Karl Håkansson

Hydrodynamic alignment and assembly of nanofibrils resulting in strong cellulose filaments.

Cellulose nanofibrils can be obtained from trees and have considerable potential as a building block for biobased materials. In order to achieve good properties of these materials, the nanostructure must be controlled. Here we present a process combining hydrodynamic alignment with a dispersion–gel transition that produces homogeneous and smooth filaments from a low-concentration dispersion of cellulose nanofibrils in water. The preferential fibril orientation along the filament direction can be controlled by the process parameters. The specific ultimate strength is considerably higher than previously reported filaments made of cellulose nanofibrils. The strength is even in line with the strongest cellulose pulp fibres extracted from wood with the same degree of fibril alignment. Successful nanoscale alignment before gelation demands a proper separation of the timescales involved. Somewhat surprisingly, the device must not be too small if this is to be achieved.

Highly conducting, strong nanocomposites based on nanocellulose-assisted aqueous dispersions of single-wall carbon nanotubes.

It is challenging to obtain high-quality dispersions of single-wall nanotubes (SWNTs) in composite matrix materials, in order to reach the full potential of mechanical and electronic properties. The most widely used matrix materials are polymers, and the route to achieving high quality dispersions of SWNT is mainly chemical functionalization of the SWNT. This leads to increased cost, a loss of strength and lower conductivity. In addition full potential of colloidal self-assembly cannot be fully exploited in a polymer matrix. This may limit the possibilities for assembly of highly ordered structural nanocomposites. Here we show that nanofibrillated cellulose (NFC) can act as an excellent aqueous dispersion agent for as-prepared SWNTs, making possible low-cost exfoliation and purification of SWNTs with dispersion limits exceeding 40 wt %. The NFC:SWNT dispersion may also offer a cheap and sustainable alternative for molecular self-assembly of advanced composites. We demonstrate semitransparent conductive films, aerogels and anisotropic microscale fibers with nanoscale composite structure. The NFC:SWNT nanopaper shows increased strength at 3 wt % SWNT, reaching a modulus of 13.3 GPa, and a strength of 307 MPa. The anisotropic microfiber composites have maximum conductivities above 200 S cm(-1) and current densities reaching 1400 A cm(-2).

Ultrastrong and Bioactive Nanostructured Bio-Based Composites

Natures design of functional materials relies on smart combinations of simple components to achieve desired properties. Silk and cellulose are two clever examples from nature-spider silk being tough due to high extensibility, whereas cellulose possesses unparalleled strength and stiffness among natural materials. Unfortunately, silk proteins cannot be obtained in large quantities from spiders, and recombinant production processes are so far rather expensive. We have therefore combined small amounts of functionalized recombinant spider silk proteins with the most abundant structural component on Earth (cellulose nanofibrils (CNFs)) to fabricate isotropic as well as anisotropic hierarchical structures. Our approach for the fabrication of bio-based anisotropic fibers results in previously unreached but highly desirable mechanical performance with a stiffness of ∼55 GPa, strength at break of ∼1015 MPa, and toughness of ∼55 MJ m-3. We also show that addition of small amounts of silk fusion proteins to CNF results in materials with advanced biofunctionalities, which cannot be anticipated for the wood-based CNF alone. These findings suggest that bio-based materials provide abundant opportunities to design composites with high strength and functionalities and bring down our dependence on fossil-based resources.

Online determination of anisotropy during cellulose nanofibril assembly in a flow focusing device

In order to utilize the high strength (ultimate tensile strength = 3 GPa) [Saito et al., Biomacromolecules, 2012, 14, 248] and stiffness (Youngs modulus = 130 GPa) [Sakurada et al., J. Polym. Sci., 1962, 57, 651] of cellulose nanofibrils in a macroscopic material or composite, the structure of the elongated fibrils in the material must be controlled. Here, cellulose nanofibrils in a dispersed state are partly aligned in a flow focusing device, whereafter the anisotropic nano-structure is locked by a dispersion–gel transition. The alignment process has been studied by Hakansson et al., [Nat. Commun., 2014, 5, 4018], however, the location of the phase transition as well as at which alignment (anisotropy) the fibrils were locked was not investigated. In this study, the degree of alignment is determined with small angle X-ray scattering experiments and the location of the phase change is measured with polarized light experiments. Furthermore, the anisotropy of the hydrogel thread is determined and the thread is seen to still be anisotropic after six months in a water bath.

Nanofibril Alignment in Flow Focusing: Measurements and Calculations

Alignment of anisotropic supermolecular building blocks is crucial to control the properties of many novel materials. In this study, the alignment process of cellulose nanofibrils (CNFs) in a flow-focusing channel has been investigated using small-angle X-ray scattering (SAXS) and modeled using the Smoluchowski equation, which requires a known flow field as input. This flow field was investigated experimentally using microparticle-tracking velocimetry and by numerically applying the two-fluid level set method. A semidilute dispersion of CNFs was modeled as a continuous phase, with a higher viscosity as compared to that of water. Furthermore, implementation of the Smoluchowski equation also needed the rotational Brownian diffusion coefficient, which was experimentally determined in a shear viscosity measurement. The order of the nanofibrils was found to increase during extension in the flow-focusing channel, after which rotational diffusion acted on the orientation distribution, driving the orientation of the fibrils toward isotropy. The main features of the alignment and dealignment processes were well predicted by the numerical model, but the model overpredicted the alignment at higher rates of extension. The apparent rotational diffusion coefficient was seen to increase steeply as the degree of alignment increased. Thus, the combination of SAXS measurements and modeling provides the necessary framework for quantified studies of hydrodynamic alignment, followed by relaxation toward isotropy.