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During the past decade, cellulose nanofibrils (CNFs) have shown tremendous potential as a building block to fabricate new advanced materials that are both biocompatible and biodegradable. The excellent mechanical properties of the individual CNF can be transferred to macroscale fibers through careful control in hydrodynamic alignment and assembly processes. The optimization of such processes relies on the understanding of nanofibril dynamics during the process, which in turn requires in situ characterization. Here, we use a shear-free mixing experiment combined with scanning small-angle X-ray scattering (scanning-SAXS) to provide time-resolved nanoscale kinetics during the in situ assembly of dispersed cellulose nanofibrils (CNFs) upon mixing with a sodium chloride solution. The addition of monovalent ions led to the transition to a volume-spanning arrested (gel) state. The transition of CNFs is associated with segmental aggregation of the particles, leading to a connected network and reduced Brownian motion, whereby an aligned structure can be preserved. Furthermore, we find that the extensional flow seems to enhance the formation of these segmental aggregates, which in turn provides a comprehensible explanation for the superior material properties obtained in shear-free processes used for spinning filaments from CNFs. This observation clearly highlights the need for different assembly strategies depending on morphology and interactions of the dispersed nanoparticles, where this work can be used as a guide for improved nanomaterial processes.
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Dynamic Assembly of Strong and Conductive Carbon Nanotube/Nanocellulose Composite Filaments and Their Application in Resistive Liquid Sensing
The continuous flow assembly of colloidal nanoparticles from aqueous suspensions into macroscopic materials in a field-assisted double flow focusing system offers an attractive way to bridge the outstanding nanoscale characteristics of renewable cellulose nanofibrils (CNFs) at scales most common to human technologies. By incorporating single-walled carbon nanotubes (SWNTs) during the fabrication process, high-performance functional filament nanocomposites were produced. CNFs and SWNTs were first dispersed in water without any external surfactants or binding agents, and the resulting nanocolloids were aligned by means of an alternating electric field combined with extensional sheath flows. The nanoscale orientational anisotropy was then locked by a liquid−gel transition during the materials assembly into macroscopic filaments, which greatly improved their mechanical, electrical, and liquid sensing properties. Significantly, these findings pave the way toward the environmentally friendly and scalable manufacturing of a variety of multifunctional fibers for diverse applications.
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- Award ID(s):
- 1927623
- PAR ID:
- 10489655
- Publisher / Repository:
- ACS Applied Materials & Interfaces
- Date Published:
- Journal Name:
- ACS Applied Materials & Interfaces
- Volume:
- 15
- Issue:
- 30
- ISSN:
- 1944-8244
- Page Range / eLocation ID:
- 36647 to 36656
- Subject(s) / Keyword(s):
- nanocellulose, carbon nanotubes, filament composite, flow focusing, dielectrophoresis
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1021/acsami.3c03906
