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| 2. |
- Brouzet, Christophe, et al.
(författare)
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Characterizing the Orientational and Network Dynamics of Polydisperse Nanofibers on the Nanoscale
- 2019
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Ingår i: Macromolecules. - : American Chemical Society (ACS). - 0024-9297 .- 1520-5835. ; 52:6, s. 2286-2295
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Tidskriftsartikel (refereegranskat)abstract
- Polydisperse fiber networks are the basis of many natural and manufactured structures, ranging from high-performance biobased materials to components of living cells and tissues. The formation and behavior of such networks are given by fiber properties such as length and stiffness as well as the number density and fiber-fiber interactions. Studies of fiber network behavior, such as connectivity or rigidity thresholds, typically assume monodisperse fiber lengths and isotropic fiber orientation distributions, specifically for nano scale fibers, where the methods providing time-resolved measurements are limited. Using birefringence measurements in a microfluidic flow-focusing channel combined with a flow stop procedure, we here propose a methodology allowing investigations of length-dependent rotational dynamics of nanoscale polydisperse fiber suspensions, including the effects of initial nonisotropic orientation distributions. Transition from rotational mobility to rigidity at entanglement thresholds is specifically addressed for a number of nanocellulose suspensions, which are used as model nanofiber systems. The results show that the proposed method allows the characterization of the subtle interplay between Brownian diffusion and nanoparticle alignment on network dynamics.
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| 3. |
- Brouzet, Christophe, et al.
(författare)
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Effect of Electric Field on the Hydrodynamic Assembly of Polydisperse and Entangled Fibrillar Suspensions
- 2021
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Ingår i: Langmuir. - : American Chemical Society (ACS). - 0743-7463 .- 1520-5827. ; 37:27, s. 8339-8347
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Tidskriftsartikel (refereegranskat)abstract
- Dynamics of colloidal particles can be controlled by the application of electric fields at micrometer-nanometer length scales. Here, an electric field-coupled microfluidic flow-focusing device is designed for investigating the effect of an externally applied alternating current (AC) electric field on the hydrodynamic assembly of cellulose nanofibrils (CNFs). We first discuss how the nanofibrils align parallel to the direction of the applied field without flow. Then, we apply an electric field during hydrodynamic assembly in the microfluidic channel and observe the effects on the mechanical properties of the assembled nanostructures. We further discuss the nanoscale orientational dynamics of the polydisperse and entangled fibrillar suspension of CNFs in the channel. It is shown that electric fields induced with the electrodes locally increase the degree of orientation. However, hydrodynamic alignment is demonstrated to be much more efficient than the electric field for aligning CNFs. The results are useful for understanding the development of the nanostructure when designing high-performance materials with microfluidics in the presence of external stimuli.
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| 4. |
- Brouzet, Christophe, et al.
(författare)
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Size-Dependent Orientational Dynamics of Brownian Nanorods
- 2018
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Ingår i: ACS Macro Letters. - : American Chemical Society (ACS). - 2161-1653. ; 7:8, s. 1022-1027
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Tidskriftsartikel (refereegranskat)abstract
- Successful assembly of suspended nanoscale rod-like particles depends on fundamental phenomena controlling rotational and translational diffusion. Despite the significant developments in fluidic fabrication of nanostructured materials, the ability to quantify the dynamics in processing systems remains challenging. Here we demonstrate an experimental method for characterization of the orientation dynamics of nanorod suspensions in assembly flows using orientation relaxation. This relaxation, measured by birefringence and obtained after rapidly stopping the flow, is deconvoluted with an inverse Laplace transform to extract a length distribution of aligned nanorods. The methodology is illustrated using nanocelluloses as model systems, where the coupling of rotational diffusion coefficients to particle size distributions as well as flow-induced orientation mechanisms are elucidated.
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| 5. |
- Gowda, V. Krishne, et al.
(författare)
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Effective interfacial tension in flow-focusing of colloidal dispersions : 3-D numerical simulations and experiments
- 2019
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Ingår i: Journal of Fluid Mechanics. - : CAMBRIDGE UNIV PRESS. - 0022-1120 .- 1469-7645. ; 876, s. 1052-1076
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 6. |
- Mittal, Nitesh, et al.
(författare)
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Multiscale Control of Nanocellulose Assembly : Transferring Remarkable Nanoscale Fibril Mechanics to Macroscale Fibers
- 2018
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 12:7, s. 6378-6388
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 7. |
- Redlinger-Pohn, Jakob D., et al.
(författare)
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Mechanisms of Cellulose Fiber Comminution to Nanocellulose by Hyper Inertia Flows
- 2022
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Ingår i: ACS Sustainable Chemistry and Engineering. - : American Chemical Society. - 2168-0485. ; 10:2, s. 703-719
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Tidskriftsartikel (refereegranskat)abstract
- Nanocelluloses are seen as the basis of high-performance materials from renewable sources, enabling a bio-based sustainable future. Unsurprisingly, research has initially been focused on the design of new material concepts and less on new and adapted fabrication processes that would allow large-scale industrial production and widespread societal impact. In fact, even the processing routes for making nanocelluloses and the understanding on how the mechanical action fibrillates plant raw materials, albeit chemically or enzymatically pre-treated, are only rudimentary and have not evolved significantly during the past three decades. To address the challenge of designing cellulose comminution processes for a reliable and predictable production of nanocelluloses, we engineered a study setup, referred to as Hyper Inertia Microfluidizer, to observe and quantify phenomena at high speeds and acceleration into microchannels, which is the underlying flow in homogenization. We study two different channel geometries, one with acceleration into a straight channel and one with acceleration into a 90° bend, which resembles the commercial equipment for microfluidization. With the purpose of intensification of the nanocellulose production process, we focused on an efficient first pass fragmentation. Fibers are strained by the extensional flow upon acceleration into the microchannels, leading to buckling deformation and, at a higher velocity, fragmentation. The treatment induces sites of structural damage along and at the end of the fiber, which become a source for nanocellulose. Irrespectively on the treatment channel, these nanocelluloses are fibril-agglomerates, which are further reduced to smaller sizes. In a theoretical analysis, we identify fibril delamination as failure mode from bending by turbulent fluctuations in the flow as a comminution mechanism at the nanocellulose scale. Thus, we argue that intensification of the fibrillation can be achieved by an initial efficient fragmentation of the cellulose in smaller fragments, leading to a larger number of damaged sites for the nanocellulose production. Refinement of these nanocelluloses to fibrils is then achieved by an increase in critical bending events, i.e., decreasing the turbulent length scale and increasing the residence time of fibrils in the turbulent flow. © 2022 The Authors.
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| 8. |
- Rosén, Tomas, et al.
(författare)
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Three-Dimensional Orientation of Nanofibrils in Axially Symmetric Systems Using Small-Angle X-ray Scattering
- 2018
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Ingår i: The Journal of Physical Chemistry C. - : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455. ; 122:12, s. 6889-6899
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Tidskriftsartikel (refereegranskat)abstract
- The increased availability and brilliance of new X-ray facilities have in the recent years opened up the possibility to characterize the alignment of dispersed anisotropic nanoparticles in various microfluidic applications, from hydrodynamic self-assemblies to flows in complex geometries. In such applications, it is vital to study the alignment of the nanoparticles in the flow, as this in turn affects the final properties of the self-assembled superstructures or those of the flow itself. Small-angle X-ray scattering (SAXS) is a well-suited characterization technique for this but typically provides the alignment in a projected plane perpendicular to the beam direction. In this work, we demonstrate a simple method to reconstruct the full three-dimensional orientation distribution function from a SAXS experiment through the assumption that the azimuthal angle of the nanoparticles around the flow direction is distributed uniformly, an assumption that is valid for a large range of nanoparticle flow processes. For demonstration purposes, the experimental results from previous works on hydrodynamic self-assembly of cellulose nanofibrils (CNFs) into filaments have been revised, resulting in a small correction to the presented order parameters. The results are then directly compared with simple numerical models to describe the increased alignment of CNFs both in the flowing system and during the drying of the filament. The proposed reconstruction method will allow for further improvements of theoretical or numerical simulations and consequently open up new possibilities for optimizing assembly processes, which include flow alignment of elongated nanoparticles.
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