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Continuous Assembly of Cellulose Nanofibrils and Nanocrystals into Strong Macrofibers through Microfluidic Spinning
RISE Res Inst Sweden, Div Mat & Prod, POB 104, SE-43122 Mölndal, Sweden..
RISE Bioecon, POB 5604, SE-11486 Stockholm, Sweden..
KTH, School of Engineering Sciences (SCI), Centres, Linné Flow Center, FLOW. KTH, School of Engineering Sciences (SCI), Engineering Mechanics.
KTH, School of Engineering Sciences (SCI), Centres, Linné Flow Center, FLOW. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.ORCID iD: 0000-0002-2504-3969
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2019 (English)In: Advanced Materials Technologies, E-ISSN 2365-709X, Vol. 4, no 2, article id 1800557Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
WILEY , 2019. Vol. 4, no 2, article id 1800557
Keywords [en]
cellulose nanocrystals, cellulose nanofibrils, flow focusing, microfluidic fiber spinning, nanocellulose
National Category
Materials Engineering
Identifiers
URN: urn:nbn:se:kth:diva-246272DOI: 10.1002/admt.201800557ISI: 000459632800051Scopus ID: 2-s2.0-85058288929OAI: oai:DiVA.org:kth-246272DiVA, id: diva2:1299259
Note

QC 20190326

Available from: 2019-03-26 Created: 2019-03-26 Last updated: 2023-09-19Bibliographically approved
In thesis
1. Experimental and numerical investigations of hydrodynamic focusing of colloidal dispersions
Open this publication in new window or tab >>Experimental and numerical investigations of hydrodynamic focusing of colloidal dispersions
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Alternative title[sv]
Experimentell och numerisk undersökningar av hydrodynamisk fokusering med kolloidala dispersioner
Abstract [en]

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.

Abstract [sv]

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.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2023
Series
TRITA-SCI-FOU ; 2023:40
Keywords
Microfluidics, flow focusing, colloidal fiber dispersion, effective interfacial tension, microflow morphology, nanoparticle orientation, Mikrofluidik, flödesfokusering, kolloidala dispersioner, effektiv ytspänning, mikroflödesmorfologi, orientering av nanopartiklar
National Category
Fluid Mechanics
Research subject
Engineering Mechanics
Identifiers
urn:nbn:se:kth:diva-336681 (URN)978-91-8040-695-6 (ISBN)
Public defence
2023-10-06, https://kth-se.zoom.us/j/61949181313, D2, Lindstedtsvägen 9, Kungliga Tekniska Högskolan, Stockholm, 10:15 (English)
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Note

QC 230918

Available from: 2023-09-18 Created: 2023-09-17 Last updated: 2025-02-09Bibliographically approved

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Gowda, V. KrishneLundell, Fredrik

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