Advanced Cellulose-Based Materials: From Nanoparticles to Complex Structures and Composites

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

Deadline for manuscript submissions: closed (30 November 2023) | Viewed by 13735

Special Issue Editor

Institute of Engineering Materials and Design, Faculty of Mechanical Engineering, University of Maribor, 2000 Maribor, Slovenia
Interests: biopolymers; medical textiles; modification and compounding of nanocellulose of bacterial and plant origin; microstructure; scaffolds; membranes; biomaterials for medicine; composite membranes for fuel cells
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Special Issue Information

Dear Colleagues,

Along with its supreme presence in Nature, cellulose holds versatile and renewable engineering material attributes that have gained momentum in many technological areas. The polymeric structure of cellulose consists of glucopyranose monomers, linearly polymerized by β-1,4-glycosidic linkages to varying degrees of polymerization among different origins. Its nano-forms (nanocrystals, nanofibrils) are types of intermediate products, obtained either by bottom-up bio-synthetic approaches (e.g., bacteria- or fungi-mediated fermentation) or top-down chemical and mechanical disintegration approaches applied to plants and trees. In both cases, the resulting nanocellulose delivers distinctive, well-documented features, making it a highly unique material family with an immense research portfolio.

Vast research enthusiasm is needed to unlock cellulose’s full potential as a sustainable building block to deliver materials surpassing the performance of its synthetic counterparts.

This Special Issue aims to attract publications with recent theoretical and experimental findings related to cellulose and nanocellulose isolation (top-down) or bio-processing (bottom-up), as well as its future manipulation in terms of selective modification, mixing, shaping and compounding with other non-cellulosic components in light of more demanding application niches. We welcome the submission of research and review papers delivering new data and collecting and critically commenting on recent publications, giving the future perspective in this attractive research area.

Dr. Selestina Gorgieva
Guest Editor

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Keywords

  • cellulose
  • nanocellulose: processing, modification and compounding
  • composites
  • applications: technical, medical, etc.
  • analysis
  • sustainability and recyclability of cellulose-containing composites

Published Papers (8 papers)

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Research

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12 pages, 4576 KiB  
Article
Powdered Cellulose Microblasting for Dry Cleaning Printed Works on Paper
by Iris Bautista-Morenilla, Cristina Ruiz-Recasens and Gema Campo-Francés
Polymers 2024, 16(2), 176; https://doi.org/10.3390/polym16020176 - 07 Jan 2024
Viewed by 602
Abstract
This study evaluates the practical feasibility of using powdered cellulose microblasting for dry cleaning paper-based printed artworks in a real setting of conservation treatment. The control parameters used for this purpose are the potential morphological changes in the surface, the level of cleanliness [...] Read more.
This study evaluates the practical feasibility of using powdered cellulose microblasting for dry cleaning paper-based printed artworks in a real setting of conservation treatment. The control parameters used for this purpose are the potential morphological changes in the surface, the level of cleanliness achieved, and the amount of residue remaining in the artwork after the treatment. In this study, cleaning of a lithography was conducted entirely with powdered cellulose microblasting. The outcomes were evaluated before and after treatment using optical microscopy, scanning electron microscopy, energy-dispersive X-ray spectroscopy, and spectrophotometry. The results indicate that powdered cellulose microblasting is a feasible and efficient technique for conducting the dry cleaning of printed works on paper without causing morphological changes to their surface. Additionally, it offers significant benefits by enabling precise treatment control, reducing cleaning time, and using materials stable in the long term and compatible with the substrate. Moreover, it mitigates the long-term negative effects caused by synthetic polymer residues from the cleaning materials commonly used in the dry cleaning of paper. Full article
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12 pages, 3732 KiB  
Article
Facile Strategy for Boosting of Inorganic Fillers Retention in Paper
by Klaudia Maślana, Krzysztof Sielicki, Karolina Wenelska, Tomasz Kędzierski, Joanna Janusz, Grzegorz Mariańczyk, Aleksandra Gorgon-Kuza, Wojciech Bogdan, Beata Zielińska and Ewa Mijowska
Polymers 2024, 16(1), 110; https://doi.org/10.3390/polym16010110 - 29 Dec 2023
Viewed by 459
Abstract
Achieving the desired properties of paper such as strength, durability, and printability remains challenging. Paper mills employ calcium carbonate (CaCO3) as a filler to boost paper’s brightness, opacity, and printability. However, weak interaction between cellulose fibers and CaCO3 particles creates [...] Read more.
Achieving the desired properties of paper such as strength, durability, and printability remains challenging. Paper mills employ calcium carbonate (CaCO3) as a filler to boost paper’s brightness, opacity, and printability. However, weak interaction between cellulose fibers and CaCO3 particles creates different issues in the papermaking industry. Therefore, this study explores the influence of various inorganic additives as crosslinkers such as mesoporous SiO2 nanospheres, TiO2 nanoparticles, h-BN nanoflakes, and hydroxylated h-BN nanoflakes (h-BN-OH) on inorganic fillers content in the paper. They were introduced to the paper pulp in the form of a polyethylene glycol (PEG) suspension to enable bonding between the inorganic particles and the paper pulp. Our findings have been revealed based on detailed microscopic and structural analyses, e.g., transmission and scanning electron microscopy, X-ray diffraction, Raman spectroscopy, and N2 adsorption/desorption isotherms. Finally, the inorganic fillers (CaCO3 and respective inorganic additives) content was evaluated following ISO 1762:2001 guidelines. Conducted evaluations allowed us to identify the most efficient crosslinker (SiO2 nanoparticles) in terms of inorganic filler retention. Paper sheets modified with SiO2 enhance the retention of the fillers by ~12.1%. Therefore, we believe these findings offer valuable insights for enhancing the papermaking process toward boosting the quality of the resulting paper. Full article
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20 pages, 11744 KiB  
Article
Applications of Xylan Derivatives to Improve the Functional Properties of Cellulose Foams for Noise Insulation
by Silviu Marian Nastac, Petronela Nechita, Maria Violeta Guiman, Mirela Roman and Ioan Calin Rosca
Polymers 2023, 15(24), 4648; https://doi.org/10.3390/polym15244648 - 08 Dec 2023
Viewed by 809
Abstract
Cellulose-based foams present a high potential for noise insulation applications. These materials are bio-degradable, eco-friendly by both embedded components and manufacturing process, have low density and high porosity, and are able to provide good noise insulation characteristics compared with available petroleum-based foams currently [...] Read more.
Cellulose-based foams present a high potential for noise insulation applications. These materials are bio-degradable, eco-friendly by both embedded components and manufacturing process, have low density and high porosity, and are able to provide good noise insulation characteristics compared with available petroleum-based foams currently used on a large scale. This paper presents the results of some investigations performed by the authors in order to improve the functional characteristics in terms of free surface wettability and structural integrity. Native xylan and xylan-based derivatives (in terms of acetylated and hydrophobized xylan) were taken into account for surface treatment of cellulose foams, suggesting that hemicelluloses represent by-products of pulp and paper industry, and xylan polysaccharides are the most abundant hemicelluloses type. The investigations were mainly conducted in order to evaluate the level to which surface treatments have affected the noise insulation properties of basic cellulose foams. The results indicate that surface treatments with xylan derivatives have slowly affected the soundproofing characteristics of foams, but these clearly have to be taken into account because of their high decrease in wettability level and improving structural integrity. Full article
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15 pages, 8282 KiB  
Article
Spray Drying Enzyme-Treated Cellulose Nanofibrils
by Sungjun Hwang, Colleen C. Walker, Donna Johnson, Yousoo Han and Douglas J. Gardner
Polymers 2023, 15(20), 4086; https://doi.org/10.3390/polym15204086 - 14 Oct 2023
Cited by 1 | Viewed by 964
Abstract
Enzyme-treated cellulose nanofibrils (CNFs) were produced via a lab-scale mass colloider using bleached kraft pulp (BKP) to evaluate their processability and power requirements during refining and spray-drying operations. To evaluate the energy efficiency in the CNF refining process, the net energy consumption, degree [...] Read more.
Enzyme-treated cellulose nanofibrils (CNFs) were produced via a lab-scale mass colloider using bleached kraft pulp (BKP) to evaluate their processability and power requirements during refining and spray-drying operations. To evaluate the energy efficiency in the CNF refining process, the net energy consumption, degree of polymerization (DP), and viscosity were determined. Less energy was consumed to attain a given fines level by using the endoglucanase enzymes. The DP and viscosity were also decreased using the enzymes. The morphological properties of the enzyme-pretreated spray-dried CNF powders (SDCNFs) were measured. Subsequently, the enzyme-pretreated SDCNFs were added to a PP matrix with MAPP as a coupling agent. The mixture was then compounded through a co-rotating twin-screw extruder to determine whether the enzyme treatment of the CNFs affects the mechanical properties of the composites. Compared to earlier studies on enhancing PMCs with SDCNF powders, this research investigates the use of enzyme-pretreated SDCNF powders. It was confirmed that the strength properties of PP increased by adding SDCNFs, and the strength properties were maintained after adding enzyme-pretreated SDCNFs. Full article
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18 pages, 10148 KiB  
Article
Cellulose Fibers-Based Porous Lightweight Foams for Noise Insulation
by Mihai Seciureanu, Silviu-Marian Nastac, Maria-Violeta Guiman and Petronela Nechita
Polymers 2023, 15(18), 3796; https://doi.org/10.3390/polym15183796 - 17 Sep 2023
Cited by 1 | Viewed by 1401
Abstract
This paper examines effective and environmentally friendly materials intended for noise insulation and soundproofing applications, starting with materials that have gained significant attention within last years. Foam-formed materials based on cellulose fibers have emerged as a promising solution. The aim of this study [...] Read more.
This paper examines effective and environmentally friendly materials intended for noise insulation and soundproofing applications, starting with materials that have gained significant attention within last years. Foam-formed materials based on cellulose fibers have emerged as a promising solution. The aim of this study was to obtain a set of foam-formed, porous, lightweight materials based on cellulose fibers from a resinous slurry pulp source, and to investigate the impact of surfactant percentage of the foam mixtures on their noise insulation characterisitcs. The basic foam-forming technique was used for sample assembly, with three percentages of sodium dodecyl sulphate (as anionic surfactant) related to fiber weight, and a standardised sound transmission loss tube procedure was used to evaluate noise insulation performance. Results were obtained as observations of internal structural configurations and material characteristics, and as measurements of sound absorption/reflection, sound transmission loss, and surface acoustic impedance. Based on the findings within this study, the conclusions highlight the strong potential of these cellulosic foams to replace widely used synthetic materials, at least into the area of practical noise insulation applications. Full article
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12 pages, 2880 KiB  
Article
Compressible Cellulose Wood Prepared with Deep Eutectic Solvents and Its Improved Technology
by Wenhao Wang, Mengyao Chen and Yan Wu
Polymers 2023, 15(7), 1593; https://doi.org/10.3390/polym15071593 - 23 Mar 2023
Cited by 3 | Viewed by 1830
Abstract
Elastic materials have a wide range of applications in many industries, but their widespread use is often limited by small-scale production methods and the use of highly polluting chemical reagents. In this study, we drew inspiration from research on wood softening to develop [...] Read more.
Elastic materials have a wide range of applications in many industries, but their widespread use is often limited by small-scale production methods and the use of highly polluting chemical reagents. In this study, we drew inspiration from research on wood softening to develop an environmentally friendly and scalable approach for producing a new type of compressible wood material called CW from natural wood. To achieve this, we employed a top-down approach using a novel type of “ionic liquid” eutectic solvent (DES) that is cost-effective, environmentally friendly, and recyclable. After treatment with DES, the resulting CW demonstrated good elasticity and durable compressibility, which was achieved by removing some lignin and hemicellulose from the wood and thinning the cell walls, thereby creating a honeycomb structure that allows for sustained compression and rebound. However, we found that the wood treated with a single eutectic solvent showed some softening (CW-1), although there was still room for further improvement of its elasticity. To address this, we used a secondary treatment with sodium hydroxide alkali solution to produce a softer and more elastic wood (CW-2). We conducted a series of comparative analyses and performance tests on natural wood (NW) and CW, including microscopic imaging; determination of chemical composition, mechanical properties, and compressive stress effects; and laser confocal testing. The results show that the DES and sodium hydroxide alkali solution treatments effectively removed some lignin, hemicellulose, and cellulose from the wood, resulting in the thinning of the cell walls and creating a more elastic material with a sustainable compression rebound rate of over 90%. The various properties of CW, including its elasticity, durability, and sustainability, provide great potential for its application in a range of fields, such as sensors, water purification, and directional tissue engineering. Full article
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20 pages, 5592 KiB  
Article
Efficiency of Neat and Quaternized-Cellulose Nanofibril Fillers in Chitosan Membranes for Direct Ethanol Fuel Cells
by Maša Hren, Damjan Makuc, Janez Plavec, Michaela Roschger, Viktor Hacker, Boštjan Genorio, Mojca Božič and Selestina Gorgieva
Polymers 2023, 15(5), 1146; https://doi.org/10.3390/polym15051146 - 24 Feb 2023
Cited by 1 | Viewed by 1353
Abstract
In this work, fully polysaccharide based membranes were presented as self-standing, solid polyelectrolytes for application in anion exchange membrane fuel cells (AEMFCs). For this purpose, cellulose nanofibrils (CNFs) were modified successfully with an organosilane reagent, resulting in quaternized CNFs (CNF (D)), as shown [...] Read more.
In this work, fully polysaccharide based membranes were presented as self-standing, solid polyelectrolytes for application in anion exchange membrane fuel cells (AEMFCs). For this purpose, cellulose nanofibrils (CNFs) were modified successfully with an organosilane reagent, resulting in quaternized CNFs (CNF (D)), as shown by Fourier Transform Infrared Spectroscopy (FTIR), Carbon-13 (C13) nuclear magnetic resonance (13C NMR), Thermogravimetric Analysis (TGA)/Differential Scanning Calorimetry (DSC), and ζ-potential measurements. Both the neat (CNF) and CNF(D) particles were incorporated in situ into the chitosan (CS) membrane during the solvent casting process, resulting in composite membranes that were studied extensively for morphology, potassium hydroxide (KOH) uptake and swelling ratio, ethanol (EtOH) permeability, mechanical properties, ionic conductivity, and cell performance. The results showed higher Young’s modulus (119%), tensile strength (91%), ion exchange capacity (177%), and ionic conductivity (33%) of the CS-based membranes compared to the commercial Fumatech membrane. The addition of CNF filler improved the thermal stability of the CS membranes and reduced the overall mass loss. The CNF (D) filler provided the lowest (4.23 × 10−5 cm2 s−1) EtOH permeability of the respective membrane, which is in the same range as that of the commercial membrane (3.47 × 10−5 cm2s−1). The most significant improvement (~78%) in power density at 80 °C was observed for the CS membrane with neat CNF compared to the commercial Fumatech membrane (62.4 mW cm−2 vs. 35.1 mW cm−2). Fuel cell tests showed that all CS-based anion exchange membranes (AEMs) exhibited higher maximum power densities than the commercial AEMs at 25 °C and 60 °C with humidified or non-humidified oxygen, demonstrating their potential for low-temperature direct ethanol fuel cell (DEFC) applications. Full article
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Review

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25 pages, 5939 KiB  
Review
From Nature to Lab: Sustainable Bacterial Cellulose Production and Modification with Synthetic Biology
by Vid Potočnik, Selestina Gorgieva and Janja Trček
Polymers 2023, 15(16), 3466; https://doi.org/10.3390/polym15163466 - 18 Aug 2023
Cited by 4 | Viewed by 5513
Abstract
Bacterial cellulose (BC) is a macromolecule with versatile applications in medicine, pharmacy, biotechnology, cosmetology, food and food packaging, ecology, and electronics. Although many bacteria synthesize BC, the most efficient BC producers are certain species of the genera Komagataeibacter and Novacetimonas. These are [...] Read more.
Bacterial cellulose (BC) is a macromolecule with versatile applications in medicine, pharmacy, biotechnology, cosmetology, food and food packaging, ecology, and electronics. Although many bacteria synthesize BC, the most efficient BC producers are certain species of the genera Komagataeibacter and Novacetimonas. These are also food-grade bacteria, simplifying their utilization at industrial facilities. The basic principles of BC synthesis are known from studies of Komagataeibacter xylinus, which became a model species for studying BC at genetic and molecular levels. Cellulose can also be of plant origin, but BC surpasses its purity. Moreover, the laboratory production of BC enables in situ modification into functionalized material with incorporated molecules during its synthesis. The possibility of growing Komagataeibacter and Novacetimonas species on various organic substrates and agricultural and food waste compounds also follows the green and sustainable economy principles. Further intervention into BC synthesis was enabled by genetic engineering tools, subsequently directing it into the field of synthetic biology. This review paper presents the development of the fascinating field of BC synthesis at the molecular level, seeking sustainable ways for its production and its applications towards genetic modifications of bacterial strains for producing novel types of living biomaterials using the flexible metabolic machinery of bacteria. Full article
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