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Special Issue "Advances in Cellulose-Based Polymers and Composites"

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A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Biomacromolecules, Biobased and Biodegradable Polymers".

Deadline for manuscript submissions: 15 September 2023 | Viewed by 7122

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Special Issue Editors

Dr. Anamaria Irimia

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Guest Editor

Petru Poni Institute of Macromolecular Chemistry, Iasi, Romania
Interests: cellulosic materials; bioactive materials; surface modification of natural polymers; polymer blends and composites; physico-chemical characterization

Dr. Carmen-Mihaela Popescu

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Guest Editor

Petru Poni Institute of Macromolecular Chemistry of the Romanian Academy, 700487 Iasi, Romania
Interests: thermal and chemical modification of wood; degradation processes affecting historic wood, the effect of different degradative factors and the degradation/ageing mechanisms involved in wood degradation; formulations with superhydrophobic and antibacterial properties for wood, wood-based products and other organic substrate protection; cellulose nanocrystals, lignin nanoparticles and silica based nano-composites; pickering emulsion polymerization
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Dear Colleagues,

Green chemistry and renewable natural resources have received considerable interest due to environmental requirements as well as their possible applications.

Cellulose has demonstrated its utility in many fields; however, it does not possess the special characteristics needed for certain applications without further treatments. The pre-treatment of cellulosic materials can be based on various techniques such as enzymes, physical or chemical methods, dissolution, fractionation, etc. Native cellulose is scarcely used due to its strong hydrophilic nature, pure solubility, and high crystallinity. Hence, cellulose-based polymers (i.e., cellulose fibers, cellulose membranes, cellulose nanomaterials or bacterial cellulose) have found a large spectrum of applications. They are used as synthetized or chemically modified in different composite materials in order to improve or modify the properties of the final product towards the desired application.

In recent years the research community has demonstrated a great deal of interest in finding and using unconventional sources as well as more ecofriendly methods for the extraction and modification of cellulose and cellulose nanomaterials.

This Special Issue on “Advances in Cellulose-Based Polymers and Composites” is dedicated to the most recent research regarding the preparation, properties, and applications of cellulose-based polymers, and their use in different composite formulations.

Both original contributions and comprehensive reviews are welcome.

Dr. Anamaria Irimia
Dr. Carmen-Mihaela Popescu
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. 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 2400 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

cellulose fibers
cellulose nanomaterials
bacterial cellulose
cellulose membranes
extraction methods
structural modification
cellulose based (nano)composites
biomaterials
(bio)degradability
functional materials

Published Papers (10 papers)

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Research

Open AccessArticle

Oil Media on Paper: Investigating the Interaction of Cold-Pressed Linseed Oil with Paper Supports with FTIR Analysis

Penelope Banou

Stamatis Boyatzis

Konstantinos Choulis

Charis Theodorakopoulos

and

Athena Alexopoulou

Polymers 2023, 15(11), 2567; https://doi.org/10.3390/polym15112567 - 02 Jun 2023

Viewed by 200

Abstract

Previous works of the authors have presented the changes in the optical, mechanical, and chemical properties of the oiled areas of the supports that occur upon ageing due to oil-binder absorption in works of art on paper and printed material. In this framework, transmittance FTIR analysis has indicated that the presence of linseed oil induces the conditions to promote the deterioration of the oil-impregnated areas of the paper supports. However, the analysis of oil-impregnated mock-ups did not provide detailed information about the input of linseed oil formulations and the different types of paper support on the chemical changes that occur upon ageing. This work presents the results of ATR-FTIR and reflectance FTIR, which were used for compensating the previous results, proving indications on the effect of different materials (linseed oil formulations, and cellulosic and lignocellulosic papers) on the development of chemical changes, thus, on the condition of the oiled areas upon ageing. Although linseed oil formulations have a determining effect on the condition of the oiled areas of the support, the paper pulp content appears to have an input to the chemical changes that occur in the system of paper–linseed oil upon ageing. The results presented are more focused on the oil-impregnated mock-ups with cold-pressed linseed oil since results have indicated that this causes more extended changes upon ageing. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

Thiol-Surface-Engineered Cellulose Nanocrystals in Favor of Copper Ion Uptake

and

Polymers 2023, 15(11), 2562; https://doi.org/10.3390/polym15112562 - 02 Jun 2023

Viewed by 234

Abstract

Cellulose, the most abundant natural polymer on earth, has recently gained attention for a large spectrum of applications. At a nanoscale, nanocelluloses (mainly involving cellulose nanocrystals or cellulose nanofibrils) possess many predominant features, such as highly thermal and mechanical stability, renewability, biodegradability and non-toxicity. More importantly, the surface modification of such nanocelluloses can be efficiently obtained based on the native surface hydroxyl groups, acting as metal ions chelators. Taking into account this fact, in the present work, the sequential process involving chemical hydrolysis of cellulose and autocatalytic esterification using thioglycolic acid was performed to obtain thiol-functionalized cellulose nanocrystals. The change in chemical compositions was attributed to thiol-functionalized groups and explored via the degree of substitution using a back titration method, X-ray powder diffraction, Fourier-transform infrared spectroscopy and thermogravimetric analysis. Cellulose nanocrystals were spherical in shape and ca. 50 nm in diameter as observed via transmission electron microscopy. The adsorption behavior of such a nanomaterial toward divalent copper ions from an aqueous solution was also assessed via isotherm and kinetic studies, elucidating a chemisorption mechanism (ion exchange, metal chelation and electrostatic force) and processing its operational parameters. In contrast to an inactive configure of unmodified cellulose, the maximum adsorption capacity of thiol-functionalized cellulose nanocrystals toward divalent copper ions from an aqueous solution was 4.244 mg g⁻¹ at a pH of 5 and at room temperature. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

Development of New Accelerated Aging Test for Comparison of the Quality of Different Insulating Papers Based on Cellulose

Draginja Mihajlovic

Valentina Vasovic

and

Jelena Lukic

Polymers 2023, 15(11), 2556; https://doi.org/10.3390/polym15112556 - 01 Jun 2023

Viewed by 259

Abstract

The aim of this study is to propose a test method for the determination of the quality of transformer paper insulation. For this purpose, the oil/cellulose insulation systems were exposed to various accelerated aging tests. The results of the aging experiments of normal Kraft and thermally upgraded papers, two different types of transformer oil (mineral and natural ester), and copper are shown. Aging was carried out in various experiments at 150 °C, 160 °C, 170 °C, and 180 °C with dry (initial values ≤ 0.5%) and moistened cellulose insulation (initial values 3–3.5%). Following insulating oil and paper, degradation markers were measured: the degree of polymerization, tensile strength, furan derivates, methanol/ethanol, acidity, interfacial tension, and dissipation factor. It was found that the aging of cellulose insulation in cycles was 1.5–1.6 times faster in comparison to continuous aging, due to the more pronounced effect of hydrolytic mechanism in cyclic aging owing to the produced and absorbed water. Furthermore, it was observed that the high initial water content in cellulose increases the aging rate two to three times more than in the dry experimental setup. The proposed aging test in cycles can be used to achieve faster aging and to compare the quality of different insulating papers. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

Investigation on Properties of Raw and Alkali Treated Novel Cellulosic Root Fibres of Zea Mays for Polymeric Composites

S. Anne Kavitha

R. Krishna Priya

Krishna Prakash Arunachalam

Siva Avudaiappan

Nelson Maureira-Carsalade

and

Ángel Roco-Videla

Polymers 2023, 15(7), 1802; https://doi.org/10.3390/polym15071802 - 06 Apr 2023

Cited by 4 | Viewed by 676

Abstract

Today, new materials based on natural fibres have been emerging day by day to completely eradicate plastics to favour our environmental nature. In this view, the present work is based on the extraction and characterisation of the novel root fibres of the Zea mays (Zm) plant, grown by the hydroponic method. Both the dried untreated and alkali treated root fibres are investigated using a variety of structural, morphological, thermal, elemental and mechanical tests by subjecting both the samples to p-XRD, FT-IR, SEM-EDAX, TGA-DTA, CHNS and tensile strength analyses. Thermal conductivity of the untreated and treated fibres is found using Lee’s disc experiment. From p-XRD analysis, the Crystallinity Index, Percentage Crystallinity and Crystallite size of the samples are found. FT-IR studies clarify the different vibrational groups associated with the fibre samples. SEM images show that the surface roughness increases for the chemically treated samples, such that it may be effectively utilised as reinforcement for polymeric composites. The diameter of the fibre samples is found using SEM analysis. According to the EDAX spectrum, Zm fibres in both their raw and processed forms have high levels of Carbon (C) and Oxygen (O). The TGA-DTA tests revealed that the samples of natural fibre have good thermal characteristics. CHNS studies show that Carbon content is high for these samples, which is the characteristic of many natural fibres. Chemical analysis is used to ascertain the prepared samples’ chemical makeup. It reveals that both samples have significant amounts of cellulose. The density of the fibres is found to be in the range 0.3–0.6 g/cc, which is much less than any other natural fibre. Therefore, it can be used in light weight applications. From the tensile strength analysis, physical properties such as Young’s modulus and micro-fibril angle are determined. The fibres in the roots exhibit a lower tensile strength. Thus, these fibres can be used in powdered form as reinforcement for natural rubber or epoxy composites. After examining all of its properties, it could be reasonably speculated that Zea mays root fibres can be considered as an efficient reinforcement for various matrices to produce attractive bio-composites. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

Effect of Heating and Citric Acid on the Performance of Cellulose Nanocrystal Thin Films

Emília Csiszár

Imola Herceg

and

Erika Fekete

Polymers 2023, 15(7), 1698; https://doi.org/10.3390/polym15071698 - 29 Mar 2023

Viewed by 599

Abstract

Cellulose nanocrystals (CNCs) were extracted from bleached cotton by sulfuric acid hydrolysis. Thin films were prepared from the aqueous suspension of CNCs by casting and evaporation with 15% glycerol as a plasticizer. Our research aimed to create stable films resistant to water. The structure and the interactions of the films were modified by short (10 min) heating at different temperatures (100, 140, and 160 °C) and by adding different amounts of citric acid (0, 10, 20, and 30%). Various analytical methods were used to determine the structure, surface properties, and mechanical properties. The interaction of composite films with water and water vapor was also investigated. Heat treatment did not significantly affect the film properties. Citric acid, without heat treatment, acted as a plasticizer. It promoted the disintegration of films in water, increased water vapor sorption, and reduced tensile strength, resulting in flexible and easy-to-handle films. The combination of heat treatment and citric acid resulted in stable liquid-water-resistant films with excellent mechanical properties. A minimum heating temperature of 120 °C and a citric acid concentration of 20% were required to obtain a stable CNC film structure resistant to liquid water. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

Influence of Accelerated Aging on the Fiber-Matrix Adhesion of Regenerated Cellulose Fiber-Reinforced Bio-Polyamide

Celia Katharina Falkenreck

Nicole Gemmeke

Jan-Christoph Zarges

and

Hans-Peter Heim

Polymers 2023, 15(7), 1606; https://doi.org/10.3390/polym15071606 - 23 Mar 2023

Viewed by 583

Abstract

With regard to the sustainability and biological origin of plastic components, regenerated cellulose fiber (RCF)-reinforced polymers are expected to replace other composites in the future. For use under severe conditions, for example, as a housing in the engine compartment, the resistance of the composites and the impact on the fiber and fiber-matrix adhesion must be investigated. Composites of bio-polyamide with a reinforcement of 20 wt.% RCF were compounded using a twin-screw extruder. The test specimens were manufactured with an injection molding machine and aged under conditions of high humidity at 90% r. H, a high temperature of 70 °C, and water storage using a water temperature of 23 °C for 504 h. Mechanical tests, single-fiber tensile tests (SFTT), single-fibre pull-out tests (SFPT), and optical characterization revealed significant changes in the properties of the composites. The results of the SFPT show that accelerated aging had a significant effect on the bio-polymer and an even stronger effect on the fiber, as the single-fiber tensile strength decreased by 27.5%. Supplementary notched impact strength tests revealed a correlation of the impact strength and the accelerated aging of the RCF-reinforced composites. In addition, it could be verified that the tensile strength also decreased at about 37% due to the aging effect on the RCF and a lowered fiber-matrix adhesion. The largest aging impact was on the Young’s modulus with a decrease of 45% due to the accelerated aging. In summary, the results show that the strengthening effect with 20 wt.% RCF was highly decreased subsequent to the accelerated aging due to hydrolysis and debonding because of the shrinkage and swelling of the matrix and fiber. These scientific findings are essential, as it is important to ensure that this bio-based material used in the automotive sector can withstand these stresses without severe degradation. This study provides information about the aging behavior of RCF-reinforced bio-based polyamide, which provides fundamental insights for future research. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

Preventing the Collapse Behavior of Polyurethane Foams with the Addition of Cellulose Nanofiber

and

Polymers 2023, 15(6), 1499; https://doi.org/10.3390/polym15061499 - 17 Mar 2023

Viewed by 903

Abstract

Polyurethane foam manufacturing depends on its materials and processes. A polyol that contains primary alcohol is very reactive with isocyanate. Sometimes, this may cause unexpected problems. In this study, a semi-rigid polyurethane foam was fabricated; however, its collapse occurred. The cellulose nanofiber was fabricated to solve this problem, and a weight ratio of 0.25, 0.5, 1, and 3% (based on total parts per weight of polyols) of the nanofiber was added to the polyurethane foams. The effect of the cellulose nanofiber on the polyurethane foams’ rheological, chemical, morphological, thermal, and anti-collapse performances was analyzed. The rheological analysis showed that 3 wt% of the cellulose nanofiber was unsuitable because of the aggregation of the filler. It was observed that the addition of the cellulose nanofiber showed the improved hydrogen bonding of the urethane linkage, even if it was not chemically reacted with the isocyanate groups. Moreover, due to the nucleating effect of the cellulose nanofiber, the average cell area of the produced foams decreased according to the amount of the cellulose nanofiber present, and the average cell area especially was reduced about five times when it contained 1 wt% more of the cellulose nanofiber than the neat foam. Although the thermal stability declined slightly, the glass transition temperature shifted from 25.8 °C to 37.6, 38.2, and 40.1 °C by when the cellulose nanofiber increased. Furthermore, the shrinkage ratio after 14 days from the foaming (%_shrinkage) of the polyurethane foams decreased 15.4 times for the 1 wt% cellulose nanofiber polyurethane composite. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

High-Performance Cladophora-Algae-Based Paper for Honeycomb Core in Sandwich-Structured Composite: Preparation and Characterizations

and

Polymers 2023, 15(6), 1359; https://doi.org/10.3390/polym15061359 - 09 Mar 2023

Viewed by 931

Abstract

Cellulose is classified as one of the most abundant biopolymers in nature. Its excellent properties have gained a lot of interest as an alternative material for synthetic polymers. Nowadays, cellulose can be processed into numerous derivative products, such as microcrystalline cellulose (MCC) and nanocrystalline cellulose (NCC). MCC and NCC have demonstrated outstanding mechanical properties owing to their high degree of crystallinity. One of the promising applications of MCC and NCC is high-performance paper. It can be utilized as a substitute for the aramid paper that has been commercially used as a honeycomb core material for sandwich-structured composites. In this study, MCC and NCC were prepared by extracting cellulose from the Cladophora algae resource. MCC and NCC possessed different characteristics because of their distinct morphologies. Furthermore, MCC and NCC were formed into a paper at various grammages and then impregnated with epoxy resin. The effect of paper grammage and epoxy resin impregnation on the mechanical properties of both materials was studied. Then, MCC and NCC paper was prepared as a raw material for honeycomb core applications. The results showed that epoxy-impregnated MCC paper outperformed epoxy-impregnated NCC paper with a compression strength of 0.72 MPa. The interesting result from this study is that the compression strength of the MCC-based honeycomb core was comparable to the commercial ones despite being made of a natural resource, which is sustainable and renewable. Therefore, cellulose-based paper is promising to be used for honeycomb core applications in sandwich-structured composites. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

Investigating Variation in Compressional Behavior of a Ternary Mixture from a Plastic, Elastic and Brittle Fracture Perspective in the Context of Optimum Composition of a Pharmaceutical Blend

Hiba Hani Mohammed Ali

Faisal Al-Akayleh

Abdel Hadi Al Jafari

and

Iyad Rashid

Polymers 2023, 15(5), 1063; https://doi.org/10.3390/polym15051063 - 21 Feb 2023

Viewed by 738

Abstract

The choice of optimum composition of a mixture of binary and ternary excipients for optimum compressional properties was investigated in this work. Excipients were chosen based on three types of excipients: plastic, elastic, and brittle fracture. Mixture compositions were selected based on a one-factor experimental design using the response surface methodology technique. Compressive properties comprising Heckel and Kawakita parameters, work of compression, and tablet hardness were measured as the main responses of this design. The one-factor RSM analysis revealed that there exist specific mass fractions that are associated with optimum responses for binary mixtures. Furthermore, the RSM analysis of the ‘mixture’ design type for the three components revealed a region of optimal responses around a specific composition. The foregoing had a mass ratio of 80:15:5 for microcrystalline cellulose: starch: magnesium silicate, respectively. Upon comparison using all RSM data, ternary mixtures were found to perform better in compression and tableting properties than binary mixtures. Finally, the finding of an optimal mixture composition has proven effective in its applicability in the context of the dissolution of model drugs (metronidazole and paracetamol). Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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Open AccessArticle

In Vivo Modification of Microporous Structure in Bacterial Cellulose by Exposing Komagataeibacter xylinus Culture to Physical and Chemical Stimuli

Yolanda González-García

Juan C. Meza-Contreras

José A. Gutiérrez-Ortega

and

Ricardo Manríquez-González

Polymers 2022, 14(20), 4388; https://doi.org/10.3390/polym14204388 - 18 Oct 2022

Viewed by 980

Abstract

Bacterial cellulose (BC) samples were obtained in a static culture of K. xylinus under the effect of a low-intensity magnetic field, UV light, NaCl, and chloramphenicol. The effect of such stimuli on the amount of BC produced and its production rate, specific area, pore volume, and pore diameter were evaluated. The polysaccharide production was enhanced 2.28-fold by exposing K. xylinus culture to UV light (366 nm) and 1.7-fold by adding chloramphenicol (0.25 mM) to the medium in comparison to BC control. All the stimuli triggered a decrease in the rate of BC biosynthesis. BC membranes were found to be mesoporous materials with an average pore diameter from 21.37 to 25.73 nm. BC produced under a magnetic field showed the lowest values of specific area and pore volume (2.55 m² g⁻¹ and 0.024 cm³ g⁻¹), while the BC synthesized in the presence of NaCl showed the highest (15.72 m² g⁻¹ and 0.11 cm³ g⁻¹). FTIR spectra of the BC samples also demonstrated changes related to structural order. The rehydration property in these BC samples is not mainly mediated by the crystallinity level or porosity. In summary, these results support that BC production, surface, and structural properties could be modified by manipulating the physical and chemical stimuli investigated. Full article

(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)

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