This critical review provides a processing-structure-property perspective on recent advances in cellulose nanoparticles and composites produced from them. It summarizes cellulose nanoparticles in terms of particle morphology, crystal structure, and properties. Also described are the self-assembly and rheological properties of cellulose nanoparticle suspensions. The methodology of composite processing and resulting properties are fully covered, with an emphasis on neat and high fraction cellulose composites. Additionally, advances in predictive modeling from molecular dynamic simulations of crystalline cellulose to the continuum modeling of composites made with such particles are reviewed (392 references).

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Cellulose nanomaterials review: structure, properties and nanocomposites

Cellulose fibrils with widths in the nanometer range are nature-based materials with unique and potentially useful features. Most importantly, these novel nanocelluloses open up the strongly expanding fields of sustainable materials and nanocomposites, as well as medical and life-science devices, to the natural polymer cellulose. The nanodimensions of the structural elements result in a high surface area and hence the powerful interaction of these celluloses with surrounding species, such as water, organic and polymeric compounds, nanoparticles, and living cells. This Review assembles the current knowledge on the isolation of microfibrillated cellulose from wood and its application in nanocomposites; the preparation of nanocrystalline cellulose and its use as a reinforcing agent; and the biofabrication of bacterial nanocellulose, as well as its evaluation as a biomaterial for medical implants.

Nanocelluloses: A New Family of Nature-Based Materials

Due to their abundance, high strength and stiffness, low weight and biodegradability, nano-scale cellulose fiber materials (e.g., microfibrillated cellulose and bacterial cellulose) serve as promising candidates for bio-nanocomposite production. Such new high-value materials are the subject of continuing research and are commercially interesting in terms of new products from the pulp and paper industry and the agricultural sector. Cellulose nanofibers can be extracted from various plant sources and, although the mechanical separation of plant fibers into smaller elementary constituents has typically required high energy input, chemical and/or enzymatic fiber pre-treatments have been developed to overcome this problem. A challenge associated with using nanocellulose in composites is the lack of compatibility with hydrophobic polymers and various chemical modification methods have been explored in order to address this hurdle. This review summarizes progress in nanocellulose preparation with a particular focus on microfibrillated cellulose and also discusses recent developments in bio-nanocomposite fabrication based on nanocellulose.

Microfibrillated cellulose and new nanocomposite materials: a review

Native wood celluloses can be converted to individual nanofibers 3–4 nm wide that are at least several microns in length, i.e. with aspect ratios >100, by TEMPO (2,2,6,6-tetramethylpiperidine-1-oxyl radical)-mediated oxidation and successive mild disintegration in water. Preparation methods and fundamental characteristics of TEMPO-oxidized cellulose nanofibers (TOCN) are reviewed in this paper. Significant amounts of C6 carboxylate groups are selectively formed on each cellulose microfibril surface by TEMPO-mediated oxidation without any changes to the original crystallinity (∼74%) or crystal width of wood celluloses. Electrostatic repulsion and/or osmotic effects working between anionically-charged cellulose microfibrils, the ζ-potentials of which are approximately −75 mV in water, cause the formation of completely individualized TOCN dispersed in water by gentle mechanical disintegration treatment of TEMPO-oxidized wood cellulose fibers. Self-standing TOCN films are transparent and flexible, with high tensile strengths of 200–300 MPa and elastic moduli of 6–7 GPa. Moreover, TOCN-coated poly(lactic acid) films have extremely low oxygen permeability. The new cellulose-based nanofibers formed by size reduction process of native cellulose fibers by TEMPO-mediated oxidation have potential application as environmentally friendly and new bio-based nanomaterials in high-tech fields.

TEMPO-oxidized cellulose nanofibers

This paper provides an overview of recent progress made in the area of cellulose nanofibre-based nanocomposites. An introduction into the methods used to isolate cellulose nanofibres (nanowhiskers, nanofibrils) is given, with details of their structure. Following this, the article is split into sections dealing with processing and characterisation of cellulose nanocomposites and new developments in the area, with particular emphasis on applications. The types of cellulose nanofibres covered are those extracted from plants by acid hydrolysis (nanowhiskers), mechanical treatment and those that occur naturally (tunicate nanowhiskers) or under culturing conditions (bacterial cellulose nanofibrils). Research highlighted in the article are the use of cellulose nanowhiskers for shape memory nanocomposites, analysis of the interfacial properties of cellulose nanowhisker and nanofibril-based composites using Raman spectroscopy, switchable interfaces that mimic sea cucumbers, polymerisation from the surface of cellulose nanowhiskers by atom transfer radical polymerisation and ring opening polymerisation, and methods to analyse the dispersion of nanowhiskers. The applications and new advances covered in this review are the use of cellulose nanofibres to reinforce adhesives, to make optically transparent paper for electronic displays, to create DNA-hybrid materials, to generate hierarchical composites and for use in foams, aerogels and starch nanocomposites and the use of all-cellulose nanocomposites for enhanced coupling between matrix and fibre. A comprehensive coverage of the literature is given and some suggestions on where the field is likely to advance in the future are discussed.

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Review: current international research into cellulose nanofibres and nanocomposites

Enzymatic hydrolysis combined with mechanical shearing and high-pressure homogenization for nanoscale cellulose fibrils and strong gels.

The present invention provides a method for treatment of chemical pulp for the manufacturing of microfibrillated cellulose comprising the following steps: a) providing a hemicellulose containing pulp, b) refining said pulp in at least one step and treating said pulp with one or more wood degrading enzymes at a relatively low enzyme dosage, and c) homogenizing said pulp thus providing s aid microfibrillated cellulose. According to a second aspect of the invention a microfibrillated cellulose obtainable by the method according to the first aspect is provided . According to a third aspect of the invention, use of said microfibrillated cellulose according to the second aspect in food products, paper products, composite materials, coatings or in rheology modifiers (e.g. drilling muds) is provided .

Method for the manufacturing of microfibrillated cellulose

The present invention provides a method for the manufacturing of nanocellulose. The method includes a first mod-ification of the cellulose material, where the cellulose fibres are treated with an aqueous electrolyte-containing solution of an am-photeric cellulose derivative. The modification is followed by a mechanical treatment. By using this method for manufacturing nanocellulose, clogging of the mechanical apparatus is avoided. Also disclosed is nanocellulose manufactured in accordance with said method and uses of said cellulose.

Method for providing a nanocellulose involving modifying cellulose fibers

The invention relates to compositions for coating of printing paper, said compositions comprising microfibrillated cellulose (MFC) and one or more polysaccharide hydrocolloids, and use of said compositions. Further, the invention relates to coated paper, comprising a first layer of polysaccharide hydrocolloid(s) and a second layer of MFC, and use of said paper. A method for reducing the linting and/or dusting of a paper is also disclosed.

Composition for coating of printing paper

A method for treatment of chemical pulp for the manufacturing of microfibrillated cellulose includes the following steps: a) providing a hemicellulose containing pulp, b) refining the pulp in at least one step and treating the pulp with one or more wood degrading enzymes at a relatively low enzyme dosage, and c) homogenizing the pulp thus providing the microfibrillated cellulose. According to a second aspect of the invention a microfibrillated cellulose obtainable by the method according to the first aspect is provided. According to a third aspect of the invention, use of the microfibrillated cellulose according to the second aspect in food products, paper products, composite materials, coatings or in rheology modifiers (e.g. drilling muds) is provided.

Tom Lindström

Papers

Enzymatic hydrolysis combined with mechanical shearing and high-pressure homogenization for nanoscale cellulose fibrils and strong gels.

Method for the manufacturing of microfibrillated cellulose

Method for providing a nanocellulose involving modifying cellulose fibers

Composition for coating of printing paper

Method for the manufacture of microfibrillated cellulose