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Advanced Nanocellulose-Based Materials: Production, Properties and Applications

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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Nanocomposite Materials".

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 31466

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Special Issue Editors

Dr. Carla Vilela

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CICECO–Aveiro Institute of Materials, Department of Chemistry, University of Aveiro, 3810-193 Aveiro, Portugal
Interests: sustainable use of biopolymers (nanocellulose, chitosan, pullulan, proteins, etc.) for the design of functional nanostructured materials for biomedical (e.g., drug delivery and wound healing) and technological (e.g., active packaging, fuel cells, and water remediation) applications
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Prof. Dr. Carmen S. R. Freire

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Guest Editor

CICECO—Aveiro Institute of Materials, Department of Chemistry, University of Aveiro, 3810-193 Aveiro, Portugal
Interests: production and application of biogenic nanofibers (bacterial cellulose and protein fibrils); nanostructured biocomposites; bio-based materials for biomedical applications (wound healing, drug delivery and 3D-bioprinting); biocomposites and functional paper materials; chemical modification of (nano)cellulose fibers and other polysaccharides and their characterization and applications; chemistry of lignocellulosic materials (cellulose, wood, cork, etc.)
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Bacterial nanocellulose (BNC), cellulose nanocrystals (CNCs), and cellulose nanofibers (CNFs) are three nanometric forms of the most abundant natural polymer (viz. cellulose), and are currently at the spotlight in numerous fields of modern science and technology. The eco-friendly connotation, peculiar features, and multiple functionalities of these nanoscale cellulosic substrates are being explored to engineer advanced nanocomposites and nanohybrid materials for application in manifold domains, such as mechanics, optics, electronics, energy, environment, biology, and medicine.

The aim of this Special Issue titled “Advanced Nanocellulose-Based Materials: Production, Properties, and Applications” is to gather a collection of original research and review contributions from the world-leading scientists working with nanocellulose. Thus, research that is representative of the current developments dealing with the production methodologies, properties, and applications of nanocellulose-based materials (e.g., nanocomposites, hybrids, aerogels, hydrogels, films, and fibers), are very welcome to the Special Issue.

Dr. Carla Vilela
Dr. Carmen S.R. Freire
Guest Editors

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Keywords

bacterial nanocellulose
cellulose nanocrystals
cellulose nanofibers
nanocomposites
hybrids
aerogels
films
fibers
biomedical applications
technological applications

Published Papers (10 papers)

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Editorial

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4 pages, 208 KiB

Open AccessEditorial

Advanced Nanocellulose-Based Materials: Production, Properties, and Applications

by Carmen S. R. Freire and Carla Vilela

Nanomaterials 2022, 12(3), 431; https://doi.org/10.3390/nano12030431 - 27 Jan 2022

Cited by 1 | Viewed by 2277

Abstract

Natural polymers, such as polysaccharides and proteins, are being extensively utilized as substrates to create advanced materials [...] Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

Research

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18 pages, 6026 KiB

Open AccessArticle

High-Strength Regenerated Cellulose Fiber Reinforced with Cellulose Nanofibril and Nanosilica

by Yu Xue, Letian Qi, Zhaoyun Lin, Guihua Yang, Ming He and Jiachuan Chen

Nanomaterials 2021, 11(10), 2664; https://doi.org/10.3390/nano11102664 - 11 Oct 2021

Cited by 12 | Viewed by 2259

Abstract

In this study, a novel type of high-strength regenerated cellulose composite fiber reinforced with cellulose nanofibrils (CNFs) and nanosilica (nano-SiO₂) was prepared. Adding 1% CNF and 1% nano-SiO₂ to pulp/AMIMCl improved the tensile strength of the composite cellulose by 47.46%. The surface of the regenerated fiber exhibited a scaly structure with pores, which could be reduced by adding CNF and nano-SiO₂, resulting in the enhancement of physical strength of regenerated fibers. The cellulose/AMIMCl mixture with or without the addition of nanomaterials performed as shear thinning fluids, also known as “pseudoplastic” fluids. Increasing the temperature lowered the viscosity. The yield stress and viscosity sequences were as follows: RCF-CNF² > RCF-CNF²-SiO₂² > RCF-SiO₂² > RCF > RCF-CNF¹-SiO₂¹. Under the same oscillation frequency, G’ and G” decreased with the increase of temperature, which indicated a reduction in viscoelasticity. A preferred cellulose/AMIMCl mixture was obtained with the addition of 1% CNF and 1% nano-SiO₂, by which the viscosity and shear stress of the adhesive were significantly reduced at 80 °C. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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17 pages, 3031 KiB

Open AccessArticle

Cellulose Nanocrystals/Chitosan-Based Nanosystems: Synthesis, Characterization, and Cellular Uptake on Breast Cancer Cells

by Ricardo J. B. Pinto, Nicole S. Lameirinhas, Gabriela Guedes, Gustavo H. Rodrigues da Silva, Párástu Oskoei, Stefan Spirk, Helena Oliveira, Iola F. Duarte, Carla Vilela and Carmen S. R. Freire

Nanomaterials 2021, 11(8), 2057; https://doi.org/10.3390/nano11082057 - 12 Aug 2021

Cited by 16 | Viewed by 3253

Abstract

Cellulose nanocrystals (CNCs) are elongated biobased nanostructures with unique characteristics that can be explored as nanosystems in cancer treatment. Herein, the synthesis, characterization, and cellular uptake on folate receptor (FR)-positive breast cancer cells of nanosystems based on CNCs and a chitosan (CS) derivative are investigated. The physical adsorption of the CS derivative, containing a targeting ligand (folic acid, FA) and an imaging agent (fluorescein isothiocyanate, FITC), on the surface of the CNCs was studied as an eco-friendly methodology to functionalize CNCs. The fluorescent CNCs/FA-CS-FITC nanosystems with a rod-like morphology showed good stability in simulated physiological and non-physiological conditions and non-cytotoxicity towards MDA-MB-231 breast cancer cells. These functionalized CNCs presented a concentration-dependent cellular internalization with a 5-fold increase in the fluorescence intensity for the nanosystem with the higher FA content. Furthermore, the exometabolic profile of the MDA-MB-231 cells exposed to the CNCs/FA-CS-FITC nanosystems disclosed a moderate impact on the cells’ metabolic activity, limited to decreased choline uptake and increased acetate release, which implies an anti-proliferative effect. The overall results demonstrate that the CNCs/FA-CS-FITC nanosystems, prepared by an eco-friendly approach, have a high affinity towards FR-positive cancer cells and thus might be applied as nanocarriers with imaging properties for active targeted therapy. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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17 pages, 4504 KiB

Open AccessEditor’s ChoiceArticle

Influence of Drying Method and Argon Plasma Modification of Bacterial Nanocellulose on Keratinocyte Adhesion and Growth

by Anna Kutová, Lubica Staňková, Kristýna Vejvodová, Ondřej Kvítek, Barbora Vokatá, Dominik Fajstavr, Zdeňka Kolská, Antonín Brož, Lucie Bačáková and Václav Švorčík

Nanomaterials 2021, 11(8), 1916; https://doi.org/10.3390/nano11081916 - 26 Jul 2021

Cited by 9 | Viewed by 2455

Abstract

Due to its nanostructure, bacterial nanocellulose (BC) has several advantages over plant cellulose, but it exhibits weak cell adhesion. To overcome this drawback, we studied the drying method of BC and subsequent argon plasma modification (PM). BC hydrogels were prepared using the Komagataeibacter sucrofermentans (ATCC 700178) bacteria strain. The hydrogels were transformed into solid samples via air-drying (BC-AD) or lyophilization (BC-L). The sample surfaces were then modified by argon plasma. SEM revealed that compared to BC-AD, the BC-L samples maintained their nanostructure and had higher porosity. After PM, the contact angle decreased while the porosity increased. XPS showed that the O/C ratio was higher after PM. The cell culture experiments revealed that the initial adhesion of human keratinocytes (HaCaT) was supported better on BC-L, while the subsequent growth of these cells and final cell population density were higher on BC-AD. The PM improved the final colonization of both BC-L and BC-AD with HaCaT, leading to formation of continuous cell layers. Our work indicates that the surface modification of BC renders this material highly promising for skin tissue engineering and wound healing. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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21 pages, 4625 KiB

Open AccessArticle

5-Fluorouracil Encapsulated Chitosan-Cellulose Fiber Bionanocomposites: Synthesis, Characterization and In Vitro Analysis towards Colorectal Cancer Cells

by Mostafa Yusefi, Hui-Yin Chan, Sin-Yeang Teow, Pooneh Kia, Michiele Lee-Kiun Soon, Nor Azwadi Bin Che Sidik and Kamyar Shameli

Nanomaterials 2021, 11(7), 1691; https://doi.org/10.3390/nano11071691 - 28 Jun 2021

Cited by 28 | Viewed by 3254

Abstract

Cellulose and chitosan with remarkable biocompatibility and sophisticated physiochemical characteristics can be a new dawn to the advanced drug nano-carriers in cancer treatment. This study aims to synthesize layer-by-layer bionanocomposites from chitosan and rice straw cellulose encapsulated 5-Fluorouracil (CS-CF/5FU BNCs) using the ionic gelation method and the sodium tripolyphosphate (TPP) cross-linker. Data from X-ray and Fourier-transform infrared spectroscopy showed successful preparation of CS-CF/5FU BNCs. Based on images of scanning electron microscopy, 48.73 ± 1.52 nm was estimated for an average size of the bionanocomposites as spherical chitosan nanoparticles mostly coated rod-shaped cellulose reinforcement. 5-Fluorouracil indicated an increase in thermal stability after its encapsulation in the bionanocomposites. The drug encapsulation efficiency was found to be 86 ± 2.75%. CS-CF/5FU BNCs triggered higher drug release in a media simulating the colorectal fluid with pH 7.4 (76.82 ± 1.29%) than the gastric fluid with pH 1.2 (42.37 ± 0.43%). In in vitro cytotoxicity assays, cellulose fibers, chitosan nanoparticles and the bionanocomposites indicated biocompatibility towards CCD112 normal cells. Most promisingly, CS-CF/5FU BNCs at 250 µg/mL concentration eliminated 56.42 ± 0.41% of HCT116 cancer cells and only 8.16 ± 2.11% of CCD112 normal cells. Therefore, this study demonstrates that CS-CF/5FU BNCs can be considered as an eco-friendly and innovative nanodrug candidate for potential colorectal cancer treatment. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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13 pages, 3086 KiB

Open AccessFeature PaperArticle

The Effect of High Lignin Content on Oxidative Nanofibrillation of Wood Cell Wall

by Simon Jonasson, Anne Bünder, Linn Berglund, Magnus Hertzberg, Totte Niittylä and Kristiina Oksman

Nanomaterials 2021, 11(5), 1179; https://doi.org/10.3390/nano11051179 - 29 Apr 2021

Cited by 5 | Viewed by 2102

Abstract

Wood from field-grown poplars with different genotypes and varying lignin content (17.4 wt % to 30.0 wt %) were subjected to one-pot 2,2,6,6-Tetramethylpiperidin-1-yl)oxyl catalyzed oxidation and high-pressure homogenization in order to investigate nanofibrillation following simultaneous delignification and cellulose oxidation. When comparing low and high lignin wood it was found that the high lignin wood was more easily fibrillated as indicated by a higher nanofibril yield (68% and 45%) and suspension viscosity (27 and 15 mPa·s). The nanofibrils were monodisperse with diameter ranging between 1.2 and 2.0 nm as measured using atomic force microscopy. Slightly less cellulose oxidation (0.44 and 0.68 mmol·g⁻¹) together with a reduced process yield (36% and 44%) was also found which showed that the removal of a larger amount of lignin increased the efficiency of the homogenization step despite slightly reduced oxidation of the nanofibril surfaces. The surface area of oxidized high lignin wood was also higher than low lignin wood (114 m²·g⁻¹ and 76 m²·g⁻¹) which implicates porosity as a factor that can influence cellulose nanofibril isolation from wood in a beneficial manner. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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14 pages, 3828 KiB

Open AccessEditor’s ChoiceArticle

Ice-Templated Cellulose Nanofiber Filaments as a Reinforcement Material in Epoxy Composites

by Tuukka Nissilä, Jiayuan Wei, Shiyu Geng, Anita Teleman and Kristiina Oksman

Nanomaterials 2021, 11(2), 490; https://doi.org/10.3390/nano11020490 - 15 Feb 2021

Cited by 20 | Viewed by 3654

Abstract

Finding renewable alternatives to the commonly used reinforcement materials in composites is attracting a significant amount of research interest. Nanocellulose is a promising candidate owing to its wide availability and favorable properties such as high Young’s modulus. This study addressed the major problems inherent to cellulose nanocomposites, namely, controlling the fiber structure and obtaining a sufficient interfacial adhesion between nanocellulose and a non-hydrophilic matrix. Unidirectionally aligned cellulose nanofiber filament mats were obtained via ice-templating, and chemical vapor deposition was used to cover the filament surfaces with an aminosilane before impregnating the mats with a bio-epoxy resin. The process resulted in cellulose nanocomposites with an oriented structure and a strong fiber–matrix interface. Diffuse reflectance infrared Fourier transform and X-ray photoelectron spectroscopy studies revealed the presence of silane on the filaments. The improved interface, resulting from the surface treatment, was observable in electron microscopy images and was further confirmed by the significant increase in the tan delta peak temperature. The storage modulus of the matrix could be improved up to 2.5-fold with 18 wt% filament content and was significantly higher in the filament direction. Wide-angle X-ray scattering was used to study the orientation of cellulose nanofibers in the filament mats and the composites, and the corresponding orientation indices were 0.6 and 0.53, respectively, indicating a significant level of alignment. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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16 pages, 2463 KiB

Open AccessArticle

Antibacterial Multi-Layered Nanocellulose-Based Patches Loaded with Dexpanthenol for Wound Healing Applications

by Daniela F. S. Fonseca, João P. F. Carvalho, Verónica Bastos, Helena Oliveira, Catarina Moreirinha, Adelaide Almeida, Armando J. D. Silvestre, Carla Vilela and Carmen S. R. Freire

Nanomaterials 2020, 10(12), 2469; https://doi.org/10.3390/nano10122469 - 09 Dec 2020

Cited by 19 | Viewed by 2750

Abstract

Antibacterial multi-layered patches composed of an oxidized bacterial cellulose (OBC) membrane loaded with dexpanthenol (DEX) and coated with several chitosan (CH) and alginate (ALG) layers were fabricated by spin-assisted layer-by-layer (LbL) assembly. Four patches with a distinct number of layers (5, 11, 17, and 21) were prepared. These nanostructured multi-layered patches reveal a thermal stability up to 200 °C, high mechanical performance (Young’s modulus ≥ 4 GPa), and good moisture-uptake capacity (240–250%). Moreover, they inhibited the growth of the skin pathogen Staphylococcus aureus (3.2–log CFU mL⁻¹ reduction) and were non-cytotoxic to human keratinocytes (HaCaT cells). The in vitro release profile of DEX was prolonged with the increasing number of layers, and the time-dependent data imply a diffusion/swelling-controlled drug release mechanism. In addition, the in vitro wound healing assay demonstrated a good cell migration capacity, headed to a complete gap closure after 24 h. These results certify the potential of these multi-layered polysaccharides-based patches toward their application in wound healing. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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13 pages, 2255 KiB

Open AccessArticle

Flexible Nanocellulose/Lignosulfonates Ion-Conducting Separators for Polymer Electrolyte Fuel Cells

by Carla Vilela, João D. Morais, Ana Cristina Q. Silva, Daniel Muñoz-Gil, Filipe M. L. Figueiredo, Armando J. D. Silvestre and Carmen S. R. Freire

Nanomaterials 2020, 10(9), 1713; https://doi.org/10.3390/nano10091713 - 29 Aug 2020

Cited by 27 | Viewed by 3407

Abstract

The utilization of biobased materials for the fabrication of naturally derived ion-exchange membranes is breezing a path to sustainable separators for polymer electrolyte fuel cells (PEFCs). In this investigation, bacterial nanocellulose (BNC, a bacterial polysaccharide) and lignosulfonates (LS, a by-product of the sulfite pulping process), were blended by diffusion of an aqueous solution of the lignin derivative and of the natural-based cross-linker tannic acid into the wet BNC nanofibrous three-dimensional structure, to produce fully biobased ion-exchange membranes. These freestanding separators exhibited good thermal-oxidative stability of up to about 200 °C, in both inert and oxidative atmospheres (N₂ and O₂, respectively), high mechanical properties with a maximum Young’s modulus of around 8.2 GPa, as well as good moisture-uptake capacity with a maximum value of ca. 78% after 48 h for the membrane with the higher LS content. Moreover, the combination of the conducting LS with the mechanically robust BNC conveyed ionic conductivity to the membranes, namely a maximum of 23 mS cm⁻¹ at 94 °C and 98% relative humidity (RH) (in-plane configuration), that increased with increasing RH. Hence, these robust water-mediated ion conductors represent an environmentally friendly alternative to the conventional ion-exchange membranes for application in PEFCs. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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Review

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18 pages, 3430 KiB

Open AccessReview

Recent Progress on the Characterization of Cellulose Nanomaterials by Nanoscale Infrared Spectroscopy

by Qianqian Zhu, Rui Zhou, Jun Liu, Jianzhong Sun and Qianqian Wang

Nanomaterials 2021, 11(5), 1353; https://doi.org/10.3390/nano11051353 - 20 May 2021

Cited by 18 | Viewed by 4008

Abstract

Researches of cellulose nanomaterials have seen nearly exponential growth over the past several decades for versatile applications. The characterization of nanostructural arrangement and local chemical distribution is critical to understand their role when developing cellulose materials. However, with the development of current characterization methods, the simultaneous morphological and chemical characterization of cellulose materials at nanoscale resolution is still challenging. Two fundamentally different nanoscale infrared spectroscopic techniques, namely atomic force microscope based infrared spectroscopy (AFM-IR) and infrared scattering scanning near field optical microscopy (IR s-SNOM), have been established by the integration of AFM with IR spectroscopy to realize nanoscale spatially resolved imaging for both morphological and chemical information. This review aims to summarize and highlight the recent developments in the applications of current state-of-the-art nanoscale IR spectroscopy and imaging to cellulose materials. It briefly outlines the basic principles of AFM-IR and IR s-SNOM, as well as their advantages and limitations to characterize cellulose materials. The uses of AFM-IR and IR s-SNOM for the understanding and development of cellulose materials, including cellulose nanomaterials, cellulose nanocomposites, and plant cell walls, are extensively summarized and discussed. The prospects of future developments in cellulose materials characterization are provided in the final part. Full article

(This article belongs to the Special Issue Advanced Nanocellulose-Based Materials: Production, Properties and Applications)

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