viewed by 6030
Abstract
Intense research has been conducted to produce environmentally friendly biopolymers obtained from renewable feedstock to substitute fossil-based materials. This is an essential aspect for implementing the circular bioeconomy strategy, expressly declared by the European Commission in 2018 in terms of “repair, reuse, and [...] Read more.
Intense research has been conducted to produce environmentally friendly biopolymers obtained from renewable feedstock to substitute fossil-based materials. This is an essential aspect for implementing the circular bioeconomy strategy, expressly declared by the European Commission in 2018 in terms of “repair, reuse, and recycling”. Competent carbon-neutral alternatives are renewable biomass waste for chemical element production, with proficient recyclability properties. Itaconic acid (IA) is a valuable platform chemical integrated into the first 12 building block compounds the achievement of which is feasible from renewable biomass or bio-wastes (agricultural, food by-products, or municipal organic waste) in conformity with the US Department of Energy. IA is primarily obtained through fermentation with Aspergillus terreus, but nowadays several microorganisms are genetically engineered to produce this organic acid in high quantities and on different substrates. Given its trifunctional structure, IA allows the synthesis of various novel biopolymers, such as drug carriers, intelligent food packaging, antimicrobial biopolymers, hydrogels in water treatment and analysis, and superabsorbent polymers binding agents. In addition, IA shows antimicrobial, anti-inflammatory, and antitumor activity. Moreover, this biopolymer retains qualities like environmental effectiveness, biocompatibility, and sustainability. This manuscript aims to address the production of IA from renewable sources to create a sustainable circular economy in the future. Moreover, being an essential monomer in polymer synthesis it possesses a continuous provocation in the biopolymer chemistry domain and technologies, as defined in the present review. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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15 pages, 2746 KiB  
Review
A Review: Research Progress in Modification of Poly (Lactic Acid) by Lignin and Cellulose
by Sixiang Zhai, Qingying Liu, Yuelong Zhao, Hui Sun, Biao Yang and Yunxuan Weng
Polymers 2021, 13(5), 776; https://doi.org/10.3390/polym13050776 - 3 Mar 2021
Cited by 23 | Viewed by 4620
Abstract
With the depletion of petroleum energy, the possibility of prices of petroleum-based materials increasing, and increased environmental awareness, biodegradable materials as a kind of green alternative have attracted more and more research attention. In this context, poly (lactic acid) has shown a unique [...] Read more.
With the depletion of petroleum energy, the possibility of prices of petroleum-based materials increasing, and increased environmental awareness, biodegradable materials as a kind of green alternative have attracted more and more research attention. In this context, poly (lactic acid) has shown a unique combination of properties such as nontoxicity, biodegradability, biocompatibility, and good workability. However, examples of its known drawbacks include poor tensile strength, low elongation at break, poor thermal properties, and low crystallization rate. Lignocellulosic materials such as lignin and cellulose have excellent biodegradability and mechanical properties. Compounding such biomass components with poly (lactic acid) is expected to prepare green composite materials with improved properties of poly (lactic acid). This paper is aimed at summarizing the research progress of modification of poly (lactic acid) with lignin and cellulose made in in recent years, with emphasis on effects of lignin and cellulose on mechanical properties, thermal stability and crystallinity on poly (lactic acid) composite materials. Development of poly (lactic acid) composite materials in this respect is forecasted. Full article
(This article belongs to the Special Issue Design and Modification of Bio-Based Polymers, Blends and Composites)
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