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ACS Appl Mater Interfaces. 2017 Sep 13;9(36):31095-31101. doi: 10.1021/acsami.7b08783. Epub 2017 Aug 28.

Smart Cellulose Nanofluids Produced by Tunable Hydrophobic Association of Polymer-Grafted Cellulose Nanocrystals.

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Department of Bionano Technology, Hanyang University , Ansan 15588, Republic of Korea.
Amore-Pacific R&D Centre , Yongin 17074, Republic of Korea.
SK Bioland R&D Co. Ltd. , Osong 28162, Republic of Korea.
Department of Chemical and Environmental Engineering, Yale University , New Haven, Connecticut 06511, United States.
Department of Chemical and Molecular Engineering, Hanyang University , Ansan 15588, Republic of Korea.


Cellulose fibrils, unique plant-derived semicrystalline nanomaterials with exceptional mechanical properties, have significant potential for rheology modification of complex fluids due to their ability to form a physically associated semiflexible fibrillary network. Here, we report new associative cellulose nanocrystals (ACNCs) with stress-responsive rheological behaviors in an aqueous solution. The surface-mediated living radical polymerization was employed to graft poly(stearyl methacrylate-co-2-methacryloxyethyl phosphorylcholine) brushes onto the nanofibrils, and then 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-mediated oxidation was conducted to produce nanoscale ACNCs in the aqueous solution. The ACNCs displayed interfibril association driven by the hydrophobic interaction that resulted in the formation of a nanofibrillar crystalline gel phase. We observed that the viscosity of the ACNC fluid showed reversible shear thinning and temperature-induced thickening in response to applied shear stress and thermal shock. Moreover, thanks to generation of a mechanically robust nanofibrillar crystalline gel network, the ACNC suspension showed extraordinary stability to changes in salinity and pH. These results highlighted that the interfibril hydrophobic association of ACNCs was vital and played an essential role in regulation of stimuli-responsive sol-gel transitions.


associative cellulose nanocrystals; hydrophobic interaction; nanofibrillar crystallinity; smart nanofluids; sol−gel transition


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