Advances in Cellulose-Based Polymers and Composites

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Circular and Green Polymer Science".

Deadline for manuscript submissions: closed (25 March 2024) | Viewed by 30503

Special Issue Editors


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Guest Editor
Petru Poni Institute of Macromolecular Chemistry, Grigore Ghica Voda Alley 41A, 700487 Iasi, Romania
Interests: polymer surface functionalization by various methods; cellulosic materials; bioactive materials (active, bioactive, smart, and (bio)degradable); polymer blends and composites; physico-chemical characterization
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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
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

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

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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

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

Published Papers (21 papers)

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Research

15 pages, 2830 KiB  
Article
Active Cellulose-Based Food Packaging and Its Use on Foodstuff
by Anamaria Irimia, Vasile Cristian Grigoraș and Carmen-Mihaela Popescu
Polymers 2024, 16(3), 389; https://doi.org/10.3390/polym16030389 - 31 Jan 2024
Viewed by 889
Abstract
The essential role of active packaging is food quality improvement, which results in an extension of shelf life. Active packaging can also further enhance distribution from the origin point, and contributes to food waste reduction, offering greater sustainability. In this study, we introduced [...] Read more.
The essential role of active packaging is food quality improvement, which results in an extension of shelf life. Active packaging can also further enhance distribution from the origin point, and contributes to food waste reduction, offering greater sustainability. In this study, we introduced a new method for obtaining cellulose-based active packages, combining gamma irradiation as an eco-friendly activation process, and clove essential oil and cold-pressed rosehip seed oil as bioactive agents. Newly obtained bioactive materials were evaluated to assess their structural, hydrophobic, and morphological properties, thermal stability, and antioxidant and antimicrobial properties. The results showed that the plant oils induced their antimicrobial effects on paper, using both in vitro tests, against several bacterial strains (Gram-positive bacteria Listeria monocytogenes and Gram-negative bacteria Salmonella enteritidis and Escherichia coli), and in vivo tests, on fresh cheese curd and beef. Moreover, these oils can help control foodborne pathogens, which leads to extended shelf life. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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16 pages, 10870 KiB  
Article
Compatibilization of Cellulose Nanocrystal-Reinforced Natural Rubber Nanocomposite by Modified Natural Rubber
by Punyarat Jantachum and Pranee Phinyocheep
Polymers 2024, 16(3), 363; https://doi.org/10.3390/polym16030363 - 29 Jan 2024
Viewed by 672
Abstract
Due to global warming and environmental concerns, developing a fully bio-based nanocomposite is an attractive issue. In this work, the cellulose nanocrystals (CNCs) extracted from Luffa cylindrica, a renewable resource, were explored as a bio-based reinforcing filler in natural rubber (NR) nanocomposites. [...] Read more.
Due to global warming and environmental concerns, developing a fully bio-based nanocomposite is an attractive issue. In this work, the cellulose nanocrystals (CNCs) extracted from Luffa cylindrica, a renewable resource, were explored as a bio-based reinforcing filler in natural rubber (NR) nanocomposites. In addition, modified natural rubber was explored as a potential compatibilizer to assist the filler dispersion in the rubber nanocomposite. The effect of the CNC content (0–15 phr) on cure characteristics and the mechanical, dynamic, and thermal properties of NR/CNC nanocomposites was investigated. The results showed that the scorch time and cure time of the nanocomposites increased with increased CNC contents. The optimum tensile strength of NR nanocomposites having 5 phr of the CNC (NR-CNC5) was 20.60% higher than the corresponding unfilled NR vulcanizate, which was related to the increased crosslink density of the rubber nanocomposite. The incorporation of oxidized-degraded NR (ODNR) as a compatibilizer in the NR-CNC5 nanocomposite exhibited a considerably reduced cure time, which will lead to energy conservation during production. Moreover, the cure rate index of NR-CNC5-ODNR is much higher than using a petroleum-based silane coupling agent (Si69) as a compatibilizer in the NR-CNC5 nanocomposite. The good filler dispersion in the NR-CNC5 nanocomposite compatibilized by ODNR is comparable to the use of Si69, evidenced by scanning electron microscopy. There is, therefore, a good potential for the use of modified NR as a bio-based compatibilizer for rubber nanocomposites. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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16 pages, 3407 KiB  
Article
Cation-Selective Actuator–Sensor Response of Microcrystalline Cellulose Multi-Walled Carbon Nanotubes of Different Electrolytes Using Propylene Carbonate Solvent
by Fred Elhi, Quoc Bao Le and Rudolf Kiefer
Polymers 2024, 16(3), 339; https://doi.org/10.3390/polym16030339 - 26 Jan 2024
Viewed by 702
Abstract
Microcrystalline cellulose (MC) with 50 wt.% multi-walled carbon nanotube (MCNT) composites is obtained through extrusion, forming MC-MCNT fiber. In this study, we concentrate on three different electrolytes in propylene carbonate (PC) which have the same anions (TF, trifluoro-methanesulfonate CF3SO [...] Read more.
Microcrystalline cellulose (MC) with 50 wt.% multi-walled carbon nanotube (MCNT) composites is obtained through extrusion, forming MC-MCNT fiber. In this study, we concentrate on three different electrolytes in propylene carbonate (PC) which have the same anions (TF, trifluoro-methanesulfonate CF3SO3) but different cations, EDMI+ (1-ethyl-2,3-dimethylimidazolium), Li+ (lithium ion), and TBA+ (tetrabutylammonium). Cyclic voltammetry and square wave potential steps, in combination with linear actuation measurements in a potential range of 0.7 V to −0.2 V, were conducted. Our goal in this work was to establish a cation-selective actuator–sensor device capable of distinguishing different cations. The linear actuation of MC-MCNT fiber had its main expansion at discharge due to the incorporation of TF in the MC-MCNT fiber with the cations. In the following order, TBA+ > EDMI+ > Li+ had the best stress, strain, charge density, diffusion coefficients, and long-term stability. Chronopotentiometric measurements revealed that the cations in the PC solvent can be differentiated by their ion sizes. Further characterization of the MC-MCNT fiber was completed using scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and FTIR and Raman spectroscopy. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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15 pages, 5399 KiB  
Article
Influence of Partially Carboxylated Powdered Lignocellulose from Oat Straw on Technological and Strength Properties of Water-Swelling Rubber
by Elena Cherezova, Yulia Karaseva, Abdirakym Nakyp, Airat Nuriev, Bakytbek Islambekuly and Nurgali Akylbekov
Polymers 2024, 16(2), 282; https://doi.org/10.3390/polym16020282 - 19 Jan 2024
Viewed by 666
Abstract
The work is aimed at the development of an energy-saving technique involving the partial carboxylation of powdered lignocellulose products from the straw of annual agricultural plants and the use of the obtained products in rubber compositions as a water-swelling filler. Lignocellulose powder from [...] Read more.
The work is aimed at the development of an energy-saving technique involving the partial carboxylation of powdered lignocellulose products from the straw of annual agricultural plants and the use of the obtained products in rubber compositions as a water-swelling filler. Lignocellulose powder from oat straw (composition: α-cellulose—77.0%, lignin—3.8%, resins and fats—1.8%) was used for carboxylation without preliminary separation into components. Microwave radiation was used to activate the carboxylation process. This reduced the reaction time by 2–3 times. The synthesized products were analyzed by IR spectroscopy, thermogravimetry and scanning electron microscopy. Industrial product sodium carboxymethylcellulose (Na-CMC) was used as a swelling filler for comparison. The swelling fillers were fractionated by the sieve method; particles with the size of 0–1 mm were used for filling rubber compounds. The amount of swelling filler was 150 parts per 100 parts of rubber (phr). Due to the high filling of rubber compounds, plasticizer Oxal T-92 was added to the composition of a number of samples to facilitate the processing and uniform distribution of ingredients. The rubber composition was prepared in two stages. In the first stage, ingredients without swelling filler were mixed with rubber on a laboratory two-roll mill to create a base rubber compound (BRC). In the second stage, the BRC was mixed with the swelling filler in a closed laboratory plasti-corder rubber mixer, the Brabender Plasti-Corder® Lab-Station. Vulcanization was carried out at 160 °C. For the obtained samples, the physical-mechanical and sorption properties were determined. It has been shown that the carboxylated powdered lignocellulose from oat straw increases the strength properties of rubber in comparison with Na-CMC. It has been shown that when the carboxylated powdered lignocellulose from oat straw is introduced into the rubber composition, the degree of rubber swelling in aqueous solutions of various mineralizations increases by 50 and 100% in comparison with a noncarboxylated lignocellulose. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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20 pages, 7875 KiB  
Article
Simultaneous Production of Cellulose Nitrates and Bacterial Cellulose from Lignocellulose of Energy Crop
by Ekaterina I. Kashcheyeva, Anna A. Korchagina, Yulia A. Gismatulina, Evgenia K. Gladysheva, Vera V. Budaeva and Gennady V. Sakovich
Polymers 2024, 16(1), 42; https://doi.org/10.3390/polym16010042 - 21 Dec 2023
Cited by 1 | Viewed by 1001
Abstract
This study is focused on exploring the feasibility of simultaneously producing the two products, cellulose nitrates (CNs) and bacterial cellulose (BC), from Miscanthus × giganteus. The starting cellulose for them was isolated by successive treatments of the feedstock with HNO3 and [...] Read more.
This study is focused on exploring the feasibility of simultaneously producing the two products, cellulose nitrates (CNs) and bacterial cellulose (BC), from Miscanthus × giganteus. The starting cellulose for them was isolated by successive treatments of the feedstock with HNO3 and NaOH solutions. The cellulose was subjected to enzymatic hydrolysis for 2, 8, and 24 h. The cellulose samples after the hydrolysis were distinct in structure from the starting sample (degree of polymerization (DP) 1770, degree of crystallinity (DC) 64%) and between each other (DP 1510–1760, DC 72–75%). The nitration showed that these samples and the starting cellulose could successfully be nitrated to furnish acetone-soluble CNs. Extending the hydrolysis time from 2 h to 24 h led to an enhanced yield of CNs from 116 to 131%, with the nitrogen content and the viscosity of the CN samples increasing from 11.35 to 11.83% and from 94 to 119 mPa·s, respectively. The SEM analysis demonstrated that CNs retained the fiber shape. The IR spectroscopy confirmed that the synthesized material was specifically CNs, as evidenced by the characteristic frequencies of 1657–1659, 1277, 832–833, 747, and 688–690 cm−1. Nutrient media derived from the hydrolyzates obtained in 8 h and 24 h were of good quality for the synthesis of BC, with yields of 11.1% and 9.6%, respectively. The BC samples had a reticulate structure made of interlaced microfibrils with 65 and 81 nm widths and DPs of 2100 and 2300, respectively. It is for the first time that such an approach for the simultaneous production of CNs and BC has been employed. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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16 pages, 8645 KiB  
Article
The Effect of Cellulose Nanocrystal-Based Nanofluid on Milling Performance: An Investigation of Dillimax 690T
by Üsame Ali Usca
Polymers 2023, 15(23), 4521; https://doi.org/10.3390/polym15234521 - 24 Nov 2023
Cited by 3 | Viewed by 738
Abstract
Machining high-strength structural steels often requires challenging processes. It is essential to improve the machinability of such materials, which are frequently needed in industrial manufacturing areas. Recently, it has become necessary to enhance the machinability of such materials using different nanopowders. In this [...] Read more.
Machining high-strength structural steels often requires challenging processes. It is essential to improve the machinability of such materials, which are frequently needed in industrial manufacturing areas. Recently, it has become necessary to enhance the machinability of such materials using different nanopowders. In this study, different cooling/lubricating (C/L) liquids were prepared with cellulose nanocrystal (CNC) nanopowder. The aim was to improve the machinability properties of Dillimax 690T material with the prepared CNC-based cutting fluids. CNC nanopowders were added to 0.5% distilled water by volume, and a new nanofluid was produced. Unlike previous studies, base synthetic oil and CNC-based cutting fluid were sprayed on the cutting area with a double minimum quantity lubrication (MQL) system. Machinability tests were carried out by milling. Two different cutting speeds (Vc = 120–150 m/min), two different feed rates (f = 0.05–0.075 mm/tooth), and four different C/L environments (dry, MQL oil, CNC nanofluid, MQL oil + CNC nanofluid) were used in the experiments. In the study, where a total of 16 experiments were performed, cutting temperature (Tc), surface roughness (Ra), tool wear (Vb), and energy consumption results were analyzed in detail. According to the test results, significant improvements were achieved in the machinability properties of the material in the experiments carried out using CNC nanofluid. In particular, the hybrid C/L environment using MQL oil + CNC nanofluid improved all machinability metrics by over 15% compared to dry machining. In short, using CNC nanopowders offers a good milling process of Dillimax 690T material with effective lubrication and cooling ability. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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16 pages, 11428 KiB  
Article
Active Contraction in the Stable Mechanical Environment of the Tunic of the Ascidian, Halocynthia roretzi, a Polysaccharide-Based Tissue with Blood Circulatory System
by Yoko Kato
Polymers 2023, 15(21), 4329; https://doi.org/10.3390/polym15214329 - 05 Nov 2023
Viewed by 933
Abstract
Halocynthia roretzi, a member of Ascidiacea, is covered with its own tunic, which is composed of polysaccharides, such as cellulose Iβ and sulfated chitin. H. roretzi has an open-vessel system, whose blood vessels and hemocytes are found in the tunic, so that [...] Read more.
Halocynthia roretzi, a member of Ascidiacea, is covered with its own tunic, which is composed of polysaccharides, such as cellulose Iβ and sulfated chitin. H. roretzi has an open-vessel system, whose blood vessels and hemocytes are found in the tunic, so that the mechanical environment of the tunic could be carefully controlled because of its influence on hemocyte behaviors. While active deformation of the tunic and related phenomena have been previously reported, the mechanical environment in the tunic, which directly influences its deformation, has been rarely investigated. Meanwhile, the developments of actuators based on cellulose and chitin have been frequently reported. However, a cellulose–sulfated chitin actuator has not been proposed. In this study, the mechanical environment of the tunic, which has been rarely investigated despite its importance in the active deformation of the tunic, was evaluated using finite element analysis. A finite element model of the tunic, based on its histological characteristics as well as deformation patterns, was developed. The results showed that the shape of the tunic, the pattern of fiber distribution, and control of the water content influenced the mechanical environment. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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16 pages, 5002 KiB  
Article
Characterization of Cellulose Fiber Derived from Hemp and Polyvinyl Alcohol-Based Composite Hydrogel as a Scaffold Material
by Praewa Promdontree, Pakpoom Kheolamai, Artjima Ounkaew, Ravin Narain and Sarute Ummartyotin
Polymers 2023, 15(20), 4098; https://doi.org/10.3390/polym15204098 - 16 Oct 2023
Viewed by 1251
Abstract
Cellulose nanocrystals (CNCs) were successfully extracted and purified from hemp using an alkaline treatment and bleaching process and subsequently used in conjunction with polyvinyl alcohol to form a composite hydrogel. Cellulose nanocrystals (1–10% (w/v)) were integrated into polyvinyl alcohol, [...] Read more.
Cellulose nanocrystals (CNCs) were successfully extracted and purified from hemp using an alkaline treatment and bleaching process and subsequently used in conjunction with polyvinyl alcohol to form a composite hydrogel. Cellulose nanocrystals (1–10% (w/v)) were integrated into polyvinyl alcohol, and sodium tetraborate (borax) was employed as a crosslinking agent. Due to the small number of cellulose nanocrystals, no significant peak change was observed in the FT-IR spectra compared to pristine polyvinyl alcohol. The porosity was created upon the removal of the water molecules, and the material was thermally stable up to 200 °C. With the presence of cellulose nanocrystals, the melting temperature was slightly shifted to a higher temperature, while the glass transition temperature remained practically unchanged. The swelling behavior was examined for 180 min in deionized water and PBS solution (pH 7.4) at 37 °C. The degree of swelling of the composite with cellulose nanocrystals was found to be higher than that of pristine PVA hydrogel. The cell viability (%) of the prepared hydrogel with different proportions of cellulose nanocrystals was higher than that of pristine PVA hydrogel. Based on the results, the prepared composite hydrogels from cellulose nanocrystals extracted from hemp and polyvinyl alcohol were revealed to be an excellent candidate for scaffold material for medical usage. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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22 pages, 7095 KiB  
Article
Antimicrobial Wound Dressings based on Bacterial Cellulose and Independently Loaded with Nutmeg and Fir Needle Essential Oils
by Georgiana-Madalina Lemnaru (Popa), Ludmila Motelica, Roxana Doina Trusca, Cornelia Ioana Ilie, Alexa-Maria Croitoru, Denisa Ficai, Ovidiu Oprea, Anicuta Stoica-Guzun, Anton Ficai, Lia-Mara Ditu and Bianca-Maria Tihăuan
Polymers 2023, 15(17), 3629; https://doi.org/10.3390/polym15173629 - 01 Sep 2023
Cited by 1 | Viewed by 1399
Abstract
The aim of the present study was to obtain antimicrobial dressings from bacterial cellulose loaded with nutmeg and of fir needle essential oils. The attractive properties of BC, such as biocompatibility, good physicochemical and mechanical stability, and high water absorption, led to the [...] Read more.
The aim of the present study was to obtain antimicrobial dressings from bacterial cellulose loaded with nutmeg and of fir needle essential oils. The attractive properties of BC, such as biocompatibility, good physicochemical and mechanical stability, and high water absorption, led to the choice of this material to be used as a support. Essential oils have been added to provide antimicrobial properties to these dressings. The results confirmed the presence of oils in the structure of the bacterial cellulose membrane and the ability of the materials to inhibit the adhesion of Staphylococcus aureus and Escherichia coli. By performing antibacterial tests on membranes loaded with fir needle essential oil, we demonstrated the ability of these membranes to inhibit bacterial adhesion to the substrate. The samples loaded with nutmeg essential oil exhibited the ability to inhibit the adhesion of bacteria to the surface of the materials, with the 5% sample showing a significant decrease. The binding of essential oils to the membrane was confirmed by thermal analysis and infrared characterization. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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17 pages, 3768 KiB  
Article
Facile Hydrothermal Synthesis of Ag/Fe3O4/Cellulose Nanocomposite as Highly Active Catalyst for 4-Nitrophenol and Organic Dye Reduction
by An Nang Vu, Hoa Ngoc Thi Le, Thang Bach Phan and Hieu Van Le
Polymers 2023, 15(16), 3373; https://doi.org/10.3390/polym15163373 - 11 Aug 2023
Cited by 2 | Viewed by 994
Abstract
Novel effluent treatment solutions for dangerous organic pollutants are crucial worldwide. In recent years, chemical reduction using noble metal-based nanocatalysts and NaBH4, a reducing agent, has become common practice for eliminating organic contaminants from aquatic environments. We suggest a straightforward approach [...] Read more.
Novel effluent treatment solutions for dangerous organic pollutants are crucial worldwide. In recent years, chemical reduction using noble metal-based nanocatalysts and NaBH4, a reducing agent, has become common practice for eliminating organic contaminants from aquatic environments. We suggest a straightforward approach to synthesizing magnetic cellulose nanocrystals (CNCs) modified with magnetite (Fe3O4) and silver nanoparticles (Ag NPs) as a catalyst for organic contamination removal. Significantly, the CNC surface was decorated with Ag NPs without using any reducing agents or stabilizers. PXRD, FE-SEM, TEM, EDX, VSM, BET, and zeta potential tests characterized the Ag/Fe3O4/CNC nanocomposite. The nanocomposite’s catalytic activity was tested by eliminating 4-nitrophenol (4-NP) and the organic dyes methylene blue (MB) and methyl orange (MO) in an aqueous solution at 25 °C. The Ag/Fe3O4/CNC nanocomposite reduced 4-NP and decolored these hazardous organic dyes in a short time (2 to 5 min) using a tiny amount of catalyst (2.5 mg for 4-NP and 15 mg for MO and MB). The magnetic catalyst was removed and reused three times without losing catalytic activity. This work shows that the Ag/Fe3O4/CNC nanocomposite can chemically reduce harmful pollutants in effluent for environmental applications. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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11 pages, 1291 KiB  
Article
Comparative Study on the Stiffness of Poly(lactic acid) Reinforced with Untreated and Bleached Hemp Fibers
by Roberto J. Aguado, Gabriela A. Bastida, Francisco X. Espinach, Joan Llorens, Quim Tarrés, Marc Delgado-Aguilar and Pere Mutjé
Polymers 2023, 15(13), 2960; https://doi.org/10.3390/polym15132960 - 06 Jul 2023
Cited by 1 | Viewed by 1088
Abstract
Composite materials containing natural reinforcement fibers, generally called biocomposites, have attracted the interest of both researchers and manufacturers, but the most environmentally advantageous combinations include a bio-based matrix, as well. With this in mind, a poly(lactic acid) (PLA) matrix was reinforced with natural [...] Read more.
Composite materials containing natural reinforcement fibers, generally called biocomposites, have attracted the interest of both researchers and manufacturers, but the most environmentally advantageous combinations include a bio-based matrix, as well. With this in mind, a poly(lactic acid) (PLA) matrix was reinforced with natural fibers from hemp, both untreated strands (UHSs) and soda-bleached fibers (SBHFs). The preparation of the subsequent fully bio-sourced, discontinuously reinforced composites involved kinetic mixing, intensive single-screw extrusion, milling, and injection molding. Up to a fiber content of 30 wt%, the tensile modulus increased linearly with the volume fraction of the dispersed phase. Differences between SBHFs (up to 7.6 Gpa) and UHSs (up to 6.9 Gpa) were hardly significant (p = 0.1), but SBHF-reinforced composites displayed higher strain at failure. In any case, for the same fiber load (30 wt%), the Young’s modulus of PLA/hemp biocomposites was greater than that of glass fiber (GF)-reinforced polypropylene (5.7 GPa), albeit lower than that of PLA/GF (9.8 GPa). Considering all the measurements, the contribution of each phase was analyzed by applying the Hirsch model and the Tsai-Pagano model. As a concluding remark, although the intrinsic tensile modulus of SBHFs was lower than that of GF, the efficiency of those natural fibers as reinforcement (according to the rule of mixtures) was found to be higher. Full article
(This article belongs to the Special Issue Advances in Cellulose-Based Polymers and Composites)
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19 pages, 6972 KiB  
Article
Oil Media on Paper: Investigating the Interaction of Cold-Pressed Linseed Oil with Paper Supports with FTIR Analysis
by 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
Cited by 1 | Viewed by 1497
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, [...] Read more.
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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13 pages, 7824 KiB  
Article
Thiol-Surface-Engineered Cellulose Nanocrystals in Favor of Copper Ion Uptake
by Trung Dang-Bao, Thi-My-Chau Nguyen, Gia-Han Hoang, Hoa-Hung Lam, Hong-Phuong Phan and Thi-Kieu-Anh Tran
Polymers 2023, 15(11), 2562; https://doi.org/10.3390/polym15112562 - 02 Jun 2023
Cited by 3 | Viewed by 1220
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 [...] Read more.
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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11 pages, 1952 KiB  
Article
Development of New Accelerated Aging Test for Comparison of the Quality of Different Insulating Papers Based on Cellulose
by Draginja Mihajlovic, Valentina Vasovic and Jelena Lukic
Polymers 2023, 15(11), 2556; https://doi.org/10.3390/polym15112556 - 01 Jun 2023
Viewed by 1092
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 [...] Read more.
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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21 pages, 6009 KiB  
Article
Investigation on Properties of Raw and Alkali Treated Novel Cellulosic Root Fibres of Zea Mays for Polymeric Composites
by 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 17 | Viewed by 1820
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 [...] Read more.
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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15 pages, 6308 KiB  
Article
Effect of Heating and Citric Acid on the Performance of Cellulose Nanocrystal Thin Films
by Emília Csiszár, Imola Herceg and Erika Fekete
Polymers 2023, 15(7), 1698; https://doi.org/10.3390/polym15071698 - 29 Mar 2023
Viewed by 1906
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 [...] Read more.
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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18 pages, 8417 KiB  
Article
Influence of Accelerated Aging on the Fiber-Matrix Adhesion of Regenerated Cellulose Fiber-Reinforced Bio-Polyamide
by 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
Cited by 3 | Viewed by 1507
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 [...] Read more.
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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13 pages, 3184 KiB  
Article
Preventing the Collapse Behavior of Polyurethane Foams with the Addition of Cellulose Nanofiber
by Sanghyeon Ju, Ajeong Lee, Youngeun Shin, Hyekyeong Jang, Jin-Woo Yi, Youngseok Oh, Nam-Ju Jo and Teahoon Park
Polymers 2023, 15(6), 1499; https://doi.org/10.3390/polym15061499 - 17 Mar 2023
Cited by 2 | Viewed by 3491
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 [...] Read more.
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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16 pages, 18382 KiB  
Article
High-Performance Cladophora-Algae-Based Paper for Honeycomb Core in Sandwich-Structured Composite: Preparation and Characterizations
by Yati Mardiyati, Anna Niska Fauza, Steven Steven, Onny Aulia Rachman, Tatacipta Dirgantara and Arief Hariyanto
Polymers 2023, 15(6), 1359; https://doi.org/10.3390/polym15061359 - 09 Mar 2023
Viewed by 1811
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 [...] Read more.
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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13 pages, 1413 KiB  
Article
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
by 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 1470
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 [...] Read more.
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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14 pages, 1382 KiB  
Article
In Vivo Modification of Microporous Structure in Bacterial Cellulose by Exposing Komagataeibacter xylinus Culture to Physical and Chemical Stimuli
by 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
Cited by 1 | Viewed by 1696
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, [...] Read more.
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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