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.

Nanoscale building blocks of many materials exhibit extraordinary mechanical properties due to their defect-free molecular structure. Translation of these high mechanical properties to macroscopic materials represents a difficult materials engineering challenge due to the necessity to organize these building blocks into multiscale patterns and mitigate defects emerging at larger scales. Cellulose nanofibrils (CNFs), the most abundant structural element in living systems, has impressively high strength and stiffness, but natural or artificial cellulose composites are 3-15 times weaker than the CNFs. Here, we report the flow-assisted organization of CNFs into macroscale fibers with nearly perfect unidirectional alignment. Efficient stress transfer from macroscale to individual CNF due to cross-linking and high degree of order enables their Young's modulus to reach up to 86 GPa and a tensile strength of 1.57 GPa, exceeding the mechanical properties of known natural or synthetic biopolymeric materials. The specific strength of our CNF fibers engineered at multiscale also exceeds that of metals, alloys, and glass fibers, enhancing the potential of sustainable lightweight high-performance materials with multiscale self-organization.

The reproducible low-cost fabrication of functional metal-polymer nanocomposites with tailored optoelectronic properties for advanced applications remains a major challenge in applied nanotechnology. To obtain full control over the nanostructural evolution at the metal-polymer interface and its impact on optoelectronic properties, we employed combined in situ time-resolved microfocus grazing incidence small angle X-ray scattering (μGISAXS) with in situ UV/vis specular reflectance spectroscopy (SRS) during sputter deposition of gold on thin polystyrene films. On the basis of the temporal evolution of the key scattering features in the real-time μGISAXS experiment, we directly observed four different growth regimes: nucleation, isolated island growth, growth of larger aggregates via partial coalescence, and continuous layer growth. Moreover, their individual thresholds were identified with subnanometer resolution and correlated to the changes in optical properties. During sputter deposition, a change in optical reflectivity of the pristine gray-blue PS film was observed ranging from dark blue color due to the presence of isolated nanoclusters at the interface to bright red color from larger Au aggregates. We used simplified geometrical assumptions to model the evolution of average real space parameters (distance, size, density, contact angle) in excellent agreement with the qualitative observation of key scattering features. A decrease of contact angles was observed during the island-to-percolation transition and confirmed by simulations. Furthermore, a surface diffusion coefficient according to the kinetic freezing model and interfacial energy of Au on PS at room temperature were calculated based on a real-time experiment. The morphological characterization is complemented by X-ray reflectivity, optical, and electron microscopy. Our study permits a better understanding of the growth kinetics of gold clusters and their self-organization into complex nanostructures on polymer substrates. It opens up the opportunity to improve nanofabrication and tailoring of metal-polymer nanostructures for optoelectronic applications, organic photovoltaics, and plasmonic-enhanced technologies.

The flow orientation of anisotropic particles through narrow channels is of importance in many fields, ranging from the spinning and molding of fibers to the flow of cells and proteins through thin capillaries. It is commonly assumed that anisotropic particles align parallel to the flow direction. When flowing through narrowed channel sections, one expects the increased flow rate to improve the parallel alignment. Here, we show by microfocus synchrotron X-ray scattering and polarized optical microscopy that anisotropic colloidal particles align perpendicular to the flow direction after passing a narrow channel section. We find this to be a general behavior of anisotropic colloids, which is also observed for disk-like particles. This perpendicular particle alignment is stable, extending downstream throughout the remaining part of the channel. We show by microparticle image velocimetry that the particle reorientation in the expansion zone after a narrow channel section occurs in a region with considerable extensional flow. This extensional flow is promoted by shear thinning, a typical property of complex fluids. Our discovery has important consequences when considering the flow orientation of polymers, micelles, fibers, proteins, or cells through narrow channels, pipes, or capillary sections. An immediate consequence for the production of fibers is the necessity for realignment by extension in the flow direction. For fibrous proteins, reorientation and stable plug flow are likely mechanisms for protein coagulation.block copolymers | microfluidics | small-angle X-ray scattering T he flow orientation of anisotropic particles in narrow channels is relevant in many fields, ranging from the spinning and molding of fibers to the flow of cells or proteins through thin capillaries (1-4). It is commonly assumed that anisotropic particles align parallel to the flow direction (5). When flowing through thin channel sections, one expects the increased flow rate to improve the alignment. We investigated the alignment of anisotropic colloids (i.e., cylindrical micelles) flowing through thin sections of microchannels using synchrotron microfocus small-angle X-ray diffraction and polarized optical microscopy. Surprisingly, we find that anisotropic colloids orient perpendicular to the flow direction after passing through narrow channel sections. The perpendicular alignment is surprisingly stable, extending throughout the remaining part downstream of the channel. Ongoing experimental studies indicate that this observation holds for other anisotropic cylindrical or disk-like colloids as well. We show by microparticle image velocimetry and finite element fluid dynamics simulations that the perpendicular flow orientation is induced by perpendicular extensional flow in the expansion zone after the narrow section. Only close to the channel walls does shear flow dominate, leading to parallel flow orientation of anisotropic particles.In situ investigations of the flow orientation of colloids in solution under very well-defined flow conditi...