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Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials

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

Deadline for manuscript submissions: closed (20 July 2021) | Viewed by 33227

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Special Issue Editors

Prof. Dr. Mirta I. Aranguren

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Guest Editor

Instituto de Investigaciones en Ciencia y Tecnología de Materiales (INTEMA) and Facultad de Ingeniería, in Universidad Nacional de Mar del Plata (UNMdP) - Consejo Nacional de Investigaciones Científicas y Técnicas, Av. Juan B Justo 4302, 7600 Mar del Plata, Argentina
Interests: polymers; bio-based polymers; biocomposites; nanocellulose; bio-nanocomposites; applied rheology; vegetable-oil-based polymers; viscoelasticity

Prof. Dr. Maria Soledad Peresin

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Guest Editor

Forest Products Development Center, School of Forestry and Wildlife Science, Auburn University, Auburn, AL 36830, USA
Interests: nanocellulose; value-added products from biomass; surface chemistry and interfaces; colloids; nanocomposites; hydrogels; sensing and detection
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

During the last few decades, renewable resources have experienced a well-deserved revalorization in the field of new and advanced materials. This has served to uncover and highlight the remarkable properties and great availability of cellulose. The obtention of a variety of micro- and nanocelluloses has opened possibilities for the fabrication of materials with a wide range of applications, membranes, electronic supports, polymer reinforcement, optically active papers, films with added barrier properties, and biomedical materials, among others.

Because of the high mechanical properties of nanocelluloses together with their low density, they have been rapidly identified as efficient nanoreinforcements for polymeric matrices. Because of their properties, their incorporation in nanocomposites results in no darkening of the final materials and usually only a small reduction of the transparency, thanks to the small concentrations required to modify the material properties.

The capacity of cellulose nanocrystals to form liquid-crystal suspensions has also been investigated for the production of neat and nanocomposite materials with particular optical properties such as iridescence or photonic crystal behavior.

In this Special Issue, full original papers and comprehensive reviews will be considered in which the current developments in the preparation, characterization, and applications of nanocellulose materials and composites are addressed.

Prof. Dr. Mirta I. Aranguren
Dr. Soledad Peresin
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 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

nanocellulose
nanocomposites
cellulose nanocrystals
nanofibrillar/microfibrillar cellulose
mechanical properties
functional properties
nanocellulose liquid crystals
barrier properties
aerogels
hydrogels

Published Papers (10 papers)

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Research

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17 pages, 3899 KiB

Open AccessArticle

Scaled Synthesis of Polyamine-Modified Cellulose Nanocrystals from Bulk Cotton and Their Use for Capturing Volatile Organic Compounds

by Beau R. Brummel, Chandima J. Narangoda, Mohamed F. Attia, Maria I. Swasy, Gary D. Smith, Jr., Frank Alexis and Daniel C. Whitehead

Polymers 2021, 13(18), 3060; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13183060 - 10 Sep 2021

Cited by 2 | Viewed by 2604

Abstract

We have previously demonstrated that cellulose nanocrystals modified with poly(ethylenimine) (PEI-f-CNC) are capable of capturing volatile organic compounds (VOCs) associated with malodors. In this manuscript, we describe our efforts to develop a scalable synthesis of these materials from bulk cotton. This work culminated in a reliable protocol for the synthesis of unmodified cellulose nanocrystals (CNCs) from bulk cotton on a 0.5 kg scale. Additionally, we developed a protocol for the modification of the CNCs by means of sequential 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) oxidation and 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloride (EDC) coupling to modify their surface with poly(ethylenimine) on a 100 g scale. Subsequently, we evaluated the performance of the PEI-f-CNC materials that were prepared in a series of VOC capture experiments. First, we demonstrated their efficacy in capturing volatile fatty acids emitted at a rendering plant when formulated as packed-bed filter cartridges. Secondly, we evaluated the potential to use aqueous PEI-f-CNC suspensions as a spray-based delivery method for VOC remediation. In both cases, the PEI-f-CNC formulations reduced detectable malodor VOCs by greater than 90%. The facile scaled synthesis of these materials and their excellent performance at VOC remediation suggest that they may emerge as a useful strategy for the remediation of VOCs associated with odor. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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17 pages, 3622 KiB

Open AccessArticle

Nanocelluloses Reinforced Bio-Waterborne Polyurethane

by M. E. Victoria Hormaiztegui, Diana Marin, Piedad Gañán, Pablo Marcelo Stefani, Verónica Mucci and Mirta I. Aranguren

Polymers 2021, 13(17), 2853; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13172853 - 25 Aug 2021

Cited by 6 | Viewed by 2371

Abstract

The aim of this work was to evaluate the influence of two kinds of bio- nano-reinforcements, cellulose nanocrystals (CNCs) and bacterial cellulose (BC), on the properties of castor oil-based waterborne polyurethane (WBPU) films. CNCs were obtained by the acidolysis of microcrystalline cellulose, while BC was produced from Komagataeibacter medellinensis. A WBPU/BC composite was prepared by the impregnation of a wet BC membrane and further drying, while the WBPU/CNC composite was obtained by casting. The nanoreinforcement was adequately dispersed in the polymer using any of the preparation methods, obtaining optically transparent compounds. Thermal gravimetric analysis, Fourier-transform infrared spectroscopy, field emission scanning electron microscopy, dynamical mechanical analysis, differential scanning calorimetry, contact angle, and water absorption tests were carried out to analyze the chemical, physical, and thermal properties, as well as the morphology of nanocelluloses and composites. The incorporation of nanoreinforcements into the formulation increased the storage modulus above the glass transition temperature of the polymer. The thermal stability of the BC-reinforced composites was slightly higher than that of the CNC composites. In addition, BC allowed maintaining the structural integrity of the composites films, when they were immersed in water. The results were related to the relatively high thermal stability and the particular three-dimensional interconnected reticular morphology of BC. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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17 pages, 6718 KiB

Open AccessArticle

Fully Bio-Based Elastomer Nanocomposites Comprising Polyfarnesene Reinforced with Plasma-Modified Cellulose Nanocrystals

by Ilse Magaña, Dimitrios Georgouvelas, Rishab Handa, María Guadalupe Neira Velázquez, Héctor Ricardo López González, Francisco Javier Enríquez Medrano, Ramón Díaz de León and Luis Valencia

Polymers 2021, 13(16), 2810; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13162810 - 21 Aug 2021

Cited by 4 | Viewed by 2882

Abstract

This article proposes a process to prepare fully bio-based elastomer nanocomposites based on polyfarnesene and cellulose nanocrystals (CNC). To improve the compatibility of cellulose with the hydrophobic matrix of polyfarnesene, the surface of CNC was modified via plasma-induced polymerization, at different powers of the plasma generator, using a trans-β-farnesene monomer in the plasma reactor. The characteristic features of plasma surface-modified CNC have been corroborated by spectroscopic (XPS) and microscopic (AFM) analyses. Moreover, the cellulose nanocrystals modified at 150 W have been selected to reinforce polyfarnesene-based nanocomposites, synthesized via an in-situ coordination polymerization using a neodymium-based catalytic system. The effect of the different loading content of nanocrystals on the polymerization behavior, as well as on the rheological aspects, was evaluated. The increase in the storage modulus with the incorporation of superficially modified nanocrystals was demonstrated by rheological measurements and these materials exhibited better properties than those containing pristine cellulose nanocrystals. Moreover, we elucidate that the viscoelastic moduli of the elastomer nanocomposites are aligned with power–law model systems with characteristic relaxation time scales similar to commercial nanocomposites, also implying tunable mechanical properties. In this foreground, our findings have important implications in the development of fully bio-based nanocomposites in close competition with the commercial stock, thereby producing alternatives in favor of sustainable materials. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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15 pages, 6384 KiB

Open AccessArticle

Surface Modification of Cellulose Nanocrystals with Lactone Monomers via Plasma-Induced Polymerization and Their Application in ABS Nanocomposites

by Ramón Díaz de León, Ediberto Guzmán, Ricardo López González, Alejandro Díaz Elizondo, Ilse Magaña, Guadalupe Neira, Adali Castañeda Facio and Luis Valencia

Polymers 2021, 13(16), 2699; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13162699 - 13 Aug 2021

Cited by 11 | Viewed by 2294

Abstract

The growing concern for environmental problems has motivated the use of materials obtained from bio-based resources such as cellulose nanocrystals which have a promising application acting as fillers or reinforcements of polymeric materials. In this context, in this article, plasma-induced polymerization is proposed as a strategy to modify nanocrystals at different plasma power intensities using ε-caprolactone and δ-decalactone to improve their compatibility with polymeric matrices. The characterization was carried out using techniques such as FTIR, TGA, XRD, XPS, and AFM, with which a successful functionalization was demonstrated without altering the inherent properties of the nanocrystals. The preparation of ABS nanocomposites was carried out with the modified nanoparticles and the evaluation of the mechanical properties indicates an increase in Young’s modulus and yield stress under certain concentrations of modified cellulose nanocrystals. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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13 pages, 5834 KiB

Open AccessArticle

Cellulose-Chitosan-Nanohydroxyapatite Hybrid Composites by One-Pot Synthesis for Biomedical Applications

by Katia Jarquin-Yáñez, Efrain Rubio-Rosas, Gabriela Piñón-Zárate, Andrés Castell-Rodríguez and Martha Poisot

Polymers 2021, 13(10), 1655; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13101655 - 19 May 2021

Cited by 1 | Viewed by 1904

Abstract

The development of organic–inorganic hybrid materials deserves special interest for bone tissue engineering applications, where materials must have properties that induce the survival and activation of cells derived from the mesenchyme. In this work, four bio-nanocomposites based on cellulose and variable content of chitosan, from 15 to 50 w% based on cellulose, with nanohydroxyapatite and β-Glycerophosphate as cross-linking agent were synthesized by simplified and low-energy-demanding solvent exchange method to determine the best ratio of chitosan to cellulose matrix. This study analyzes the metabolic activity and survival of human dermal fibroblast cells cultivated in four bio-nanocomposites based on cellulose and the variable content of chitosan. The biocompatibility was tested by the in vitro cytotoxicity assays Live/Dead and PrestoBlue. In addition, the composites were characterized by FTIR, XRD and SEM. The results have shown that the vibration bands of β-Glycerophosphate have prevailed over the other components bands, while new diffraction planes have emerged from the interaction between the cross-linking agent and the biopolymers. The bio-nanocomposite micrographs have shown no surface porosity as purposely designed. On the other hand, cell death and detachment were observed when the composites of 1 and 0.1 w/v% were used. However, the composite containing 10 w% chitosan, against the sum of cellulose and β-Glycerophosphate, has shown less cell death and detachment when used at 0.01 w/v%, making it suitable for more in vitro studies in bone tissue engineering, as a promising economical biomaterial. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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14 pages, 3324 KiB

Open AccessArticle

Effect of Cellulose Nanofibrils on the Properties of Jatropha Oil-Based Waterborne Polyurethane Nanocomposite Film

by Mohamad Ridzuan Amri, Chuah Teong Guan, Syeed Saifulazry Osman Al-Edrus, Faizah Md Yasin and Siti Fatahiyah Mohamad

Polymers 2021, 13(9), 1460; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13091460 - 30 Apr 2021

Cited by 13 | Viewed by 2373

Abstract

The objective of this work was to study the influence of cellulose nanofibrils (CNF) on the physical, mechanical, and thermal properties of Jatropha oil-based waterborne polyurethane (WBPU) nanocomposite films. The polyol to produce polyurethane was synthesized from crude Jatropha oil through epoxidation and ring-opening method. The chain extender, 1,6-hexanediol, was used to improve film elasticity by 0.1, 0.25, and 0.5 wt.% of CNF loading was incorporated to enhance film performance. Mechanical performance was studied using a universal test machine as specified in ASTM D638-03 Type V and was achieved by 0.18 MPa at 0.5 wt.% of CNF. Thermal gravimetric analysis (TGA) was performed to measure the temperature of degradation and the chemical crosslinking and film morphology were studied using Fourier-transform infrared spectroscopy (FTIR) and field emission scanning electron microscopy (FESEM). The results showed that when the CNF was incorporated, it was found to enhance the nanocomposite film, in particular its mechanical and thermal properties supported by morphology. Nanocomposite film with 0.5 wt.% of CNF showed the highest improvement in terms of tensile strength, Young’s modulus, and thermal degradation. Although the contact angle decreases as the CNF content increases, the effect on the water absorption of the film was found to be relatively small (<3.5%). The difference between the neat WPBU and the highest CNF loading film was not more than 1%, even after 5 days of being immersed in water. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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17 pages, 3406 KiB

Open AccessArticle

Bacterial Cellulose Network from Kombucha Fermentation Impregnated with Emulsion-Polymerized Poly(methyl methacrylate) to Form Nanocomposite

by Helena Oliver-Ortega, Shiyu Geng, Francesc Xavier Espinach, Kristiina Oksman and Fabiola Vilaseca

Polymers 2021, 13(4), 664; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13040664 - 23 Feb 2021

Cited by 18 | Viewed by 4018

Abstract

The use of bio-based residues is one of the key indicators towards sustainable development goals. In this work, bacterial cellulose, a residue from the fermentation of kombucha tea, was tested as a reinforcing nanofiber network in an emulsion-polymerized poly(methyl methacrylate) (PMMA) matrix. The use of the nanofiber network is facilitating the formation of nanocomposites with well-dispersed nanofibers without using organic solvents or expensive methodologies. Moreover, the bacterial cellulose network structure can serve as a template for the emulsion polymerization of PMMA. The morphology, size, crystallinity, water uptake, and mechanical properties of the kombucha bacterial cellulose (KBC) network were studied. The results showed that KBC nanofibril diameters were ranging between 20–40 nm and the KBC was highly crystalline, >90%. The 3D network was lightweight and porous material, having a density of only 0.014 g/cm³. Furthermore, the compressed KBC network had very good mechanical properties, the E-modulus was 8 GPa, and the tensile strength was 172 MPa. The prepared nanocomposites with a KBC concentration of 8 wt.% were translucent with uniform structure confirmed with scanning electron microscopy study, and furthermore, the KBC network was homogeneously impregnated with the PMMA matrix. The mechanical testing of the nanocomposite showed high stiffness compared to the neat PMMA. A simple simulation of the tensile strength was used to understand the limited strain and strength given by the bacterial cellulose network. The excellent properties of the final material demonstrate the capability of a residue of kombucha fermentation as an excellent nanofiber template for use in polymer nanocomposites. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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Review

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18 pages, 3100 KiB

Open AccessReview

Sustainable Development of Hot-Pressed All-Lignocellulose Composites—Comparing Wood Fibers and Nanofibers

by Erfan Oliaei, Tom Lindström and Lars A. Berglund

Polymers 2021, 13(16), 2747; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13162747 - 16 Aug 2021

Cited by 20 | Viewed by 5586

Abstract

Low-porosity materials based on hot-pressed wood fibers or nanocellulose fibrils (no polymer matrix) represent a new concept for eco-friendly materials with interesting mechanical properties. For the replacement of fossil-based materials, physical properties of wood fiber materials need to be improved. In addition, the carbon footprint and cumulative energy required to produce the material also needs to be reduced compared with fossil-based composites, e.g., glass fiber composites. Lignin-containing fibers and nanofibers are of high yield and special interest for development of more sustainable materials technologies. The present mini-review provides a short analysis of the potential. Different extraction routes of lignin-containing wood fibers are discussed, different processing methods, and the properties of resulting fiber materials. Comparisons are made with analogous lignin-containing nanofiber materials, where mechanical properties and eco-indicators are emphasized. Higher lignin content may promote eco-friendly attributes and improve interfiber or interfibril bonding in fiber materials, for improved mechanical performance. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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30 pages, 2774 KiB

Open AccessReview

Current Status of Cellulosic and Nanocellulosic Materials for Oil Spill Cleanup

by Siegfried Fürtauer, Mostafa Hassan, Ahmed Elsherbiny, Shaimaa A. Gabal, Sherif Mehanny and Hatem Abushammala

Polymers 2021, 13(16), 2739; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13162739 - 16 Aug 2021

Cited by 26 | Viewed by 4014

Abstract

Recent developments in the application of lignocellulosic materials for oil spill removal are discussed in this review article. The types of lignocellulosic substrate material and their different chemical and physical modification strategies and basic preparation techniques are presented. The morphological features and the related separation mechanisms of the materials are summarized. The material types were classified into 3D-materials such as hydrophobic and oleophobic sponges and aerogels, or 2D-materials such as membranes, fabrics, films, and meshes. It was found that, particularly for 3D-materials, there is a clear correlation between the material properties, mainly porosity and density, and their absorption performance. Furthermore, it was shown that nanocellulosic precursors are not exclusively suitable to achieve competitive porosity and therefore absorption performance, but also bulk cellulose materials. This finding could lead to developments in cost- and energy-efficient production processes of future lignocellulosic oil spillage removal materials. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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26 pages, 4253 KiB

Open AccessEditor’s ChoiceReview

A Review of Wet Compounding of Cellulose Nanocomposites

by Craig Clemons and Ronald Sabo

Polymers 2021, 13(6), 911; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13060911 - 16 Mar 2021

Cited by 13 | Viewed by 3648

Abstract

Cellulose nanomaterials (CNs) are an emerging class of materials with numerous potential applications, including as additives or reinforcements for thermoplastics. Unfortunately, the preparation of CNs typically results in dilute, aqueous suspensions, and the lack of efficient water removal methods has hindered commercialization. However, water may also present opportunities for improving overall efficiencies if its potential is better understood and if it is better managed through the various stages of CN and composite production. Wet compounding represents one such possible opportunity by leveraging water’s ability to aid in CN dispersion, act as a transport medium for metering and feeding of CNs, plasticize some polymers, or potentially facilitate the preparation of CNs during compounding. However, there are also considerable challenges and much investigation remains. Here, we review various wet compounding approaches used in the preparation of cellulose nanocomposites as well as the related concepts of wet feeding and wet extrusion fibrillation of cellulose. We also discuss potential opportunities, remaining challenges, and research and development needs with the ultimate goal of developing a more integrated approach to cellulose nanocomposite preparation and a more sophisticated understanding of water’s role in the compounding process. Full article

(This article belongs to the Special Issue Nanocellulose: Polymer Nanocomposites and all-Cellulose Materials)

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