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RESEARCH PRODUCT

Directed Assembly of Cellulose Nanocrystals in Their Native Solid-State Template of a Processed Fiber Cell Wall

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Funding Information: I.S. thanks The Academy of Finland (grant no. 300364) for funding this work. C.D. acknowledges funding from FAPESP (grant 13/07932‐6). P.A.P. thanks the Emil Aaltonen Foundation and Academy of Finland (grant no. 315768) for funding and ESRF for beamtime at beamline D2am (experiment 02‐01‐885). Rita Hatakka is acknowledged for her assistance with the GPC measurements. Work of M.L. was supported by the Jane and Aatos Erkko Foundation. The work is a part of the FinnCERES Bioeconomy ecosystem. Publisher Copyright: © 2021 The Authors. Macromolecular Rapid Communications published by Wiley-VCH GmbH Copyright: Copyright 2021 Elsevier B.V., All rights reserved. Nanoparticle assembly is intensely surveyed because of the numerous applications within fields such as catalysis, batteries, and biomedicine. Here, directed assembly of rod-like, biologically derived cellulose nanocrystals (CNCs) within the template of a processed cotton fiber cell wall, that is, the native origin of CNCs, is reported. It is a system where the assembly takes place in solid state simultaneously with the top-down formation of the CNCs via hydrolysis with HCl vapor. Upon hydrolysis, cellulose microfibrils in the fiber break down to CNCs that then pack together, resulting in reduced pore size distribution of the original fiber. The denser packing is demonstrated by N2 adsorption, water uptake, thermoporometry, and small-angle X-ray scattering, and hypothetically assigned to attractive van der Waals interactions between the CNCs. Peer reviewed