The fabrication of responsive photonic structures from cellulose nanocrystals (CNCs) that can operate in the entire visible spectrum is challenging due to the requirements of precise periodic modulation of the pitch size of the self-assembled multilayer structures at the length scale within the wavelength of the visible light. The surface charge density of CNCs is an important factor in controlling the pitch size of the chiral nematic structure of the dried solid CNC films. The assembly of poly(ethylene glycol) (PEG) together with CNCs into smaller chiral nematic domains results in solid films with uniform helical structure upon slow drying. Large, flexible, and flat photonic composite films with uniform structure colors from blue to red are prepared by changing the composition of CNCs and PEG. The CNC/PEG(80/20) composite film demonstrates a reversible and smooth structural color change between green and transparent in response to an increase and decrease of relative humidity between 50% and 100% owing to the reversible swelling and dehydration of the chiral nematic structure. The composite also shows excellent mechanical and thermal properties, complementing the multifunctional property profile.

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In order to better understand nanostructured fiber networks, effects from high specific surface area of nanofibers are important to explore. For cellulose networks, this has so far only been achieved in nonfibrous regenerated cellulose aerogels. Here, nanofibrillated cellulose (NFC) is used to prepare high surface area nanopaper structures, and the mechanical properties are measured in tensile tests. The water in NFC hydrogels is exchanged to liquid CO2, supercritical CO2, and tert-butanol, followed by evaporation, supercritical drying, and sublimation, respectively. The porosity range is 40-86%. The nanofiber network structure in nanopaper is characterized by FE-SEM and nitrogen adsorption, and specific surface area is determined. High-porosity TEMPO-oxidized NFC nanopaper (56% porosity) prepared by critical point drying has a specific surface area as high as 482 m(2) g(-1). The mechanical properties of this nanopaper structure are better than for many thermoplastics, but at a significantly lower density of only 640 kg m(-3). The modulus is 1.4 GPa, tensile strength 84 MPa, and strain-to-failure 17%. Compared with water-dried nanopaper, the material is softer with substantiallly different deformation behavior.

Low-density structures of mechanical function in plants, arthropods and other organisms, are often based on high-strength cellulose or chitin nanofibers and show an interesting combination of flexibility and toughness. Here, a series of plant-inspired tough and mechanically very robust cellular biopolymer foams with porosities as high as 99.5% (porosity range 93.1-99.5%) were therefore prepared by solventfree freeze-drying from cellulose I wood nanofiber water suspensions. A wide range of mechanical properties was obtained by controlling density and nanofiber interaction in the foams, and densityproperty relationships were modeled and compared with those for inorganic aerogels. Inspired by cellulose-xyloglucan (XG) interaction in plant cell walls, XG was added during preparation of the toughest foams. For the cellulose-XG nanocomposite foams in particular, the mechanical properties at comparable densities were superior to those reported in the literature for clay aerogel/cellulose whisker nanocomposites, epoxy/clay aerogels, polymer/clay/nanotube aerogels, and polymer/silica aerogels. The foam structure was characterized by high-resolution field-emission scanning electron microscopy and the specific surface area was measured by nitrogen physisorption. Dynamic mechanical thermal analysis and uniaxial compression tests were performed. The foam was thermally stable up to 275 C where cellulose started to degrade.

Nanostructured materials are difficult to prepare rapidly and as large structures. The present study is thus significant because a rapid preparation procedure for large, flat, smooth, and optically transparent cellulose nanopaper structures is developed using a semiautomatic sheet former. Cellulose/inorganic hybrid nanopaper is also produced. The preparation procedure is compared with other approaches, and the nanopaper structures are tested in uniaxial tensile tests. Optical transparency and high tensile strength are demonstrated in 200 mm diameter nanopaper sheets, indicating well-dispersed nanofibrils. The preparation time is 1 h for a typical nanopaper thickness of 60 μm. In addition, the application of the nanopaper-making strategy to cellulose/inorganic hybrids demonstrates the potential for "green" processing of new types of nanostructured functional materials.

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