Properties and functions of materials assembled from nanofibrils critically depend on alignment. A material with aligned nanofibrils is typically stiffer compared with a material with a less anisotropic orientation distribution. In this work, we investigate nanofibril alignment during flow focusing, a flow case used for spinning of filaments from nanofibril dispersions. In particular, we combine experimental measurements and simulations of the flow and fibril alignment to demonstrate how a numerical model can be used to investigate how the flow geometry affects and can be used to tailor the nanofibril alignment and filament shape. The confluence angle between sheath flow and core flow, the aspect ratio of the channel and the contractions in the sheath and/or core flow channels are varied. Successful spinning of stiff filaments requires: (i) detachment of the core flow from the top and bottom channel walls and (ii) a high and homogeneous fibril alignment. Somewhat expected, the results show that the confluence angle has a relatively small effect on alignment compared with contractions. Contractions in the sheath flow channels are seen to be beneficial for detachment, and contractions in the core flow channel are found to be an efficient way to increase and homogenise the degree of alignment.

Dispersed non-spherical particles are the fundamental constituent of many complex fluids. Such fluids are studied both for their industrial and scientific importance, and for their peculiar functional properties (mechanical, optical, thermal, fluidic). One exemplar is cellulose nanofibrils (CNF), a biopolymer made of nanoscale particles with remarkable mechanical properties that has been found to be the potential candidate for the fabrication of sustainable and bio-compatible materials. To synthesize and characterise the behaviour of such non-spherical particles in flowing dispersions, microfluidic platforms have emerged as powerful tools. However, the scientific understanding of the fundamental role of the fluid dispersion properties and flow parameters on the microflow dynamics is still inadequate.  

In this thesis work, a combined numerical and experimental investigation with diverse set of microfluidic flow focusing devices are adopted to measure, analyse, and understand the micro-  and macro-scale morphologies of flowing dispersions. A high-viscosity colloidal dispersion liquid made of cellulose nanofibrils suspended in water (the solvent) is hydrodynamically focused with the low-viscosity solvent liquid. A 3D colloidal viscous thread structure is formed, which is characterized using optical coherence tomography (OCT) measurements and computational fluid dynamics (CFD) simulations. The studies show that if the Péclet number is large (diffusion of the particles is slower than the convective time scale of the flow), the concentration gradient between two in-homogeneous miscible fluids (colloidal dispersion and its own solvent) gives rise to Korteweg stresses, emulating the effect of interfacial tension in the form of effective interfacial tension (EIT). In addition, scaling laws describing the complex interplay between viscous, inertial and capillary effects in microchannels have been identified, and are in turn used to estimate the fluid properties.

Further, the collective behaviour of nanofibrils in the studied flow fields is investigated. Numerically modelled orientation distribution functions (ODF)  are compared with in-situ small angle X-ray scattering (SAXS) measurements. The calibrated SAXS-based digital twin model unveils complete 3D nanoparticle orientation both along the streamwise and cross-sectional planes of the channels. Overall, the key findings of this work open up possibilities in controlling the hydrodynamic assembly of nanoparticles in microchannels.

Icke-sfäriska nanopartiklar är den grundläggande byggstenen i många komplexa vätskor. Sådana vätskor studeras både på grund av deras industriella och vetenskapliga betydelse och på grund av deras intressanta egenskaper (mekaniska, optiska, termiska och fluidiska). Ett exempel på sådana partiklar är cellulosanofibriller (CNF), en biopolymer med anmärkningsvärda mekaniska egenskaper som har stor potential för tillverkning av hållbara och biokompatibla material. Ett kraftfullt verktyg för syntes och karakterisering av sådana icke-sfäriska partiklar i strömmande dispersioner är mikrofluidik, men den vetenskapliga förståelsen av partiklarnas och dispersionernas beteende i mikrofluidiksystem är fortfarande otillräcklig.  

I denna avhandling kombineras numeriska och experimentella metoder för att mäta, analysera och förstå flödande dispersioners makroskopiska och de ingående partiklarnas mikroskopiska beteende i olika strömningssituationer. Det specifika strömningsfall som studeras är strömningsfokusering: en högviskös kolloidal dispersion bestående av cellulosanofibriller i vatten fokuseras hydrodynamiskt av ett yttre flöde med rent vatten med låg viskositet i en kanal. Det kan då skapas högviskös "tråd" i kanalen. Detta flöde karakteriseras med hjälp av optisk koherenstomografi (OCT) och CFD-simuleringar (Computational Fluid Dynamics). Om Péclet-talet här stort (vilket betyder att partiklarnas diffusionshastighet är lägre än strömningshastigheten) ger koncentrationsgradienten mellan två homogena, blandbara  vätskor (kolloidal dispersion och dess eget lösningsmedel) upphov till Korteweg-spänningar, vilka kan modelleras med en effektiv ytspänning (EIT). Skalningslagar som beskriver de komplexa kopplingarna mellan effekter av viskositet, tröghet och ytspänning i mikrokanalen system har tagits fram, och skalningslagarna används i sin tur för att uppskatta vätskeegenskaperna.        

Även det kollektiva beteendet hos nanofibrillerna själva har studerats. Numeriskt modellerade orienteringfördelningar jämförs med in-situ röntgenspridningsmätningar (SAXS). Resultatet blir en experimentellt kalibrerad digital modell som avslöjar nanopartiklarnas 3D-orientering i hela systemet. Sammansatta gör resultaten i denna avhandling det möjligt att prediktera, optimera och kontrollera hydrodynamisk syntes av icke-sfäriska partiklar i olika kanalsystem.

The nanostructure, primarily particle orientation, controls mechanical and functional (e.g., mouthfeel, cell compatibility, optical, morphing) properties when macroscopic materials are assembled from nanofibrils. Understanding and controlling the nanostructure is therefore an important key for the continued development of nanotechnology. We merge recent developments in the assembly of biological nanofibrils, X-ray diffraction orientation measurements, and computational fluid dynamics of complex flows. The result is a digital twin, which reveals the complete particle orientation in complex and transient flow situations, in particular the local alignment and spatial variation of the orientation distributions of different length fractions, both along the process and over a specific cross section. The methodology forms a necessary foundation for analysis and optimization of assembly involving anisotropic particles. Furthermore, it provides a bridge between advanced in operandi measurements of nanostructures and phenomena such as transitions between liquid crystal states and in silico studies of particle interactions and agglomeration.

Threads of colloidal dispersions can be formed in microfluidic channel systems and are often used for analytical purposes or to assemble macroscopic structures from colloidal particles. Here, we report a combined experimental and numerical study of thread formation in channel systems with varying geometry. In the reference flow-focusing configuration, the sheath flows impinge the core flow orthogonally while in four other channel configurations, the sheath flows impinge the core flow at different confluence angles, which are both positive and negative with respect to the reference sheath direction. Tomographic measurements of the thread development are made using optical coherence tomography (OCT) and are compared to numerically simulated 3D data. The numerical simulations performed with an immiscible fluid solver show good agreement with the experiments in terms of 3D thread shapes, wetted region morphologies, and velocity fields provided an ultralow interfacial tension is applied between the low viscosity (solvent) sheath flows and the high viscosity (dispersion) core flow. Such an ultralow interfacial tension is motivated by the so-called Korteweg stresses induced as a result of the concentration gradient between two miscible fluids in nonequilibrium state. These stresses mimic the effect of interfacial tension, and are often modeled as an effective interfacial tension (EIT), an approach chosen in the present work as well. The value of interfacial tension applied in the simulations was determined through an optimization procedure and compares well with a value deduced from a scaling analysis utilizing the downstream development of experimentally determined thread shape. The experimental and numerical results show that for channel configurations with modest deviations from orthogonal sheath flows, the effect on the thread is similar regardless of whether the sheath flows are co- or counterflowing the core flow. In fact, for these cases, the effect of co- and counterflowing sheath flows can be reproduced with orthogonal sheath flows, if the sheath channel width is increased. However, for channel configurations with larger deviations from orthogonal sheath flows, the effects on the thread are direction dependent. The one-to-one comparison and analysis of numerical and experimental results bring useful insights to understand the behavior of miscible systems involving high-viscosity contrast fluids. These key results provide the foundation to tune the flow-focusing for specific applications, for example in tailoring the assembly of nanostruc-tured materials.

Microfluidic fiber spinning is a promising technique for assembling cellulose nanomaterials into macroscopic fibers. However, its implementation requires upscalabe fabrication processes while maintaining high strength of the fibers, which could not be previously achieved. Herein, a continuous wet spinning process based on microfluidic flow focusing is developed to produce strong fibers from cellulose nanofibrils (CNFs) and nanocrystals (CNCs). Fibers with an average breaking tenacity as high as 29.5 cN tex(-1) and Young's modulus of 1146 cN tex(-1) are reported for the first time, produced from nonhighly purified CNF grades. Using the same developed method, wet spinning of fibers from CNCs is achieved for the first time, reaching an average Young's modulus of 1263 cN tex(-1) and a breaking tenacity of 10.6 cN tex(-1), thus exhibiting strength twice as high as that of common CNC films. A rather similar stiffness of CNC and CNF spun fibers may originate from similar degrees of alignment, as confirmed by wide-angle X-ray scattering (WAXS) and birefringence measurements, whereas lower strength may primarily arise from the shorter length of CNCs compared to that of CNFs. The benefit of CNCs is their higher solids content in the dopes. By combining both CNCs and CNFs, the fiber properties can be tuned.

An interface between two miscible fluids is transient, existing as a non-equilibrium state before complete molecular mixing is reached. However, during the existence of such an interface, which typically occurs at relatively short time scales, composition gradients at the boundary between the two liquids cause stresses effectively mimicking an interfacial tension. Here, we combine numerical modelling and experiments to study the influence of an effective interfacial tension between a colloidal fibre dispersion and its own solvent on the flow in a microfluidic system. In a flow-focusing channel, the dispersion is injected as core flow that is hydrodynamically focused by its solvent as sheath flows. This leads to the formation of a long fluid thread, which is characterized in three dimensions using optical coherence tomography and simulated using a volume of fluid method. The simulated flow and thread geometries very closely reproduce the experimental results in terms of thread topology and velocity flow fields. By varying the interfacial tension numerically, we show that it controls the thread development, which can be described by an effective capillary number. Furthermore, we demonstrate that the applied methodology provide the means to measure the ultra-low but dynamically highly significant effective interfacial tension.

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.

We report a combined experimental and numerical investigation to decipher and delineate the role of fluid properties, flow parameters, and geometries on the dynamics of viscous thread formation in microchannels with miscible solvents. A methodological analysis based on the evolution of viscous threads unveils the significance of effective interfacial tension (EIT) induced by the virtue of concentration gradients between the non-equilibrium miscible fluid pair colloidal dispersions and their own solvent.  Functional scaling relationships developed with dimensionless capillary and Weber numbers, together with thread quantities thread detachment length, and thread width, shed light on the complex interplay of hydrodynamic effects and viscous microflow processes. The detachment of viscous threads inside microchannels is governed by the unified hydrodynamic effects of inertia, capillary, and viscous stresses in contrast to the natural phenomenon of self-lubrication,  bringing new insights to the physical phenomena involved in the confined microsystems. Exploiting the experimentally measured thread quantities, the scaling laws are practically applied to estimate the inherent fluid properties such as EIT between two inhomogeneous miscible fluids, and the fluid viscosities. In addition, the cross-sectional aspect ratio of the channels is varied numerically in conjunction with the converging shaped sections.  For specified flow rates and given rheologies of the fluids,  a flow-focusing configuration producing the shortest thread detachment length, and a longer region of strain rate along the centreline is identified. Overall, this work provides a consolidated description of the effect of fluid properties, flow parameters, and geometry on the formation of miscible viscous threads in microchannel flows.