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Emerging Trends in Nanocelluloses

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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Nanochemistry".

Deadline for manuscript submissions: closed (31 March 2019) | Viewed by 64117

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Prof. Dr. Theo Van de Ven

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Guest Editor

Department of Chemistry, McGill University, 3420 University Street, Montreal, QC, Canada
Interests: colloids; nanocellulose; paper making

Dr. Amir Sheikhi

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Guest Editor

Department of Chemical Engineering, 413 Chemical and Biomedical Engineering Building (CBEB), The Pennsylvania State University, University Park, PA 16802, USA
Interests: soft matter; colloidal systems; macromolecules; hydrogels; active interfaces; biomaterials; nanocelluloses
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Dear Colleagues,

Recent decades have witnessed a remarkable enthusiasm for taking advantage of natural resources to develop advanced materials that, not only may replace synthetic, often hazardous alternatives, but also provide unique properties, enabling significant technological advances. Among natural materials, cellulose, the most abundant biopolymer in the world, benefitting from unique physicochemical and structural characteristics, has been able to play a key role in a wide range of advanced applications. The immense interest towards cellulose relies on facile nanoengineering of cellulose fibrils, yielding a library of nanocelluloses, namely cellulose nanofibrils (CNF), cellulose nanocrystals (CNC), and hairy CNCs (HCNC), which may be produced in varying sizes (nm to µm), morphologies (e.g., fibrils, needles, spheres), surface features (bare or coated), chemical functionality (neutral, anionic, and cationic), and forms (colloids, hydrogels, aerogels, films, emulsions). To this end, understanding structure-property relationships is inevitable in exploring highly innovative nanocellulose-based solutions to the unmet materials challenges of the 21st century.

This Special Issue focuses on the state-of-the-art aspects of nanocelluloses across the breadth of applied sustainable nanomaterials and nanocomposites with special attention to structure-property relationships, which has enabled the applications of nanocelluloses in environmental remediation, water technology, rheology modification, matrix reinforcement, cargo delivery and biomedical engineering, bioinks for 3D printing, catalysis, energy storage, flexible electronics, sensors and actuators, photonics, food industry, cosmetic and hygiene products, functional emulsions, smart packaging, and other emerging horizons. Authors are welcome to submit their original research and/or review articles.

Prof. Theo van de Ven
Dr. Amir Sheikhi
Guest Editors

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Keywords

Nanocellulose
Cellulose nanocrystals
Cellulose nanofibrils
Nanocomposites
Structure-property relationships
Coating
Hierarchical templating
Water, energy, and environment
Flexible electronics, sensors, and photonics
Nanomedicine

Published Papers (10 papers)

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Research

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9 pages, 3201 KiB

Open AccessArticle

Screening of Nanocellulose from Different Biomass Resources and Its Integration for Hydrophobic Transparent Nanopaper

by Yanran Qi, Hao Zhang, Dandan Xu, Zaixin He, Xiya Pan, Shihan Gui, Xiaohan Dai, Jilong Fan, Xiaoying Dong and Yongfeng Li

Molecules 2020, 25(1), 227; https://doi.org/10.3390/molecules25010227 - 06 Jan 2020

Cited by 21 | Viewed by 4273

Abstract

Petroleum-based plastics, such as PP, PE, PVC, etc., have become an important source of environmental pollution due to their hard degradation, posing a serious threat to the human health. Isolating nanocellulose from abundant biomass waste resources and further integrating the nanocellulose into hydrophobic transparent film (i.e., nanopaper), to replace the traditional nondegradable plastic film, is of great significance for solving the problem of environmental pollution and achieving sustainable development of society. This study respectively extracted nanocellulose from the branches of Amorpha fruticosa Linn., wheat straw, and poplar residues via combined mechanical treatments of grinding and high-pressure homogenization. Among them, the nanocellulose derived from the Amorpha fruticosa has a finer structure, with diameter of about 10 nm and an aspect ratio of more than 500. With the nanocellulose as building block, we constructed hydrophilic nanopaper with high light transmittance (up to 90%) and high mechanical strength (tensile strength up to 110 MPa). After further hybridization by incorporating nano-silica into the nanopaper, followed by hydrophobic treatment, we built hydrophobic nanopaper with transmittance over 82% and a water contact angle of about 102° that could potentially replace transparent plastic film and has wide applications in food packaging, agricultural film, electronic device, and other fields. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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15 pages, 12036 KiB

Open AccessArticle

Cellulose Nanocrystal Isolation from Hardwood Pulp using Various Hydrolysis Conditions

by Kuan-Hsuan Lin, Toshiharu Enomae and Feng-Cheng Chang

Molecules 2019, 24(20), 3724; https://doi.org/10.3390/molecules24203724 - 16 Oct 2019

Cited by 23 | Viewed by 3235

Abstract

To expand the application field of the pulping industry, this study conducted a series of sample preparations for processing cellulose nanocrystals (CNCs) from a dry hardwood pulp to achieve optimal sulfuric acid hydrolysis. The properties of laboratory-prepared pulp CNCs (P-CNCs) were investigated with different preparation conditions including sulfuric acid concentrations, hydrolysis temperatures, and hydrolysis durations. Results showed a gradient of color changes observed with the increase of hydrolysis duration and temperature. Under certain conditions, the derived P-CNCs exhibited nanoscale dimensions, detected by transmission electron microscopy, and a crystallinity index similar to commercial products. In addition, the surface sulfate groups were assumed to be contributed by sulfuric acid hydrolysis. However, a high acid concentration and long hydrolysis processing duration introduced more sulfate groups on the derived P-CNCs, which may have acted as flame retardants and, thus, increased the amount of char residue. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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13 pages, 3594 KiB

Open AccessArticle

Nanocellulose-Reinforced Polyurethane for Waterborne Wood Coating

by Linglong Kong, Dandan Xu, Zaixin He, Fengqiang Wang, Shihan Gui, Jilong Fan, Xiya Pan, Xiaohan Dai, Xiaoying Dong, Baoxuan Liu and Yongfeng Li

Molecules 2019, 24(17), 3151; https://doi.org/10.3390/molecules24173151 - 29 Aug 2019

Cited by 42 | Viewed by 5885

Abstract

With the enhancement of people’s environmental awareness, waterborne polyurethane (PU) paint—with its advantages of low release of volatile organic compounds (VOCs), low temperature flexibility, acid and alkali resistance, excellent solvent resistance and superior weather resistance—has made its application for wood furniture favored by the industry. However, due to its lower solid content and weak intermolecular force, the mechanical properties of waterborne PU paint are normally less than those of the traditional solvent-based polyurethane paint, which has become the key bottleneck restricting its wide applications. To this end, this study explores nanocellulose derived from biomass resources by the 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) oxidation method to reinforce and thus improve the mechanical properties of waterborne PU paint. Two methods of adding nanocellulose to waterborne PU—chemical addition and physical blending—are explored. Results show that, compared to the physical blending method, the chemical grafting method at 0.1 wt% nanocellulose addition results in the maximum improvement of the comprehensive properties of the PU coating. With this method, the tensile strength, elongation at break, hardness and abrasion resistance of the waterborne PU paint increase by up to 58.7%, ~55%, 6.9% and 3.45%, respectively, compared to the control PU; while the glossiness and surface drying time were hardly affected. Such exploration provides an effective way for wide applications of water PU in the wood industry and nanocellulose in waterborne wood coating. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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16 pages, 2980 KiB

Open AccessArticle

Zwitterionic Acetylated Cellulose Nanofibrils

by Jowan Rostami, Aji P. Mathew and Ulrica Edlund

Molecules 2019, 24(17), 3147; https://doi.org/10.3390/molecules24173147 - 29 Aug 2019

Cited by 12 | Viewed by 3782

Abstract

A strategy is devised to synthesize zwitterionic acetylated cellulose nanofibrils (CNF). The strategy included acetylation, periodate oxidation, Schiff base reaction, borohydride reduction, and a quaternary ammonium reaction. Acetylation was performed in glacial acetic acid with a short reaction time of 90 min, yielding, on average, mono-acetylated CNF with hydroxyl groups available for further modification. The products from each step were characterized by FTIR spectroscopy, ζ-potential, SEM-EDS, AFM, and titration to track and verify the structural changes along the sequential modification route. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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17 pages, 9868 KiB

Open AccessArticle

Carbon Nanotube and Cellulose Nanocrystal Hybrid Films

by Mingzhe Jiang, Robert Seney, Paul Charles Bayliss and Christopher L. Kitchens

Molecules 2019, 24(14), 2662; https://doi.org/10.3390/molecules24142662 - 23 Jul 2019

Cited by 14 | Viewed by 4315

Abstract

The use of cellulose nanocrystals (CNC) in high performance coatings is attractive for micro-scale structures or device fabrication due to the anisotropic geometry, however CNC are insulating materials. Carbon nanotubes (CNT) are also rod-shaped nanomaterials that display high mechanical strength and electrical conductivity. The hydrophobic regions of surface-modified CNC can interact with hydrophobic CNT and aid in association between the two anisotropic nanomaterials. The long-range electrostatic repulsion of CNC plays a role in forming a stable CNT and CNC mixture dispersion in water, which is integral to forming a uniform hybrid film. At concentrations favorable for film formation, the multiwalled nanotubes + CNC mixture dispersion shows cellular network formation, indicating local phase separation, while the single-walled nanotube + CNC mixture dispersion shows schlieren texture, indicating liquid crystal mixture formation. Conductive CNT + CNC hybrid films (5–20 μm thick) were cast on glass microscope slides with and without shear by blade coating. The CNT + CNC hybrid films electrical conductivity increased with increasing CNT loadings and some anisotropy was observed with the sheared hybrid films, although to a lesser extent than what was anticipated. Percolation models were applied to model the hybrid film conductivity and correlate with the hybrid film microstructure. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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13 pages, 2947 KiB

Open AccessArticle

In Situ Production and Application of Cellulose Nanofibers to Improve Recycled Paper Production

by Ana Balea, Jose Luis Sanchez-Salvador, M. Concepcion Monte, Noemi Merayo, Carlos Negro and Angeles Blanco

Molecules 2019, 24(9), 1800; https://doi.org/10.3390/molecules24091800 - 09 May 2019

Cited by 46 | Viewed by 5372

Abstract

The recycled paper and board industry needs to improve the quality of their products to meet customer demands. The refining process and strength additives are commonly used to increase mechanical properties. Interfiber bonding can also be improved using cellulose nanofibers (CNF). A circular economy approach in the industrial implementation of CNF can be addressed through the in situ production of CNF using side cellulose streams of the process as raw material, avoiding transportation costs and reducing industrial wastes. Furthermore, CNF fit for use can be produced for specific industrial applications.This study evaluates the feasibility of using two types of recycled fibers, simulating the broke streams of two paper machines producing newsprint and liner for cartonboard, to produce in situ CNF for direct application on the original pulps, old newsprint (ONP), and old corrugated container (OCC), and to reinforce the final products. The CNF were obtained by 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO)-mediated oxidation and homogenization at 600 bar. Handsheets were prepared with disintegrated recycled pulp and different amounts of CNF using a conventional three-component retention system. Results show that 3 wt.% of CNF produced with 10 mmol of NaClO per gram of dry pulp improve tensile index of ONP ~30%. For OCC, the same treatment and CNF dose increase tensile index above 60%. In both cases, CNF cause a deterioration of drainage, but this effect is effectively counteracted by optimising the retention system. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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10 pages, 8417 KiB

Open AccessCommunication

Concerted Catalysis by Nanocellulose and Proline in Organocatalytic Michael Additions

by Naliharifetra Jessica Ranaivoarimanana, Kyohei Kanomata and Takuya Kitaoka

Molecules 2019, 24(7), 1231; https://doi.org/10.3390/molecules24071231 - 29 Mar 2019

Cited by 11 | Viewed by 3470

Abstract

Cellulose nanofibers (CNFs) have recently attracted much attention as catalysts in various reactions. Organocatalysts have emerged as sustainable alternatives to metal-based catalysts in green organic synthesis, with concerted systems containing CNFs that are expected to provide next-generation catalysis. Herein, for the first time, we report that a representative organocatalyst comprising an unexpected combination of 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO)-oxidized CNFs and proline shows significantly enhanced catalytic activity in an asymmetric Michael addition. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

17 pages, 4087 KiB

Open AccessArticle

Emulsion Stabilization with Functionalized Cellulose Nanoparticles Fabricated Using Deep Eutectic Solvents

by Jonna Ojala, Miikka Visanko, Ossi Laitinen, Monika Österberg, Juho Antti Sirviö and Henrikki Liimatainen

Molecules 2018, 23(11), 2765; https://doi.org/10.3390/molecules23112765 - 25 Oct 2018

Cited by 28 | Viewed by 7178

Abstract

In this experiment, the influence of the morphology and surface characteristics of cellulosic nanoparticles (i.e., cellulose nanocrystals [CNCs] and cellulose nanofibers [CNFs]) on oil-in-water (o/w) emulsion stabilization was studied using non-modified or functionalized nanoparticles obtained following deep eutectic solvent (DES) pre-treatments. The effect of the oil-to-water ratio (5, 10, and 20 wt.-% (weight percent) of oil), the type of nanoparticle, and the concentration of the particles (0.05–0.2 wt.-%) on the oil-droplet size (using laser diffractometry), o/w emulsion stability (via analytical centrifugation), and stabilization mechanisms (using field emission scanning electron microscopy with the model compound—i.e., polymerized styrene in water emulsions) were examined. All the cellulosic nanoparticles studied decreased the oil droplet size in emulsion (sizes varied from 22.5 µm to 8.9 µm, depending on the nanoparticle used). Efficient o/w emulsion stabilization against coalescence and an oil droplet-stabilizing web-like structure were obtained only, however, with surface-functionalized CNFs, which had a moderate hydrophilicity level. CNFs without surface functionalization did not prevent either the coalescence or the creaming of emulsions, probably due to the natural hydrophobicity of the nanoparticles and their instability in water. Moderately hydrophilic CNCs, on the other hand, distributed evenly and displayed good interaction with both dispersion phases. The rigid structure of CNCs meant, however, that voluminous web structures were not formed on the surface of oil droplets; they formed in flat, uniform layers instead. Consequently, emulsion stability was lower with CNCs, when compared with surface-functionalized CNFs. Tunable cellulose nanoparticles can be used in several applications such as in enhanced marine oil response. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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9 pages, 2977 KiB

Open AccessArticle

Morphological, Release and Antibacterial Performances of Amoxicillin-Loaded Cellulose Aerogels

by Shan Ye, Shu He, Chen Su, Lei Jiang, Yanyi Wen, Zhongjie Zhu and Wei Shao

Molecules 2018, 23(8), 2082; https://doi.org/10.3390/molecules23082082 - 20 Aug 2018

Cited by 26 | Viewed by 4644

Abstract

Cellulose has been widely used in the biomedical field. In this study, novel cellulose aerogels were firstly prepared in a NaOH-based solvent system by a facile casting method. Then amoxicillin was successfully loaded into cellulose aerogels with different loadings. The morphology and structure of the cellulose aerogels were characterized using scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR). The drug release and antibacterial activities were also evaluated. The drug release results showed that cellulose aerogels have controlled amoxicillin release performance. In vitro antibacterial assay demonstrated that the cellulose aerogels exhibited excellent antibacterial activity with the amoxicillin dose-dependent activity. Therefore, the developed cellulose aerogels display controlled release behavior and efficient antibacterial performance, thus confirming their potential for biomedical applications. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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Review

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24 pages, 5210 KiB

Open AccessReview

Cellulose Nanomaterials—Binding Properties and Applications: A Review

by Ali H. Tayeb, Ezatollah Amini, Shokoofeh Ghasemi and Mehdi Tajvidi

Molecules 2018, 23(10), 2684; https://doi.org/10.3390/molecules23102684 - 18 Oct 2018

Cited by 275 | Viewed by 21173

Abstract

Cellulose nanomaterials (CNs) are of increasing interest due to their appealing inherent properties such as bio-degradability, high surface area, light weight, chirality and the ability to form effective hydrogen bonds across the cellulose chains or within other polymeric matrices. Extending CN self-assembly into multiphase polymer structures has led to useful end-results in a wide spectrum of products and countless innovative applications, for example, as reinforcing agent, emulsion stabilizer, barrier membrane and binder. In the current contribution, after a brief description of salient nanocellulose chemical structure features, its types and production methods, we move to recent advances in CN utilization as an ecofriendly binder in several disparate areas, namely formaldehyde-free hybrid composites and wood-based panels, papermaking/coating processes, and energy storage devices, as well as their potential applications in biomedical fields as a cost-effective and tissue-friendly binder for cartilage regeneration, wound healing and dental repair. The prospects of a wide range of hybrid materials that may be produced via nanocellulose is introduced in light of the unique behavior of cellulose once in nano dimensions. Furthermore, we implement some principles of colloidal and interfacial science to discuss the critical role of cellulose binding in the aforesaid fields. Even though the CN facets covered in this study by no means encompass the great amount of literature available, they may be regarded as the basis for future developments in the binder applications of these highly desirable materials. Full article

(This article belongs to the Special Issue Emerging Trends in Nanocelluloses)

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