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A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Macromolecules".

Deadline for manuscript submissions: closed (30 November 2022) | Viewed by 13072

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Special Issue Editors

Dr. Jaroslav Mosnácek

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Guest Editor

Polymer Institute of Slovak Academy of Sciences, Bratislava, Slovakia
Interests: synthesis of well-defined polymers; reversible deactivation radical polymerizations; stimuli-responsive polymers; polymer-inorganic hybrids; modification of surfaces by polymers; synthesis of degradable polymers; polymers from renewable resources
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Dr. Anita Eckstein Andicsová

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Guest Editor

Polymer Institute, Slovak Academy of Sciences, Dubravska Cesta 9, 84541 Bratislava, Slovak Republic
Interests: fotoactive derivatives; syntetic polymers; biobased polymers; nanomaterials; composites
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

We are delighted to announce a call for submissions to a Special issue of the International Journal of Molecular Sciences devoted to “Polymers from Renewable Resources”, and focused to synthesis, modification, characterization and application of the polymers. The importance of development of polymers from renewable resources is continuously increasing due to depletion of fossil resources and issues related to wastes disposal. Therefore, bio-based polymers become more attractive for industry and academia. Similarly, government policies are more and more focused on renewable materials from the standpoints of being environmentally benign and sustainable.

Renewable polymers can be isolated from natural bio-materials followed by their modifications or synthesized from bio-based monomers. The monomers could be obtained naturally by fermentation of carbohydrates, chemical transformations of natural polymers (e.g. cellulose, lignin) or directly extracted, such as plant oils and terpenes. In these approaches wide range of monomers, including the originally petrochemical-based monomers (e.g. ethylene, terephthalic acid), can be now produced from renewable resources. In addition of these traditional polymers, many new polymers with special functionalities and novel properties can be prepared from chemically modified bio-products. Biodegradable polymers are of special importance among the polymers from renewable resources, from the point of view of the end of their life cycle.

We encourage submission of both original research articles and topical reviews.

Due to the success of the 1st edition, we would like to add more results and new insights from recent research projects. You can find the 1st edition at the following link.

https://www.mdpi.com/journal/ijms/special_issues/Renewable_Resource

Dr. Jaroslav Mosnácek
Dr. Anita Andicsova Eckstein
Guest Editors

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. International Journal of Molecular Sciences is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

biopolymers
renewable monomers
valorization of biomass
sustainable materials
biodegradable polymers
polymer composites
polyesters
polyamides
functionalization
degradation
characterization
controlled synthesis
functional polymers
(hydro)gels
controlled release
biomedicine
agriculture
packaging
environmental impact
polymers modification
vitrimers

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Published Papers (5 papers)

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Research

17 pages, 4080 KiB

Open AccessArticle

Highly Efficient Cationic Polymerization of β-Pinene, a Bio-Based, Renewable Olefin, with TiCl₄ Catalyst from Cryogenic to Energy-Saving Room Temperature Conditions

by Klára Verebélyi, Ákos Szabó, Zsombor Réti, Györgyi Szarka, Ákos Villányi and Béla Iván

Int. J. Mol. Sci. 2023, 24(6), 5170; https://doi.org/10.3390/ijms24065170 - 8 Mar 2023

Cited by 3 | Viewed by 2183

Abstract

Polymers based on renewable monomers are projected to have a significant role in the sustainable economy, even in the near future. Undoubtedly, the cationically polymerizable β-pinene, available in considerable quantities, is one of the most promising bio-based monomers for such purposes. In the course of our systematic investigations related to the catalytic activity of TiCl₄ on the cationic polymerization of this natural olefin, it was found that the 2-chloro-2,4,4-trimethylpentane (TMPCl)/TiCl₄/N,N,N′,N′-tetramethylethylenediamine (TMEDA) initiating system induced efficient polymerization in dichloromethane (DCM)/hexane (Hx) mixture at both −78 °C and room temperature. At −78 °C, 100% monomer conversion was observed within 40 min, resulting in poly(β-pinene) with relatively high M_n (5500 g/mol). The molecular weight distributions (MWD) were uniformly shifted towards higher molecular weights (MW) in these polymerizations as long as monomer was present in the reaction mixture. However, chain–chain coupling took place after reaching 100% conversion, i.e., under monomer-starved conditions, resulting in considerable molecular weight increase and MWD broadening at −78 °C. At room temperature, the polymerization rate was lower, but chain coupling did not occur. The addition of a second feed of monomer in the polymerization system led to increasing conversion and polymers with higher MWs at both temperatures. ¹H NMR spectra of the formed polymers indicated high in-chain double-bond contents. To overcome the polarity decrease by raising the temperature, polymerizations were also carried out in pure DCM at room temperature and at −20 °C. In both cases, rapid polymerization occurred with nearly quantitative yields, leading to poly(β-pinene)s with M_ns in the range of 2000 g/mol. Strikingly, polymerization by TiCl₄ alone, i.e., without any additive, also occurred with near complete conversion at room temperature within a few minutes, attributed to initiation by adventitious protic impurities. These results convincingly prove that highly efficient carbocationic polymerization of the renewable β-pinene can be accomplished with TiCl₄ as catalyst under both cryogenic conditions, applied widely for carbocationic polymerizations, and the environmentally benign, energy-saving room temperature, i.e., without any additive and cooling or heating. These findings enable TiCl₄-catalyzed eco-friendly manufacturing of poly(β-pinene)s, which can be utilized in various applications, and in addition, subsequent derivatizations could result in a range of high-added-value products. Full article

(This article belongs to the Special Issue Polymers from Renewable Resources 2.0)

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18 pages, 58318 KiB

Open AccessArticle

Preparation, Characterization, and Biological Properties of Hydroxyapatite from Bigeye Snapper (Priancanthus tayenus) Bone

by Nunnuth Jindapon, Phatthranit Klinmalai, Utoomporn Surayot, Nuttapol Tanadchangsaeng, Woradej Pichaiaukrit, Yuthana Phimolsiripol, Chaluntorn Vichasilp and Sutee Wangtueai

Int. J. Mol. Sci. 2023, 24(3), 2776; https://doi.org/10.3390/ijms24032776 - 1 Feb 2023

Cited by 8 | Viewed by 2803

Abstract

The optimum condition of acid hydrolysis for hydroxyapatite extraction from bigeye snapper (Priancanthus tayenus) bone and the effects of extraction time (10–60 min) and HCl concentration (2.0–5.0% w/v) on yield and hydroxyapatite properties were determined. The optimum extracted condition was found using 5% HCl for 60 min, which was 13.4% yield; 19.8 g/100 g Ca content; 9.6 g/100 g P content; 2.1 Ca/P ratio; L*, a*, b*; and ΔE as 84.5, 2.8, 16.5, and 15.6, respectively. The using of 5% NaOH solution was optimum for hydroxyapatite precipitation from the extracted solution. The characteristic and biological properties of the obtained hydroxyapatite were studied. Fourier transform infrared spectroscopy and X-ray diffraction results showed a good comparison between the extracted and commercial hydroxyapatite. The microstructure of the extracted hydroxyapatite from a scanning electron microscope showed an irregular and flat-plate shape, large surface area, and roughness. The extracted hydroxyapatite was non- and low-cytotoxicity at a concentration of 50 and 100–400 µg/mL, respectively. Bovine serum albumin (BSA) adsorption and desorption of hydroxyapatite was studied. An increasing BSA concentration, hydroxyapatite amount, and adsorption time significantly increased protein adsorption on hydroxyapatite. Protein desorption from BSA-loaded hydroxyapatite showed an increase of release initially in the first 4 days and became a steady release rate until 14 days. Full article

(This article belongs to the Special Issue Polymers from Renewable Resources 2.0)

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20 pages, 5207 KiB

Open AccessArticle

Thermal Insulating Rigid Polyurethane Foams with Bio-Polyol from Rapeseed Oil Modified by Phosphorus Additive and Reactive Flame Retardants

by Marcin Zemła, Aleksander Prociak, Sławomir Michałowski, Ugis Cabulis, Mikelis Kirpluks and Kirils Simakovs

Int. J. Mol. Sci. 2022, 23(20), 12386; https://doi.org/10.3390/ijms232012386 - 16 Oct 2022

Cited by 15 | Viewed by 2396

Abstract

In this article, rigid polyurethane foams obtained with the addition of a bio-polyol from rapeseed oil, were modified with the dimethyl propane phosphonate as additive flame retardant and two reactive flame retardants diethyl (hydroxymethyl)phosphonate and diethyl bis-(2-hydroxyethyl)-aminomethylphosphonate. The influence of used flame retardants on the foaming process and characteristic processing times of tested polyurethane systems were determined. The obtained foams were tested in terms of cell structure, physical and mechanical properties, as well as flammability. Modified foams had worse mechanical and thermal insulation properties, caused by lower cellular density and higher anisotropy coefficient in the cross-section parallel to the foam rise direction, compared to unmodified foam. However, the thermal conductivity of all tested foam materials was lower than 25.82 mW/m∙K. The applied modifiers effectively reduced the flammability of rigid polyurethane foams, among others, increasing the oxygen index above 21.4 vol.%, reducing the total heat released by about 41–51% and the rate of heat release by about 2–52%. A correlation between the limiting oxygen index values and both total heat released parameters from the pyrolysis combustion flow calorimetry and cone calorimetry was observed. The correlation was also visible between the value of the heat release capacity (HRC) parameter obtained from the pyrolysis combustion flow calorimetry and the maximum average rate of heat emission (MARHE) from the cone calorimeter test. Full article

(This article belongs to the Special Issue Polymers from Renewable Resources 2.0)

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17 pages, 3475 KiB

Open AccessArticle

Non-Isocyanate Aliphatic–Aromatic Poly(carbonate-urethane)s—An Insight into Transurethanization Reactions and Structure–Property Relationships

by Dominik Wołosz

Int. J. Mol. Sci. 2022, 23(19), 10999; https://doi.org/10.3390/ijms231910999 - 20 Sep 2022

Cited by 5 | Viewed by 2186

Abstract

This study reveals insights into the transurethanization reactions leading to the aliphatic–aromatic non-isocyanate poly(carbonate-urethane)s (NIPCUs) and their structure–property relationships. The crucial impact of the alkyl chain length in 4,4′-diphenylmethylene bis(hydroxyalkyl carbamate) (BHAC) on the process of transurethanization reactions was proved. The strong susceptibility of hydroxyethyl- and hydroxybutyl carbamate moieties to the back-biting side reactions was observed due to the formation of thermodynamically stable cyclic products and urea bonds in the BHACs and NIPCUs. When longer alkyl chains (hydroxypentyl-, hydroxyhexyl-, or hydroxydecyl carbamate) were introduced into the BHAC structure, it was not prone to the back-biting side reaction. Both ¹H and ¹³C NMR, as well as FT-IR spectroscopies, confirmed the presence of carbonate and urethane (and urea for some of the samples) bonds in the NIPCUs, as well as proved the lack of allophanate and ether groups. The increase in the alkyl chain length (from 5 to 10 carbon atoms) between urethane groups in the NIPCU hard segments resulted in the increase in the elongation at break and crystalline phase content, as well as the decrease in the T_g, tensile strength, and hardness. Moreover, the obtained NIPCUs exhibited exceptional mechanical properties (e.g., tensile strength of 40 MPa and elongation at break of 130%). Full article

(This article belongs to the Special Issue Polymers from Renewable Resources 2.0)

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15 pages, 3228 KiB

Open AccessArticle

Intra- and Intermolecular Hydrogen Bonding in Miscible Blends of CO₂/Epoxy Cyclohexene Copolymer with Poly(Vinyl Phenol)

by Wei-Ting Du, Yen-Ling Kuan and Shiao-Wei Kuo

Int. J. Mol. Sci. 2022, 23(13), 7018; https://doi.org/10.3390/ijms23137018 - 24 Jun 2022

Cited by 10 | Viewed by 2899

Abstract

In this study, we synthesized a poly(cyclohexene carbonate) (PCHC) through alternative ring-opening copolymerization of CO₂ with cyclohexene oxide (CHO) mediated by a binary LZn₂OAc₂ catalyst at a mild temperature. A two-dimensional Fourier transform infrared (2D FTIR) spectroscopy indicated that strong intramolecular [C–H···O=C] hydrogen bonding (H-bonding) occurred in the PCHC copolymer, thereby weakening its intermolecular interactions and making it difficult to form miscible blends with other polymers. Nevertheless, blends of PCHC with poly(vinyl phenol) (PVPh), a strong hydrogen bond donor, were miscible because intermolecular H-bonding formed between the PCHC C=O units and the PVPh OH units, as evidenced through solid state NMR and one-dimensional and 2D FTIR spectroscopic analyses. Because the intermolecular H-bonding in the PCHC/PVPh binary blends were relatively weak, a negative deviation from linearity occurred in the glass transition temperatures (T_g). We measured a single proton spin-lattice relaxation time from solid state NMR spectra recorded in the rotating frame [T_1ρ(H)], indicating full miscibility on the order of 2–3 nm; nevertheless, the relaxation time exhibited a positive deviation from linearity, indicating that the hydrogen bonding interactions were weak, and that the flexibility of the main chain was possibly responsible for the negative deviation in the values of T_g. Full article

(This article belongs to the Special Issue Polymers from Renewable Resources 2.0)

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