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              <p>Cellulose nanocrystals (CNCs) are particularly attractive crystalline nanoparticles for the design of new bio-based materials with enhanced mechanical, optical (iridescence) or barrier (oxygen or water) properties. One important challenge for reaching these specific functional properties is to control the orientation and organization of the materials during their processing, in a wide spatial scale and with controlled external fields with the best possible efficiency.Recently, we were able to evidence the ability of the ultrafiltration processes to develop well-defined layered structures of CNCs [1-2]. Furthermore, we discovered by using ultrasound waves, it was possible to align the CNCs along the wave propagation direction [3].In this work, an original combined frontal ultrafiltration (FU) and ultrasound (US) set-up compatible with in situ SAXS, SALS and dichroism observations has allowed revealing for the first time a multilayer orthotropic structuring of CNC suspensions, that mimics the organization of articular cartilage: a first layer composed of CNCs having their director aligned parallel to the horizontal membrane surface, a second intermediate isotropic layer, and a third layer of CNCs with their director vertically oriented along the direction of US wave propagation direction (Figure 1). We have interpreted our observations, in particular the length scales and time scales involved in the spectacular alignment of the CNCs along the ultrasonic wave propagation direction in terms of Rayleigh acoustic streaming initiated by the viscous attenuation of the acoustic waves generated by the vibrating blade. These results open the way for developing novel orthotropic biomaterials with tunable structured cellulosic organizations for tissue engineering applications.References[1] - C. Rey et al., ACS Sust. Chem. Eng., 7, 10679-10689, (2019). https://doi.org/10.1021/acssuschemeng.9b01333[2] - E.F. Semeraro et al., Colloids Surf. A, 584,124030, (2020). https://doi.org/10.1016/j.colsurfa.2019.124030[3] - F. Pignon et al., J. Phys. Chem. C, 125, 18409-18419, (2021). https://doi.org/10.1021/acs.jpcc.1c03506[4] - F. Pignon et al., J. Colloid Interface Sci., (2024). https://doi.org/10.1016/j.jcis.2023.12.164</p>
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